ORCID Profile
0000-0002-2411-8041
Current Organisation
University of Adelaide
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Research Topics
In Research Link Australia (RLA), "Research Topics" refer to ANZSRC FOR and SEO codes. These topics are either sourced from ANZSRC FOR and SEO codes listed in researchers' related grants or generated by a large language model (LLM) based on their publications.
Top 5 Research Topics
ANZSRC Field of Research (FoR)
Nanomaterials | Functional Materials | Materials Engineering | Renewable Power and Energy Systems Engineering (excl. Solar Cells) | Energy Generation, Conversion and Storage Engineering | Nanotechnology | Physical Chemistry of Materials | Biomaterials | Electrical and Electronic Engineering | Theory and Design of Materials | Electrochemistry | Structural Chemistry and Spectroscopy | Nanomaterials | Nanotechnology | Carbon sequestration science | Composite and Hybrid Materials | Electrochemical energy storage and conversion
ANZSRC Socio-Economic Objective (SEO)
Expanding Knowledge in the Chemical Sciences | Renewable Energy not elsewhere classified | Expanding Knowledge in Engineering | Wind Energy | Expanding Knowledge in the Medical and Health Sciences | Solid Oxide Fuel Cells | Energy Storage (excl. Hydrogen) | Solar-Photovoltaic Energy |
Related Links
Publications
Electrocatalytically Switchable CO2 Capture: First Principle Computational Exploration of Carbon Nanotubes with Pyridinic Nitrogen
Publisher: Wiley
Date: 02-2014
Abstract: Carbon nanotubes with specific nitrogen doping are proposed for controllable, highly selective, and reversible CO2 capture. Using density functional theory incorporating long-range dispersion corrections, we investigated the adsorption behavior of CO2 on (7,7) single-walled carbon nanotubes (CNTs) with several nitrogen doping configurations and varying charge states. Pyridinic-nitrogen incorporation in CNTs is found to induce an increasing CO2 adsorption strength with electron injecting, leading to a highly selective CO2 adsorption in comparison with N2 . This functionality could induce intrinsically reversible CO2 adsorption as capture/release can be controlled by switching the charge carrying state of the system on/off. This phenomenon is verified for a number of different models and theoretical methods, with clear ramifications for the possibility of implementation with a broader class of graphene-based materials. A scheme for the implementation of this remarkable reversible electrocatalytic CO2 -capture phenomenon is considered.
Self-Supported Earth-Abundant Nanoarrays as Efficient and Robust Electrocatalysts for Energy-Related Reactions
Publisher: American Chemical Society (ACS)
Date: 13-06-2018
Spatial Structure Engineering of Interactive Single Platinum Sites toward Enhanced Electrocatalytic Hydrogen Evolution
Publisher: Wiley
Date: 20-10-2023
Mesoporous Co-O-C nanosheets for electrochemical production of hydrogen peroxide in acidic medium
Publisher: Royal Society of Chemistry (RSC)
Date: 2022
DOI: 10.1039/D1TA10416K
Abstract: Mesoporous Co–O–C nanosheets enabled highly active, stable, and selective H 2 O 2 electrosynthesis in acid. Practical application was demonstrated via the effective electro-Fenton degradation of organic pollutants for on-site/-demand water treatment.
Ionic liquid-assisted synthesis of N/S-double doped graphene microwires for oxygen evolution and Zn–air batteries
Publisher: Elsevier BV
Date: 11-2015
Activity origin and catalyst design principles for electrocatalytic hydrogen evolution on heteroatom-doped graphene
Publisher: Springer Science and Business Media LLC
Date: 12-09-2016
Molecular Scaffolding Strategy with Synergistic Active Centers To Facilitate Electrocatalytic CO2 Reduction to Hydrocarbon/Alcohol
Publisher: American Chemical Society (ACS)
Date: 12-2017
DOI: 10.1021/JACS.7B10817
Abstract: A major impediment to the electrocatalytic CO
Introduction
Publisher: Springer Science and Business Media LLC
Date: 14-03-2018
DOI: 10.1557/JMR.2018.40
Charge State Manipulation of Cobalt Selenide Catalyst for Overall Seawater Electrolysis
Publisher: Wiley
Date: 14-09-2018
Electrocatalytic CO2-to-C2+ with Ampere-Level Current on Heteroatom-Engineered Copper via Tuning *CO Intermediate Coverage
Publisher: American Chemical Society (ACS)
Date: 04-08-2022
DOI: 10.1021/JACS.2C06820
Abstract: An ere-level current density of CO
Assessment of nickel cermets and La0.8Sr0.2Sc0.2Mn0.8O3 as solid-oxide fuel cell anodes operating on carbon monoxide fuel
Publisher: Elsevier BV
Date: 03-2010
Stabilizing Cu2+ Ions by Solid Solutions to Promote CO2 Electroreduction to Methane
Publisher: American Chemical Society (ACS)
Date: 28-01-2022
DOI: 10.1021/JACS.1C12212
Abstract: Copper is the only metal catalyst that can perform the electrocatalytic CO
Graphene-encapsulated nickel–copper bimetallic nanoparticle catalysts for electrochemical reduction of CO2to CO
Publisher: Royal Society of Chemistry (RSC)
Date: 2020
DOI: 10.1039/D0CC04779A
Abstract: High CO selectivity for the CO 2 electroreduction reaction was achieved on Ni–Cu bimetallic catalysts. We observed that changing the Cu content in the catalysts causes charge redistribution which results in a negative correlation with CO selectivity.
Polydopamine-inspired nanomaterials for energy conversion and storage
Publisher: Royal Society of Chemistry (RSC)
Date: 2018
DOI: 10.1039/C8TA05245J
Abstract: This review highlights the intriguing physicochemical and structural versatility of PDA-based nanomaterials and their energy conversion and storage applications.
Triple-atom catalysts for one-step N–C–N coupling toward urea synthesis: A DFT study,DFT研究三单原子催化剂用于一步N–C–N偶联合成 尿素
Publisher: Springer Science and Business Media LLC
Date: 27-03-2023
Molecular Scalpel to Chemically Cleave Metal–Organic Frameworks for Induced Phase Transition
Publisher: American Chemical Society (ACS)
Date: 23-04-2021
DOI: 10.1021/JACS.1C02379
Artificially steering electrocatalytic oxygen evolution reaction mechanism by regulating oxygen defect contents in perovskites
Publisher: American Association for the Advancement of Science (AAAS)
Date: 29-07-2022
Abstract: The regulation of mechanism on the electrocatalysis process with multiple reaction pathways is more efficient and essential than conventional material engineering for the enhancement of catalyst performance. Here, by using oxygen evolution reaction (OER) as a model, which has an adsorbate evolution mechanism (AEM) and a lattice oxygen oxidation mechanism (LOM), we demonstrate a general strategy for steering the two mechanisms on various La x Sr 1− x CoO 3−δ . By delicately controlling the oxygen defect contents, the dominant OER mechanism on La x Sr 1− x CoO 3−δ can be arbitrarily transformed between AEM-LOM-AEM accompanied by a volcano-type activity variation trend. Experimental and computational evidence explicitly reveal that the phenomenon is due to the fact that the increased oxygen defects alter the lattice oxygen activity with a volcano-type trend and preserve the Co 0 state for preferably OER. Therefore, we achieve the co-optimization between the activity and stability of catalysts by altering the mechanism rather than a specific design of catalysts.
Boosting Alkaline Hydrogen Evolution Reaction through Water Structure Manipulation
Publisher: Wiley
Date: 11-07-2023
Abstract: In the past, the design of efficient electrocatalyst materials for alkaline hydrogen evolution reaction (HER) was mostly focused on tuning the adsorption properties of reaction intermediates. A recent breakthrough shows that the performance can be improved by manipulating water structure at the electrode‐electrolyte interface using atomically localized electric fields. The new approach was realized by using IrRu dizygotic single‐atom sites and led to a significantly accelerated water dissociation and an overall improved alkaline HER performance. Supported by extensive data from advanced modeling, characterization, and electrochemical measurements, the work delivers an intricate examination of the interaction between water molecules and the catalyst surface, thereby enriching our understanding of water dissociation kinetics and offering new insights to boost overall alkaline HER efficiency.
Toward design of synergistically active carbon-based catalysts for electrocatalytic hydrogen evolution
Publisher: American Chemical Society (ACS)
Date: 05-2014
DOI: 10.1021/NN501434A
IrOx·nH2O with lattice water–assisted oxygen exchange for high-performance proton exchange membrane water electrolyzers
Publisher: American Association for the Advancement of Science (AAAS)
Date: 23-06-2023
Abstract: The trade-off between activity and stability of oxygen evolution reaction (OER) catalysts in proton exchange membrane water electrolyzer (PEMWE) is challenging. Crystalline IrO 2 displays good stability but exhibits poor activity amorphous IrO x exhibits outstanding activity while sacrificing stability. Here, we combine the advantages of these two materials via a lattice water–incorporated iridium oxide (IrO x · n H 2 O) that has short-range ordered structure of hollandite-like framework. We confirm that IrO x · n H 2 O exhibits boosted activity and ultrahigh stability of hours (~8 months) with a record-high stability number of 1.9 × 10 7 n oxygen n Ir −1 . We evidence that lattice water is active oxygen species in sustainable and rapid oxygen exchange. The lattice water–assisted modified OER mechanism contributes to improved activity and concurrent stability with no apparent structural degradation, which is different to the conventional adsorbate evolution mechanism and lattice oxygen mechanism. We demonstrate that a high-performance PEMWE with IrO x · n H 2 O as anode electrocatalyst delivers a cell voltage of 1.77 V at 1 A cm −2 for 600 hours (60°C).
An effective strategy to boost lattice-oxygen-mediated acidic oxygen evolution
Publisher: Elsevier BV
Date: 07-2023
Natural DNA-assisted ultrafine FeP embedded in N, P-codoped carbons for efficient oxygen reduction, hydrogen evolution and rechargeable zinc-air battery
Publisher: Elsevier BV
Date: 2022
Engineering High‐Energy Interfacial Structures for High‐Performance Oxygen‐Involving Electrocatalysis
Publisher: Wiley
Date: 24-03-2017
Abstract: Engineering high-energy interfacial structures for high-performance electrocatalysis is achieved by chemical coupling of active CoO nanoclusters and high-index facet Mn
Intermediate Modulation on Noble Metal Hybridized to 2D Metal-Organic Framework for Accelerated Water Electrocatalysis
Publisher: Elsevier BV
Date: 09-2019
Engineering of Carbon-Based Electrocatalysts for Emerging Energy Conversion: From Fundamentality to Functionality
Publisher: Wiley
Date: 14-07-2015
Abstract: Over the past decade, developing advanced catalysts for clean and sustainable energy conversion has been subject to extensive study. Driven by great advances achieved in computational quantum chemistry, synthetic chemistry, and material characterization techniques, the preferential design of a most-appropriate catalyst for a specific electrochemical reaction is possible. Here a universal process for the design of high-performance carbon-based electrocatalysts, by engineering their intrinsic electronic structures and physical structures to promote their extrinsic activities for different energy conversion reactions, is presented and summarized. How such a powerful strategy may aid the discovery of more electrocatalysts for a sustainable and clean energy infrastructure is discussed.
Electrocatalytically Activating and Reducing N2 Molecule by Tuning Activity of Local Hydrogen Radical
Publisher: Wiley
Date: 12-04-2023
Abstract: Decarbonizing N 2 conversion is particularly challenging, but essential for sustainable development of industry and agriculture. Herein, we achieve electrocatalytic activation/reduction of N 2 on X/Fe−N−C (X=Pd, Ir and Pt) dual‐atom catalysts under ambient condition. We provide solid experimental evidence that local hydrogen radical (H*) generated on the X site of the X/Fe−N−C catalysts can participate in the activation/reduction of N 2 adsorbed on the Fe site. More importantly, we reveal that the reactivity of X/Fe−N−C catalysts for N 2 activation/reduction can be well adjusted by the activity of H* generated on the X site, i.e., the interaction between the X−H bond. Specifically, X/Fe−N−C catalyst with the weakest X−H bonding exhibits the highest H* activity, which is beneficial to the subsequent cleavage of X−H bond for N 2 hydrogenation. With the most active H*, the Pd/Fe dual‐atom site promotes the turnover frequency of N 2 reduction by up to 10 times compared with the pristine Fe site.
Carbene Ligands Enabled C–N Coupling for Methylamine Electrosynthesis: A Computational Study
Publisher: American Chemical Society (ACS)
Date: 27-06-2022
A nano-engineered graphene/carbon nitride hybrid for photocatalytic hydrogen evolution
Publisher: Elsevier BV
Date: 03-2016
Breaking the volcano-plot limits for Pt-based electrocatalysts by selective tuning adsorption of multiple intermediates
Publisher: Royal Society of Chemistry (RSC)
Date: 2019
DOI: 10.1039/C9TA02801C
Abstract: A new general strategy for breaking the limits imposed by volcano plots is proposed for the HER under alkaline conditions.
A Three-Component Nanocomposite with Synergistic Reactivity for Oxygen Reduction Reaction in Alkaline Solution
Publisher: Wiley
Date: 29-09-2015
Recent advances in direct seawater splitting for producing hydrogen
Publisher: Royal Society of Chemistry (RSC)
Date: 2023
DOI: 10.1039/D3CC02074F
Abstract: The recent progress in designing efficient direct seawater electrolysis systems is discussed in detail, including catalyst design, electrolyser assembly, membrane regulation, and electrolyte engineering.
Tailoring Selectivity of Electrochemical Hydrogen Peroxide Generation by Tunable Pyrrolic‐Nitrogen‐Carbon
Publisher: Wiley
Date: 17-04-2020
Efficient Nitrogen Fixation to Ammonia through Integration of Plasma Oxidation with Electrocatalytic Reduction
Publisher: Wiley
Date: 11-05-2021
Abstract: Present one‐step N 2 fixation is impeded by tough activation of the N≡N bond and low selectivity to NH 3 . Here we report fixation of N 2 ‐to‐NH 3 can be decoupled to a two‐step process with one problem effectively solved in each step, including: 1) facile activation of N 2 to NO x − by a non‐thermal plasma technique, and 2) highly selective conversion of NO x − to NH 3 by electrocatalytic reduction. Importantly, this process uses air and water as low‐cost raw materials for scalable ammonia production under ambient conditions. For NO x − reduction to NH 3 , we present a surface boron‐rich core–shell nickel boride electrocatalyst. The surface boron‐rich feature is the key to boosting activity, selectivity, and stability via enhanced NO x − adsorption, and suppression of hydrogen evolution and surface Ni oxidation. A significant ammonia production of 198.3 μmol cm −2 h −1 was achieved, together with nearly 100 % Faradaic efficiency.
Nanostructured Metal‐Free Electrochemical Catalysts for Highly Efficient Oxygen Reduction
Publisher: Wiley
Date: 15-08-2012
Abstract: Replacing precious and nondurable Pt catalysts with cheap and commercially available materials to facilitate sluggish cathodic oxygen reduction reaction (ORR) is a key issue in the development of fuel cell technology. The recently developed cost effective and highly stable metal-free catalysts reveal comparable catalytic activity and significantly better fuel tolerance than that of current Pt-based catalysts therefore, they can serve as feasible Pt alternatives for the next generation of ORR electrocatalysts. Their promising electrocatalytic properties and acceptable costs greatly promote the R&D of fuel cell technology. This review provides an overview of recent advances in state-of-the-art nanostructured metal-free electrocatalysts including nitrogen-doped carbons, graphitic-carbon nitride (g-C(3) N(4) )-based hybrids, and 2D graphene-based materials. A special emphasis is placed on the molecular design of these electrocatalysts, origin of their electrochemical reactivity, and ORR pathways. Finally, some perspectives are highlighted on the development of more efficient ORR electrocatalysts featuring high stability, low cost, and enhanced performance, which are the key factors to accelerate the commercialization of fuel cell technology.
Isolated Boron Sites for Electroreduction of Dinitrogen to Ammonia
Publisher: American Chemical Society (ACS)
Date: 02-01-2020
Understanding the sulphur-oxygen exchange process of metal sulphides prior to oxygen evolution reaction
Publisher: Springer Science and Business Media LLC
Date: 07-04-2023
DOI: 10.1038/S41467-023-37751-Y
Abstract: Dynamic reconstruction of metal sulphides during electrocatalytic oxygen evolution reaction (OER) has h ered the acquisition of legible evidence for comprehensively understanding the phase-transition mechanism and electrocatalytic activity origin. Herein, modelling on a series of cobalt-nickel bimetallic sulphides, we for the first time establish an explicit and comprehensive picture of their dynamic phase evaluation pathway at the pre-catalytic stage before OER process. By utilizing the in-situ electrochemical transmission electron microscopy and electron energy loss spectroscopy, the lattice sulphur atoms of (NiCo)S 1.33 particles are revealed to be partially substituted by oxygen from electrolyte to form a lattice oxygen-sulphur coexisting shell surface before the generation of reconstituted active species. Such S-O exchange process is benefitted from the subtle modulation of metal-sulphur coordination form caused by the specific Ni and Co occupation. This unique oxygen-substitution behaviour produces an (NiCo)O x S 1.33-x surface to reduce the energy barrier of surface reconstruction for converting sulphides into active oxy/hydroxide derivative, therefore significantly increasing the proportion of lattice oxygen-mediated mechanism compared to the pure sulphide surface. We anticipate this direct observation can provide an explicit picture of catalysts’ structural and compositional evolution during the electrocatalytic process.
Mesoporous hybrid material composed of Mn3O4nanoparticles on nitrogen-doped graphene for highly efficient oxygen reduction reaction
Publisher: Royal Society of Chemistry (RSC)
Date: 2013
DOI: 10.1039/C3CC43338B
Abstract: The hybrid material composed of Mn3O4 nanoparticles on nitrogen-doped graphene was prepared via a solvothermal process and investigated for the first time as a catalyst for oxygen reduction reaction (ORR). Its high ORR activity, excellent durability and tolerance to methanol make this hybrid material a promising candidate for highly efficient ORR in fuel cells and metal-air batteries.
Customizing the microenvironment of CO2 electrocatalysis via three‐phase interface engineering
Publisher: Wiley
Date: 03-2022
DOI: 10.1002/SMM2.1109
Abstract: Converting CO 2 into high‐value fuels and chemicals by renewable‐electricity‐powered electrochemical CO 2 reduction reaction (CRR) is a viable approach toward carbon‐emissions‐neutral processes. Unlike the thermocatalytic hydrogenation of CO 2 at the solid‐gas interface, the CRR takes place at the three‐phase gas/solid/liquid interface near the electrode surface in aqueous solution, which leads to major challenges including the limited mass diffusion of CO 2 reactant, competitive hydrogen evolution reaction, and poor product selectivity. Here we critically examine the various methods of surface and interface engineering of the electrocatalysts to optimize the microenvironment for CRR, which can address the above issues. The effective modification strategies for the gas transport, electrolyte composition, controlling intermediate states, and catalyst engineering are discussed. The key emphasis is made on the erse atomic‐precision modifications to increase the local CO 2 concentration, lower the energy barriers for CO 2 activation, decrease the H 2 O coverage, and stabilize intermediates to effectively control the catalytic activity and selectivity. The perspectives on the challenges and outlook for the future applications of three‐phase interface engineering for CRR and other gas‐involving electrocatalytic reactions conclude the article.
Mesoscale Diffusion Enhancement of Carbon-Bowl-Shaped Nanoreactor toward High-Performance Electrochemical H2 O2 Production
Publisher: American Chemical Society (ACS)
Date: 15-08-2021
Impact of Interfacial Electron Transfer on Electrochemical CO 2 Reduction on Graphitic Carbon Nitride/Doped Graphene
Publisher: Wiley
Date: 04-02-2019
Abstract: Effective electrocatalysts are required for the CO
Nickel ferrocyanide as a high-performance urea oxidation electrocatalyst
Publisher: Springer Science and Business Media LLC
Date: 20-09-2021
Graphitic carbon nitride materials: controllable synthesis and applications in fuel cells and photocatalysis
Publisher: Royal Society of Chemistry (RSC)
Date: 2012
DOI: 10.1039/C2EE03479D
A computational study on Pt and Ru dimers supported on graphene for the hydrogen evolution reaction: new insight into the alkaline mechanism
Publisher: Royal Society of Chemistry (RSC)
Date: 2019
DOI: 10.1039/C8TA11626A
Abstract: The dissociative chemisorption energy of water was proposed to address both thermodynamics and kinetics of alkaline hydrogen evolution.
Electrocatalytic Refinery for Sustainable Production of Fuels and Chemicals
Publisher: Wiley
Date: 10-03-2021
Abstract: Compared to modern fossil‐fuel‐based refineries, the emerging electrocatalytic refinery (e‐refinery) is a more sustainable and environmentally benign strategy to convert renewable feedstocks and energy sources into transportable fuels and value‐added chemicals. A crucial step in conducting e‐refinery processes is the development of appropriate reactions and optimal electrocatalysts for efficient cleavage and formation of chemical bonds. However, compared to well‐studied primary reactions (e.g., O 2 reduction, water splitting), the mechanistic aspects and materials design for emerging complex reactions are yet to be settled. To address this challenge, herein, we first present fundamentals of heterogeneous electrocatalysis and some primary reactions, and then implement these to establish the framework of e‐refinery by coupling in situ generated intermediates (integrated reactions) or products (tandem reactions). We also present a set of materials design principles and strategies to efficiently manipulate the reaction intermediates and pathways.
Identification of pH-dependent synergy on Ru/MoS2 interface: a comparison of alkaline and acidic hydrogen evolution
Publisher: Royal Society of Chemistry (RSC)
Date: 2017
DOI: 10.1039/C7NR06111K
Abstract: By comparing hydrogen evolution reaction (HER) activities of Ru/MoS 2 /CP in alkaline and acidic solutions, a pH-dependent synergy has been identified on the Ru/MoS 2 interface for superior alkaline HER efficiency.
Spatial-confinement induced electroreduction of CO and CO2 to diols on densely-arrayed Cu nanopyramids
Publisher: Royal Society of Chemistry (RSC)
Date: 2021
DOI: 10.1039/D1SC01694F
Abstract: Densely-arrayed Cu nanopyramids have spatial confinement induced by the additional Cu–O bond. This promotes C–C coupling, regulates post-C–C coupling, and retains both oxygen atoms in an alternative pathway toward ethylene glycol formation from CO.
Polydopamine-graphene oxide derived mesoporous carbon nanosheets for enhanced oxygen reduction
Publisher: Royal Society of Chemistry (RSC)
Date: 2015
DOI: 10.1039/C5NR03089G
Abstract: Composite materials combining nitrogen-doped carbon (NC) with active species represent a paramount breakthrough as alternative catalysts to Pt for the oxygen reduction reaction (ORR) due to their competitive activity, low cost and excellent stability. In this paper, a simple strategy is presented to construct graphene oxide-polydopamine (GD) based carbon nanosheets. This approach does not need to modify graphene and use any catalyst for polymerization under ambient conditions, and the obtained carbon nanosheets possess adjustable thicknesses and uniform mesoporous structures without using any template. The thickness of GD hybrids and the carbonization temperature are found to play crucial roles in adjusting the microstructure of the resulting carbon nanosheets and, accordingly their ORR catalytic activity. The optimized carbon nanosheet generated by a GD hybrid of 5 nm thickness after 900 °C carbonization exhibits superior ORR activity with an onset potential of -0.07 V and a kinetic current density of 13.7 mA cm(-2) at -0.6 V. The unique mesoporous structure, high surface areas, abundant defects and favorable nitrogen species are believed to significantly benefit the ORR catalytic process. Furthermore, it also shows remarkable durability and excellent methanol tolerance outperforming those of commercial Pt/C. In view of the physicochemical versatility and structural tunability of polydopamine (PDA) materials, our work would shed new light on the understanding and further development of PDA-based carbon materials for highly efficient electrocatalysts.
Local Environment Determined Reactant Adsorption Configuration for Enhanced Electrocatalytic Acetone Hydrogenation to Propane
Publisher: Wiley
Date: 16-12-2022
Abstract: We demonstrate a widely applicable method to alter the adsorption configuration of multi‐carbon containing reactants by no catalyst engineering but simply adjusting the local reaction environment of the catalyst surface. Using electrocatalytic acetone to propane hydrogenation (APH) as a model reaction and common commercial Pt/Pt‐based materials as catalysts, we found local H + concentration can significantly influence the adsorption mode of acetone reactant, for ex le, in vertical or flat mode, and target product selectivity. Electrocatalytic measurement combined with in situ spectroscopic characterizations reveals that the vertically adsorbed acetone is favorable for propane production while the flatly adsorbed mode suppresses the reaction. DFT calculations indicate that the H coverage on catalyst surface plays a decisive role in the adsorption configuration of acetone. The increased local acidity can facilitate the adsorption configuration of acetone from flat to vertical mode and suppress the competing hydrogen evaluation reaction, which consequently enhances the APH selectivity.
Facile Oxygen Reduction on a Three‐Dimensionally Ordered Macroporous Graphitic C3N4/Carbon Composite Electrocatalyst
Publisher: Wiley
Date: 02-03-2012
Abstract: Honeycomb catalysis: a facile oxygen reduction reaction has been observed on a graphitic C(3)N(4)/carbon catalyst with three-dimensional interconnected macropores (see picture with SiO(2) template). This material not only shows catalytic activity that is comparable to that of commercial Pt/C, but also has much higher organic-fuel tolerance and long-term stability.
Role of oxygen-bound reaction intermediates in selective electrochemical CO2 reduction
Publisher: Royal Society of Chemistry (RSC)
Date: 2021
DOI: 10.1039/D1EE00740H
Abstract: The review presents the important role of oxygen-bound intermediates in directing the selectivity of electrochemical CO 2 reduction by considering available theoretical calculations, electrochemical measurements and operando spectroscopy observations.
Communication between active sites regulates heterogeneous catalysis
Publisher: Elsevier BV
Date: 11-2022
Hydrogen evolution by a metal-free electrocatalyst
Publisher: Springer Science and Business Media LLC
Date: 28-04-2014
DOI: 10.1038/NCOMMS4783
Robust Ru-N metal-support interaction to promote self-powered H2 production assisted by hydrazine oxidation
Publisher: Elsevier BV
Date: 09-2022
Heteroatom-Doped Transition Metal Electrocatalysts for Hydrogen Evolution Reaction
Publisher: American Chemical Society (ACS)
Date: 26-02-2019
C2+ Selectivity for CO2 Electroreduction on Oxidized Cu-Based Catalysts
Publisher: American Chemical Society (ACS)
Date: 21-06-2023
DOI: 10.1021/JACS.3C03022
Synthesis and assessment of La0.8Sr0.2ScyMn1-yO3-delta as cathodes for solid-oxide fuel cells on scandium-stabilized zirconia electrolyte
Publisher: Elsevier BV
Date: 09-2008
Selectivity Control for Electrochemical CO2 Reduction by Charge Redistribution on the Surface of Copper Alloys
Publisher: American Chemical Society (ACS)
Date: 05-09-2019
Emerging materials and technologies for electrocatalytic seawater splitting
Publisher: American Association for the Advancement of Science (AAAS)
Date: 20-10-2023
A 2D metal-organic framework/Ni(OH)(2) heterostructure for an enhanced oxygen evolution reaction Electronic supplementary information (ESI) available. See DOI: 10.1039/c8nr09680e
Publisher: Royal Society of Chemistry (RSC)
Date: 2019
DOI: 10.1039/C8NR09680E
Abstract: Ni-BDC/Ni(OH) 2 hybrid nanosheets were fabricated and explored as a highly efficient electrocatalyst for the oxygen evolution reaction.
Surface and Interface Engineering in Copper-Based Bimetallic Materials for Selective CO2 Electroreduction
Publisher: Elsevier BV
Date: 08-2018
Highly enhanced hydrazine oxidation on bifunctional Ni tailored by alloying for energy-efficient hydrogen production
Publisher: Elsevier BV
Date: 12-2023
Strain Effect in Bimetallic Electrocatalysts in the Hydrogen Evolution Reaction
Publisher: American Chemical Society (ACS)
Date: 27-04-2018
Molecule-Level g-C3N4 Coordinated Transition Metals as a New Class of Electrocatalysts for Oxygen Electrode Reactions
Publisher: American Chemical Society (ACS)
Date: 27-02-2017
DOI: 10.1021/JACS.6B13100
Abstract: Organometallic complexes with metal-nitrogen/carbon (M-N/C) coordination are the most important alternatives to precious metal catalysts for oxygen reduction and evolution reactions (ORR and OER) in energy conversion devices. Here, we designed and developed a range of molecule-level graphitic carbon nitride (g-C
Enhanced electrochemical catalytic activity by copper oxide grown on nitrogen-doped reduced graphene oxide
Publisher: Royal Society of Chemistry (RSC)
Date: 2013
DOI: 10.1039/C3TA13299D
N-doping goes sp-hybridized
Publisher: Springer Science and Business Media LLC
Date: 21-08-2018
Direct seawater electrolysis by adjusting the local reaction environment of a catalyst
Publisher: Springer Science and Business Media LLC
Date: 30-01-2023
Recent Advances in Atomic Metal Doping of Carbon-based Nanomaterials for Energy Conversion
Publisher: Wiley
Date: 12-04-2017
Abstract: Nanostructured metal-contained catalysts are one of the most widely used types of catalysts applied to facilitate some of sluggish electrochemical reactions. However, the high activity of these catalysts cannot be sustained over a variety of pH ranges. In an effort to develop highly active and stable metal-contained catalysts, various approaches have been pursued with an emphasis on metal particle size reduction and doping on carbon-based supports. These techniques enhances the metal-support interactions, originating from the chemical bonding effect between the metal dopants and carbon support and the associated interface, as well as the charge transfer between the atomic metal species and carbon framework. This provides an opportunity to tune the well-defined metal active centers and optimize their activity, selectivity and stability of this type of (electro)catalyst. Herein, recent advances in synthesis strategies, characterization and catalytic performance of single atom metal dopants on carbon-based nanomaterials are highlighted with attempts to understand the electronic structure and spatial arrangement of in idual atoms as well as their interaction with the supports. Applications of these new materials in a wide range of potential electrocatalytic processes in renewable energy conversion systems are also discussed with emphasis on future directions in this active field of research.
Bronze alloys with tin surface sites for selective electrochemical reduction of CO2
Publisher: Royal Society of Chemistry (RSC)
Date: 2018
DOI: 10.1039/C8CC08066F
Abstract: Low concentration tin bronze alloys show high selectivity for CO 2 electroreduction to CO, while high concentration tin bronze alloys show high selectivity for formate.
Understanding the Roadmap for Electrochemical Reduction of CO2 to Multi-Carbon Oxygenates and Hydrocarbons on Copper-Based Catalysts
Publisher: American Chemical Society (ACS)
Date: 15-04-2019
DOI: 10.1021/JACS.9B02124
Abstract: Electrochemical reduction of CO
Carbon Solving Carbon's Problems: Recent Progress of Nanostructured Carbon-Based Catalysts for the Electrochemical Reduction of CO2
Publisher: Wiley
Date: 18-07-2017
Promotion of Electrocatalytic Hydrogen Evolution Reaction on Nitrogen-Doped Carbon Nanosheets with Secondary Heteroatoms
Publisher: American Chemical Society (ACS)
Date: 29-06-2017
Abstract: Dual heteroatom-doped carbon materials are efficient electrocatalysts via a synergistic effect. With nitrogen as the primary dopant, boron, sulfur, and phosphorus can be used as secondary elements for co-doped carbons. However, evaluation and analysis of the promotional effect of B, P, and S to N-doped carbons has not been widely researched. Here we report a robust platform that is constructed through polydopamine to prepare N,B-, N,P-, and N,S-co-doped carbon nanosheets, characterized by similar N species content and efficient B, P, and S doping. Systematic investigation reveals S to have the greatest promotional effect in hydrogen evolution reactions (HER) followed by P and that B decreases the activity of N-doped carbons. Experimental and theoretical analyses show the secondary heteroatom promotional effect is impacted by the intrinsic structures and extrinsic surface areas of both materials, i.e., electronic structures exclusively determine the catalytic activity of active sites, while large surface areas optimize apparent HER performance.
Metal-organic framework assisted synthesis of single-atom catalysts for energy applications
Publisher: Oxford University Press (OUP)
Date: 23-01-2018
DOI: 10.1093/NSR/NWY010
Nitrogen Vacancies on 2D Layered W2N3: A Stable and Efficient Active Site for Nitrogen Reduction Reaction
Publisher: Wiley
Date: 13-06-2019
Abstract: Electrochemical nitrogen reduction reaction (NRR) under ambient conditions provides an avenue to produce carbon-free hydrogen carriers. However, the selectivity and activity of NRR are still hindered by the sluggish reaction kinetics. Nitrogen Vacancies on transition metal nitrides are considered as one of the most ideal active sites for NRR by virtue of their unique vacancy properties such as appropriate adsorption energy to dinitrogen molecule. However, their catalytic performance is usually limited by the unstable feature. Herein, a new 2D layered W
Mechanism of C-N bonds formation in electrocatalytic urea production revealed by ab initio molecular dynamics simulation
Publisher: Springer Science and Business Media LLC
Date: 17-09-2022
DOI: 10.1038/S41467-022-33258-0
Abstract: Electrosynthesis of urea from CO 2 and NO X provides an exceptional opportunity for human society, given the increasingly available renewable energy. Urea electrosynthesis is challenging. In order to raise the overall electrosynthesis efficiency, the most critical reaction step for such electrosynthesis, C-N coupling, needs to be significantly improved. The C-N coupling can only happen at a narrow potential window, generally in the low overpotential region, and a fundamental understanding of the C-N coupling is needed for further development of this strategy. In this regard, we perform ab initio Molecular Dynamics simulations to reveal the origin of C-N coupling under a small electrode potential window with both the dynamic nature of water as a solvent, and the electrode potentials considered. We explore the key reaction networks for urea formation on Cu(100) surface in neutral electrolytes. Our work shows excellent agreement with experimentally observed selectivity under different potentials on the Cu electrode. We discover that the * NH and * CO are the key precursors for C-N bonds formation at low overpotential, while at high overpotential the C-N coupling occurs between adsorbed * NH and solvated CO. These insights provide vital information for future spectroscopic measurements and enable us to design new electrochemical systems for more value-added chemicals.
Study on oxygen activation and methane oxidation over La0.8Sr0.2MnO3 electrode in single-chamber solid oxide fuel cells via an electrochemical approach
Publisher: Elsevier BV
Date: 03-2012
Mesoporous MnCo2O4with abundant oxygen vacancy defects as high-performance oxygen reduction catalysts
Publisher: Royal Society of Chemistry (RSC)
Date: 2014
DOI: 10.1039/C4TA01672F
Two-Dimensional Mosaic Bismuth Nanosheets for Highly Selective Ambient Electrocatalytic Nitrogen Reduction
Publisher: American Chemical Society (ACS)
Date: 21-02-2019
Molten Salt-Directed Catalytic Synthesis of 2D Layered Transition-Metal Nitrides for Efficient Hydrogen Evolution
Publisher: Elsevier BV
Date: 09-2020
Soft‐Templating Synthesis of N‐Doped Mesoporous Carbon Nanospheres for Enhanced Oxygen Reduction Reaction
Publisher: Wiley
Date: 12-05-2015
Abstract: The development of ordered mesoporous carbon materials with controllable structures and improved physicochemical properties by doping heteroatoms such as nitrogen into the carbon framework has attracted a lot of attention, especially in relation to energy storage and conversion. Herein, a series of nitrogen-doped mesoporous carbon spheres (NMCs) was synthesized via a facile dual soft-templating procedure by tuning the nitrogen content and carbonization temperature. Various physical and (electro)chemical properties of the NMCs have been comprehensively investigated to pave the way for a feasible design of nitrogen-containing porous carbon materials. The optimized s le showed a favorable electrocatalytic activity as evidenced by a high kinetic current and positive onset potential for oxygen reduction reaction (ORR) due to its large surface area, high pore volume, good conductivity, and high nitrogen content, which make it a highly efficient ORR metal-free catalyst in alkaline solutions.
Origin of the Electrocatalytic Oxygen Reduction Activity of Graphene-Based Catalysts: A Roadmap to Achieve the Best Performance
Publisher: American Chemical Society (ACS)
Date: 11-03-2014
DOI: 10.1021/JA500432H
Polydopamine-Derived, In Situ N-Doped 3D Mesoporous Carbons for Highly Efficient Oxygen Reduction
Publisher: Wiley
Date: 06-03-2018
The Dynamic Formation from Metal-Organic Frameworks of High-Density Platinum Single-Atom Catalysts with Metal-Metal Interactions
Publisher: Wiley
Date: 27-10-2022
Abstract: Single‐atom catalysts (SACs) hold great promise for highly efficient heterogeneous catalysis, yet the practical applications require the development of high‐density active sites with flexible geometric structures. The lack of understanding in the dynamic formation process of single atoms in the host framework has been plaguing the controllable synthesis of next generation SACs. Here using Co‐based metal‐organic frameworks (MOFs) as a starting substrate, we fully elucidated the formation of high‐density Pt single atoms with inter‐site interactions in derived Co 3 O 4 host. The cation exchange process and dynamic evolution of Pt−Pt interactions, organic ligand cleavage and Pt‐oxygen coordination formation during the pyrolysis process have been unambiguously interpreted by a series of in situ/ex situ spectroscopic measurements and theoretical computation. These findings would direct the synthesis of high‐density SACs with metal‐metal interactions, which demonstrate significantly enhanced structural flexibility and catalytic properties.
Evaluation of Ba0.5Sr0.5Co0.8Fe0.2O3-delta as a potential cathode for an anode-supported proton-conducting solid-oxide fuel cell
Publisher: Elsevier BV
Date: 05-2008
Observation of Active Sites for Oxygen Reduction Reaction on Nitrogen-Doped Multilayer Graphene
Publisher: American Chemical Society (ACS)
Date: 03-06-2014
DOI: 10.1021/NN501506P
Abstract: Active sites and the catalytic mechanism of nitrogen-doped graphene in an oxygen reduction reaction (ORR) have been extensively studied but are still inconclusive, partly due to the lack of an experimental method that can detect the active sites. It is proposed in this report that the active sites on nitrogen-doped graphene can be determined via the examination of its chemical composition change before and after ORR. Synchrotron-based X-ray photoelectron spectroscopy analyses of three nitrogen-doped multilayer graphene s les reveal that oxygen reduction intermediate OH(ads), which should chemically attach to the active sites, remains on the carbon atoms neighboring pyridinic nitrogen after ORR. In addition, a high amount of the OH(ads) attachment after ORR corresponds to a high catalytic efficiency and vice versa. These pinpoint that the carbon atoms close to pyridinic nitrogen are the main active sites among the different nitrogen doping configurations.
Cr doping effect in B-site of La0.75Sr0.25MnO3 on its phase stability and performance as an SOFC anode
Publisher: Springer Science and Business Media LLC
Date: 24-07-2009
Nanoporous Graphitic-C3N4@Carbon Metal-Free Electrocatalysts for Highly Efficient Oxygen Reduction
Publisher: American Chemical Society (ACS)
Date: 29-11-2011
DOI: 10.1021/JA209206C
Abstract: Based on theoretical prediction, a g-C(3)N(4)@carbon metal-free oxygen reduction reaction (ORR) electrocatalyst was designed and synthesized by uniform incorporation of g-C(3)N(4) into a mesoporous carbon to enhance the electron transfer efficiency of g-C(3)N(4). The resulting g-C(3)N(4)@carbon composite exhibited competitive catalytic activity (11.3 mA cm(-2) kinetic-limiting current density at -0.6 V) and superior methanol tolerance compared to a commercial Pt/C catalyst. Furthermore, it demonstrated significantly higher catalytic efficiency (nearly 100% of four-electron ORR process selectivity) than a Pt/C catalyst. The proposed synthesis route is facile and low-cost, providing a feasible method for the development of highly efficient electrocatalysts.
Carbon-Based Electrochemical Oxygen Reduction and Hydrogen Evolution Catalysts
Publisher: Wiley
Date: 03-09-2018
The Crucial Role of Charge Accumulation and Spin Polarization in Activating Carbon-Based Catalysts for Electrocatalytic Nitrogen Reduction
Publisher: Wiley
Date: 03-02-2020
Abstract: Cost-effective carbon-based catalysts are promising for catalyzing the electrochemical N
Constructing tunable dual active sites on two-dimensional C3N4@MoN hybrid for electrocatalytic hydrogen evolution
Publisher: Elsevier BV
Date: 11-2018
Electrochemical Reduction of Carbon Dioxide to Solid Carbon: Development, Challenges, and Perspectives
Publisher: American Chemical Society (ACS)
Date: 17-08-2023
Integrating Interactive Noble Metal Single-Atom Catalysts into Transition Metal Oxide Lattices
Publisher: American Chemical Society (ACS)
Date: 07-12-2022
DOI: 10.1021/JACS.2C11374
Activation and Deactivation Kinetics of Oxygen Reduction over a La(0.8)Sr(0.2)Sc(0.1)Mn(0.9)O(3) Cathode
Publisher: American Chemical Society (ACS)
Date: 05-11-2008
DOI: 10.1021/JP806941D
Synthesis of Bandgap‐tunable Transition Metal Sulfides through Gas‐phase Cation Exchange‐induced Topological Transformation
Publisher: Wiley
Date: 24-03-2023
Abstract: Oriented synthesis of transition metal sulfides (TMSs) with controlled compositions and crystal structures has long been promising for electronic devices and energy applications. Liquid‐phase cation exchange (LCE) is a well‐studied route by varying the compositions. However, achieving crystal structure selectivity is still a great challenge. Here, we demonstrate gas‐phase cation exchange (GCE), which can induce a specific topological transformation (TT), for the synthesis of versatile TMSs with identified cubic or hexagonal crystal structures. The parallel six‐sided subunit (PSS), a new descriptor, is defined to describe the substitution of cations and the transition of the anion sublattice. Under this principle, the band gap of targeted TMSs can be tailored. Using the photocatalytic hydrogen evolution as an ex le, the optimal hydrogen evolution rate of a zinc‐cadmium sulfide (ZCS4) is determined to be 11.59 mmol h −1 g −1 , showing a 36.2‐fold improvement over CdS.
Facile Fabrication of Core–Shell‐Structured Ag@Carbon and Mesoporous Yolk–Shell‐Structured Ag@Carbon@Silica by an Extended Stöber Method
Publisher: Wiley
Date: 15-04-2013
Multifunctional Iron Oxide Nanoflake/Graphene Composites Derived from Mechanochemical Synthesis for Enhanced Lithium Storage and Electrocatalysis
Publisher: American Chemical Society (ACS)
Date: 29-06-2015
Abstract: Composites consisting of nanoparticles of iron oxides and graphene have attracted considerable attention in numerous applications however, the synthesis methods used to achieve superior functionalities are often complex and unamenable to low-cost large-scale industrial production. Here, we report our findings in exploring a simple strategy for low-cost fabrication of multifunctional composites with enhanced properties. In particular, we have successfully prepared FeO(OH) nanoflake/graphene and nano-Fe3O4/graphene composites from commercially available Fe powders and graphite oxides using a simple and low-cost solid-state process, where the metallic Fe is converted to FeO(OH) nanoflake and graphite oxide is reduced/exfoliated to graphene. The resultant nano-Fe3O4/graphene composite is multifunctional, demonstrates specific capacities of 802 and 629 mA h g(-1), respectively, at 1000 and 2000 mA g(-1) as an electrode material for lithium-ion batteries (LIBs), and also displays efficient catalytic activity for both oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) the nominal overpotentials are lower than those for previously reported metal-based catalysts (e.g., IrO2, RuO2, and Pt/C). The dramatically enhanced properties are attributed to the synergistic mechanochemical coupling effects between iron oxide and graphene introduced by the facile process, which is well suited for large-scale cost-effective fabrication.
Charge-Redistribution-Enhanced Nanocrystalline Ru@IrOx Electrocatalysts for Oxygen Evolution in Acidic Media
Publisher: Elsevier BV
Date: 02-2019
Electronic and Structural Engineering of Carbon-Based Metal-Free Electrocatalysts for Water Splitting
Publisher: Wiley
Date: 10-2019
Abstract: Since first being reported as possible electrocatalysts to substitute platinum for the oxygen reduction reaction (ORR), carbon-based metal-free nanomaterials have been considered a class of promising low-cost materials for clean and sustainable energy-conversion reactions. However, beyond the ORR, the development of carbon-based catalysts for other electrocatalytic reactions is still limited. More importantly, the intrinsic activity of most carbon-based metal-free catalysts is inadequate compared to their metal-based counterparts. To address this challenge, more design strategies are needed in order to improve the overall performance of carbon-based materials. Herein, using water splitting as an ex le, some state-of-the-art strategies in promoting carbon-based nanomaterials are summarized, including graphene, carbon nanotubes, and graphitic-carbon nitride, as highly active electrocatalysts for hydrogen evolution and oxygen evolution reactions. It is shown that by rationally tuning the electronic and/or physical structure of the carbon nanomaterials, adsorption of reaction intermediates is optimized, consequently improving the apparent electrocatalytic performance. These strategies may facilitate the development in this area and lead to the discovery of advanced carbon-based nanomaterials for various applications in energy-conversion processes.
Synergistic catalysis between atomically dispersed Fe and a pyrrolic-N-C framework for CO2 electroreduction
Publisher: Royal Society of Chemistry (RSC)
Date: 2019
DOI: 10.1039/C9NH00361D
Abstract: Atomically dispersed Fe immobilized within N-doped carbon nanosheets was synthesized. The synergistic effect between the metal atom and its anchoring framework sites has been investigated for efficient CO 2 reduction.
Free-standing single-crystalline NiFe-hydroxide nanoflake arrays: a self-activated and robust electrocatalyst for oxygen evolution
Publisher: Royal Society of Chemistry (RSC)
Date: 2018
DOI: 10.1039/C7CC08843D
Abstract: A strategy for engineering single-crystalline nanoarrays is presented as an effective way to manipulate the catalytic activity and operational stability of NiFe-hydroxide.
Engineering surface atomic structure of single-crystal cobalt (II) oxide nanorods for superior electrocatalysis
Publisher: Springer Science and Business Media LLC
Date: 21-09-2016
DOI: 10.1038/NCOMMS12876
Abstract: Engineering the surface structure at the atomic level can be used to precisely and effectively manipulate the reactivity and durability of catalysts. Here we report tuning of the atomic structure of one-dimensional single-crystal cobalt (II) oxide (CoO) nanorods by creating oxygen vacancies on pyramidal nanofacets. These CoO nanorods exhibit superior catalytic activity and durability towards oxygen reduction/evolution reactions. The combined experimental studies, microscopic and spectroscopic characterization, and density functional theory calculations reveal that the origins of the electrochemical activity of single-crystal CoO nanorods are in the oxygen vacancies that can be readily created on the oxygen-terminated {111} nanofacets, which favourably affect the electronic structure of CoO, assuring a rapid charge transfer and optimal adsorption energies for intermediates of oxygen reduction/evolution reactions. These results show that the surface atomic structure engineering is important for the fabrication of efficient and durable electrocatalysts.
Correction: Mesoporous hybrid material composed of Mn3O4 nanoparticles on nitrogen-doped graphene for highly efficient oxygen reduction reaction
Publisher: Royal Society of Chemistry (RSC)
Date: 2016
DOI: 10.1039/C6CC90177H
Abstract: Correction for ‘Mesoporous hybrid material composed of Mn 3 O 4 nanoparticles on nitrogen-doped graphene for highly efficient oxygen reduction reaction’ by Jingjing Duan et al., Chem. Commun. , 2013, 49 , 7705–7707.
Surface and Interface Engineering of Noble-Metal-Free Electrocatalysts for Efficient Energy Conversion Processes
Publisher: American Chemical Society (ACS)
Date: 16-02-2017
DOI: 10.1021/ACS.ACCOUNTS.6B00635
Abstract: Developing cost-effective and high-performance electrocatalysts for renewable energy conversion and storage is motivated by increasing concerns regarding global energy security and creating sustainable technologies dependent on inexpensive and abundant resources. Recent achievements in the design and synthesis of efficient non-precious-metal and even non-metal electrocatalysts make the replacement of noble metal counterparts for the hydrogen evolution reaction (HER), oxygen evolution reaction (OER), and oxygen reduction reaction (ORR) with earth-abundant elements, for ex le, C, N, Fe, Mn, and Co, a realistic possibility. It has been found that surface atomic engineering (e.g., heteroatom-doping) and interface atomic or molecular engineering (e.g., interfacial bonding) can induce novel physicochemical properties and strong synergistic effects for electrocatalysts, providing new and efficient strategies to greatly enhance the catalytic activities. In this Account, we discuss recent progress in the design and fabrication of efficient electrocatalysts based on carbon materials, graphitic carbon nitride, and transition metal oxides or hydroxides for efficient ORR, OER, and HER through surface and interfacial atomic and molecular engineering. Atomic and molecular engineering of carbon materials through heteroatom doping with one or more elements of noticeably different electronegativities can maximally tailor their electronic structures and induce a synergistic effect to increase electrochemical activity. Nonetheless, the electrocatalytic performance of chemically modified carbonaceous materials remains inferior to that of their metallic counterparts, which is mainly due to the relatively limited amount of electrocatalytic active sites induced by heteroatom doping. Accordingly, coupling carbon substrates with other active electrocatalysts to produce composite structures can impart novel physicochemical properties, thereby boosting the electroactivity even further. Although the majority of carbon-based materials remain uncompetitive with state-of-the-art metal-based catalysts for the aforementioned catalytic processes, non-metal carbon hybrids have already shown performance that typically only conventional noble metals or transition metal materials can achieve. The idea of hybridized carbon-based catalysts possessing unique active surfaces and macro- or nanostructures is addressed herein. For metal-carbon couples, the incorporation of carbon can effectively compensate for the intrinsic deficiency in conductivity of the metallic components. Chemical modification of carbon frameworks, such as nitrogen doping, not only can change the electron-donor character, but also can introduce anchoring sites for immobilizing active metallic centers to form metal-nitrogen-carbon (M-N-C) species, which are thought to facilitate the electrocatalytic process. With thoughtful material design, control over the porosity of composites, the molecular architecture of active metal moieties and macromorphologies of the whole catalysts can be achieved, leading to a better understanding structure-activity relationships. We hope that we can offer new insight into material design, particularly the role of chemical composition and structural properties in electrochemical performance and reaction mechanisms.
Syngas production from electrocatalytic CO2 reduction with high energetic efficiency and current density
Publisher: Royal Society of Chemistry (RSC)
Date: 2019
DOI: 10.1039/C9TA01932D
Abstract: The direct conversion of CO 2 to syngas with controllable composition remains an intense interest for the production of renewable fuels.
Key to C2 production: selective C–C coupling for electrochemical CO2 reduction on copper alloy surfaces
Publisher: Royal Society of Chemistry (RSC)
Date: 2021
DOI: 10.1039/D1CC03796J
Abstract: The OC–COH coupling is kinetically facilitated compared to OC–CHO coupling, which is induced by the optimized composition and electronic structures of copper alloys.
Electrochemical Nitrogen Reduction: Identification and Elimination of Contamination in Electrolyte
Publisher: American Chemical Society (ACS)
Date: 14-08-2019
Significant Enhancement of Water Splitting Activity of N‐Carbon Electrocatalyst by Trace Level Co Doping
Publisher: Wiley
Date: 06-2016
Abstract: Replacement of precious metal electrocatalysts with highly active and cost efficient alternatives for complete water splitting at low voltage has attracted a growing attention in recent years. Here, this study reports a carbon-based composite co-doped with nitrogen and trace amount of metallic cobalt (1 at%) as a bifunctional electrocatalyst for water splitting at low overpotential and high current density. An excellent electrochemical activity of the newly developed electrocatalyst originates from its graphitic nanostructure and highly active Co-Nx sites. In the case of carefully optimized s le of this electrocatalyst, 10 mA cm(-2) current density can be achieved for two half reactions in alkaline solutions-hydrogen evolution reaction and oxygen evolution reaction-at low overpotentials of 220 and 350 mV, respectively, which are smaller than those previously reported for nonprecious metal and metal-free counterparts. Based on the spectroscopic and electrochemical investigations, the newly identified Co-Nx sites in the carbon framework are responsible for high electrocatalytic activity of the Co,N-doped carbon. This study indicates that a trace level of the introduced Co into N-doped carbon can significantly enhance its electrocatalytic activity toward water splitting.
Regulating Ru active sites by Pd alloying to significantly enhance hydrazine oxidation for energy-saving hydrogen production
Publisher: Royal Society of Chemistry (RSC)
Date: 2023
DOI: 10.1039/D3TA02238B
Abstract: Ultrafine RuPd nanoalloy on carbon was facilely prepared with outstanding activity for the HER and HzOR, benefitting from bifunctional Ru active sites tailored by Pd alloying.
Selectivity roadmap for electrochemical CO2 reduction on copper-based alloy catalysts
Publisher: Elsevier BV
Date: 05-2020
Metal-metal interactions in correlated single-atom catalysts
Publisher: American Association for the Advancement of Science (AAAS)
Date: 29-04-2022
Abstract: Single-atom catalysts (SACs) include a promising family of electrocatalysts with unique geometric structures. Beyond conventional ones with fully isolated metal sites, an emerging class of catalysts with the adjacent metal single atoms exhibiting intersite metal-metal interactions appear in recent years and can be denoted as correlated SACs (C-SACs). This type of catalysts provides more opportunities to achieve substantial structural modification and performance enhancement toward a wider range of electrocatalytic applications. On the basis of a clear identification of metal-metal interactions, this review critically examines the recent research progress in C-SACs. It shows that the control of metal-metal interactions enables regulation of atomic structure, local coordination, and electronic properties of metal single atoms, which facilitate the modulation of electrocatalytic behavior of C-SACs. Last, we outline directions for future work in the design and development of C-SACs, which is indispensable for creating high-performing new SAC architectures.
Applications of Rare Earth Promoted Transition Metal Sulfides in Electrocatalysis†
Publisher: Wiley
Date: 21-04-2023
Abstract: With the rapid consumption of fossil fuels and the resulting environmental problems, researchers are working to find sustainable alternative energy and energy storage and conversion methods. Transition metal sulfur compounds have attracted extensive attention due to their excellent electrical conductivity, low cost, adjustable components and good electrocatalytic performance. As an alternative to noble metal catalysts, they have emerged as a promising electrocatalyst. However, their low catalytic activity and poor stability limit their large‐scale practical applications. Rare earth elements, known as industrial vitamins, are widely used in various fields due to their special redox properties, oxygen affinity and electronic structure. Therefore, the construction of rare earth promoted transition metal sulfides is of far‐reaching significance for the development of catalysts. Here, we review the applications of various rare earth promoted transition metal sulfides in energy storage and conversion in recent years, which focuses on three ways in rare earth promoted transition metal sulfide, including doping, interfacial modification engineering and structural facilitation. As well, these materials are used in electrochemical reactions such as OER, HER, ORR, CO 2 RR, and so on, in order to explore the important role of rare earth in the field of electrocatalysis, the future challenges and opportunities.
Controlled synthesis of ultrasmall RuP2 particles on N,P-codoped carbon as superior pH-wide electrocatalyst for hydrogen evolution
Publisher: Springer Science and Business Media LLC
Date: 21-01-2021
Directed Urea‐to‐Nitrite Electrooxidation via Tuning Intermediate Adsorption on Co, Ge Co‐Doped Ni Sites
Publisher: Wiley
Date: 16-03-2023
Abstract: The electrochemical urea oxidation reaction (UOR) is an alternative to electrooxidation of water for energy–saving hydrogen (H 2 ) production. To maximize this purpose, design of catalysts for selective urea‐to‐nitrite (NO 2 – ) electrooxidation with increased electron transfer and high current is practically important. Herein, a cobalt, germanium (Co, Ge) co‐doped nickel (Ni) oxyhydroxide catalyst is reported first time that directs urea‐to‐NO 2 – conversion with a significant Faradaic efficiency of 84.9% at 1.4 V versus reversible hydrogen electrode and significantly boosts UOR activity to 448.0 mA cm −2 . Importantly, this performance is greater than for most reported Ni‐based catalysts. Based on judiciously combined synchrotron‐based measurement, in situ spectroscopy and density functional theoretical computation, significantly boosted urea‐to‐NO 2 – production results from Co, Ge co‐doping is demonstrated that optimizes electronic structure of Ni sites in which urea adsorption is altered as NO‐terminal configuration to facilitate CN cleavage for *NH formation, and thereby expedites pathway for urea to NO 2 – conversion. Findings highlight the importance of tuning intermediate adsorption behavior for design of high‐performance UOR electrocatalysts, and will be of practical benefit to a range of researchers and manufacturers in replacing conventional water electrooxidation with UOR for energy‐saving H 2 production.
Graphene oxide-polydopamine derived N, S-codoped carbon nanosheets as superior bifunctional electrocatalysts for oxygen reduction and evolution
Publisher: Elsevier BV
Date: 2016
Electrocatalytic Refinery for Sustainable Production of Fuels and Chemicals
Publisher: Wiley
Date: 10-03-2021
Abstract: Compared to modern fossil‐fuel‐based refineries, the emerging electrocatalytic refinery (e‐refinery) is a more sustainable and environmentally benign strategy to convert renewable feedstocks and energy sources into transportable fuels and value‐added chemicals. A crucial step in conducting e‐refinery processes is the development of appropriate reactions and optimal electrocatalysts for efficient cleavage and formation of chemical bonds. However, compared to well‐studied primary reactions (e.g., O 2 reduction, water splitting), the mechanistic aspects and materials design for emerging complex reactions are yet to be settled. To address this challenge, herein, we first present fundamentals of heterogeneous electrocatalysis and some primary reactions, and then implement these to establish the framework of e‐refinery by coupling in situ generated intermediates (integrated reactions) or products (tandem reactions). We also present a set of materials design principles and strategies to efficiently manipulate the reaction intermediates and pathways.
Co (II) Boron Imidazolate Framework with Rigid Auxiliary Linkers for Stable Electrocatalytic Oxygen Evolution Reaction
Publisher: Wiley
Date: 18-03-2019
Abstract: Metal–organic frameworks (MOFs) have significant potential for practical application in catalysis. However, many MOFs are shown to be sensitive to aqueous solution. This severely limits application of MOFs in electrocatalytic operations for energy production and storage. Here, a Co (II) boron imidazolate framework CoB(im) 4 (ndc) 0.5 ( BIF‐91 , im = imidazolate, ndc = 2,6‐naphthalenedicarboxylate) that is rationally designed and successfully tested for electrocatalytic application in strong alkaline (pH ≈ 14) solution is reported. In such a BIF system, the inherent carboxylate species segment large channel spaces into multiple domains in which each single channel is filled with ndc ligands through the effect of zeolite channel confinement. These ligands, with strong CH···π interaction, act as a rigid auxiliary linker to significantly enhance the structural stability of the BIF‐91 framework. Additionally, the π‐conjugated effect in BIF‐91 stabilizes dopant Fe (III) at the atomic scale to construct Fe‐immobilized BIF‐91 ( Fe@BIF‐91 ). Due to the synergistic effect between Fe (III) guest and Co (II) in the framework, the Fe@BIF‐91 acts as an active and stable electrocatalyst for the oxygen evolution reaction in alkaline solution.
Short-Range Ordered Iridium Single Atoms Integrated into Cobalt Oxide Spinel Structure for Highly Efficient Electrocatalytic Water Oxidation
Publisher: American Chemical Society (ACS)
Date: 25-03-2021
DOI: 10.1021/JACS.1C01525
Strategies for design of electrocatalysts for hydrogen evolution under alkaline conditions
Publisher: Elsevier BV
Date: 06-2020
Natural DNA-derived highly-graphitic N, P, S-tridoped carbon nanosheets for multiple electrocatalytic applications
Publisher: Elsevier BV
Date: 02-2022
Ethylene Electrooxidation to 2-Chloroethanol in Acidic Seawater with Natural Chloride Participation
Publisher: American Chemical Society (ACS)
Date: 03-07-2023
DOI: 10.1021/JACS.3C05114
Advancing the Electrochemistry of the Hydrogen‐Evolution Reaction through Combining Experiment and Theory
Publisher: Wiley
Date: 10-11-2014
Abstract: The electrocatalytic hydrogen‐evolution reaction (HER), as the main step of water splitting and the cornerstone of exploring the mechanism of other multi‐electron transfer electrochemical processes, is the subject of extensive studies. A large number of high‐performance electrocatalysts have been developed for HER accompanied by recent significant advances in exploring its electrochemical nature. Herein we present a critical appraisal of both theoretical and experimental studies of HER electrocatalysts with special emphasis on the electronic structure, surface (electro)chemistry, and molecular design. It addresses the importance of correlating theoretical calculations and electrochemical measurements toward better understanding of HER electrocatalysis at the atomic level. Fundamental concepts in the computational quantum chemistry and its relation to experimental electrochemistry are also presented along with some featured ex les.
Two‐Step Boron and Nitrogen Doping in Graphene for Enhanced Synergistic Catalysis
Publisher: Wiley
Date: 22-01-2013
Determination of the Electron Transfer Number for the Oxygen Reduction Reaction: From Theory to Experiment
Publisher: American Chemical Society (ACS)
Date: 21-06-2016
Boosting Alkaline Hydrogen Evolution Reaction through Water Structure Manipulation
Publisher: Wiley
Date: 11-07-2023
Abstract: In the past, the design of efficient electrocatalyst materials for alkaline hydrogen evolution reaction (HER) was mostly focused on tuning the adsorption properties of reaction intermediates. A recent breakthrough shows that the performance can be improved by manipulating water structure at the electrode‐electrolyte interface using atomically localized electric fields. The new approach was realized by using IrRu dizygotic single‐atom sites and led to a significantly accelerated water dissociation and an overall improved alkaline HER performance. Supported by extensive data from advanced modeling, characterization, and electrochemical measurements, the work delivers an intricate examination of the interaction between water molecules and the catalyst surface, thereby enriching our understanding of water dissociation kinetics and offering new insights to boost overall alkaline HER efficiency.
Direct Growth of Well-Aligned MOF Arrays onto Various Substrates
Publisher: Elsevier BV
Date: 06-2017
High Electrocatalytic Hydrogen Evolution Activity of an Anomalous Ruthenium Catalyst
Publisher: American Chemical Society (ACS)
Date: 06-12-2016
DOI: 10.1021/JACS.6B11291
Abstract: Hydrogen evolution reaction (HER) is a critical process due to its fundamental role in electrocatalysis. Practically, the development of high-performance electrocatalysts for HER in alkaline media is of great importance for the conversion of renewable energy to hydrogen fuel via photoelectrochemical water splitting. However, both mechanistic exploration and materials development for HER under alkaline conditions are very limited. Precious Pt metal, which still serves as the state-of-the-art catalyst for HER, is unable to guarantee a sustainable hydrogen supply. Here we report an anomalously structured Ru catalyst that shows 2.5 times higher hydrogen generation rate than Pt and is among the most active HER electrocatalysts yet reported in alkaline solutions. The identification of new face-centered cubic crystallographic structure of Ru nanoparticles was investigated by high-resolution transmission electron microscopy imaging, and its formation mechanism was revealed by spectroscopic characterization and theoretical analysis. For the first time, it is found that the Ru nanocatalyst showed a pronounced effect of the crystal structure on the electrocatalytic activity tested under different conditions. The combination of electrochemical reaction rate measurements and density functional theory computation shows that the high activity of anomalous Ru catalyst in alkaline solution originates from its suitable adsorption energies to some key reaction intermediates and reaction kinetics in the HER process.
Polydopamine-Inspired, Dual Heteroatom-Doped Carbon Nanotubes for Highly Efficient Overall Water Splitting
Publisher: Wiley
Date: 29-12-2017
Engineering 2D Metal-Organic Framework/MoS Interface for Enhanced Alkaline Hydrogen Evolution.
Publisher: Wiley
Date: 03-03-2019
Abstract: 2D metal-organic frameworks (MOFs) have been widely investigated for electrocatalysis because of their unique characteristics such as large specific surface area, tunable structures, and enhanced conductivity. However, most of the works are focused on oxygen evolution reaction. There are very limited numbers of reports on MOFs for hydrogen evolution reaction (HER), and generally these reported MOFs suffer from unsatisfactory HER activities. In this contribution, novel 2D Co-BDC/MoS
Transition-Metal-Doped RuIr Bifunctional Nanocrystals for Overall Water Splitting in Acidic Environments.
Publisher: Wiley
Date: 27-02-2019
Abstract: The establishment of electrocatalysts with bifunctionality for efficient oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) in acidic environments is necessary for the development of proton exchange membrane (PEM) water electrolyzers for the production of clean hydrogen fuel. RuIr alloy is considered to be a promising electrocatalyst because of its favorable OER performance and potential for HER. Here, the design of a bifunctional electrocatalyst with greatly boosted water‐splitting performance from doping RuIr alloy nanocrystals with transition metals that modify electronic structure and binding strength of reaction intermediates is reported. Significantly, Co‐RuIr results in small overpotentials of 235 mV for OER and 14 mV for HER (@ 10 mA cm −2 current density) in 0.1 m HClO 4 media. Therefore a cell voltage of just 1.52 V is needed for overall water splitting to produce hydrogen and oxygen. More importantly, for a series of M‐RuIr (M = Co, Ni, Fe), the catalytic activity dependence at fundamental level on the chemical/valence states is used to establish a novel composition‐activity relationship. This permits new design principles for bifunctional electrocatalysts.
Less‐Coordinated Atomic Copper‐Dimer Boosted Carbon–Carbon Coupling During Electrochemical CO2 Reduction
Publisher: Wiley
Date: 20-04-2023
Abstract: This work reports a metal–organic framework (MOF) with less‐coordinated copper dimers, which displays excellent electrochemical CO 2 reduction (eCO 2 RR) performance with an advantageous current density of 0.9 A cm −2 and a high Faradaic efficiency of 71% to C 2 products. In comparison with MOF with Cu monomers that are present as Cu 1 O 4 with a coordination number of 3.8 ± 0.2, Cu dimers exist as O 3 Cu 1 ···Cu 2 O 2 with a coordination number of 2.8 ± 0.1. In situ characterizations together with theoretical calculations reveal that two *CO intermediates are stably adsorbed on each site of less‐coordinated Cu dimers, which favors later dimerization via a key intermediate of *CH 2 CHO. The highly unsaturated dual‐atomic Cu provides large‐quantity and high‐quality actives sites for carbon–carbon coupling, achieving the optimal trade‐off between activity and selectivity of eCO 2 RR to C 2 products.
Boosting urea electrooxidation on oxyanion-engineered nickel sites via inhibited water oxidation
Publisher: Springer Science and Business Media LLC
Date: 20-09-2023
Recent Progress of 3d Transition Metal Single-Atom Catalysts for Electrochemical CO2 Reduction
Publisher: Wiley
Date: 31-12-2021
Identifying the roles of Ru single atoms and nanoclusters for energy-efficient hydrogen production assisted by electrocatalytic hydrazine oxidation
Publisher: Elsevier BV
Date: 04-2023
Regulating Electrocatalysts via Surface and Interface Engineering for Acidic Water Electrooxidation
Publisher: American Chemical Society (ACS)
Date: 08-10-2019
Direct seawater splitting to hydrogen by a membrane electrolyzer
Publisher: Elsevier BV
Date: 2023
Initialization of a methane-fueled single-chamber solid-oxide fuel cell with NiO plus SDC anode and BSCF plus SDC cathode
Publisher: Elsevier BV
Date: 05-2008
A boron imidazolate framework with mechanochromic and electrocatalytic properties
Publisher: Royal Society of Chemistry (RSC)
Date: 2018
DOI: 10.1039/C8MH00859K
Abstract: An alkaline-stable anionic Cd( ii ) boron imidazolate framework ( BIF-89 ) not only exhibits unique mechanochromic behavior, but also shows an enhanced oxygen evolution reaction (OER) catalytic activity due to the presence of uncoordinated −COO groups able to capture Fe at the atomic level.
A new symmetric solid-oxide fuel cell with La0.8Sr0.2Sc0.2Mn0.8O3-delta perovskite oxide as both the anode and cathode
Publisher: Elsevier BV
Date: 02-2009
Single-Crystal Nitrogen-Rich Two-Dimensional Mo5N6 Nanosheets for Efficient and Stable Seawater Splitting
Publisher: American Chemical Society (ACS)
Date: 29-11-2018
Abstract: Transition metal nitrides (TMNs) have great potential for energy-related electrocatalysis because of their inherent electronic properties. However, incorporating nitrogen into a transition metal lattice is thermodynamically unfavorable, and therefore most of the developed TMNs are deficient in nitrogen. Consequently, these TMNs exhibit poor structural stability and unsatisfactory performance for electrocatalytic applications. In this work, we design and synthesize an atomically thin nitrogen-rich nanosheets, Mo
Efficient Nitrogen Fixation to Ammonia through Integration of Plasma Oxidation with Electrocatalytic Reduction
Publisher: Wiley
Date: 11-05-2021
Abstract: Present one‐step N 2 fixation is impeded by tough activation of the N≡N bond and low selectivity to NH 3 . Here we report fixation of N 2 ‐to‐NH 3 can be decoupled to a two‐step process with one problem effectively solved in each step, including: 1) facile activation of N 2 to NO x − by a non‐thermal plasma technique, and 2) highly selective conversion of NO x − to NH 3 by electrocatalytic reduction. Importantly, this process uses air and water as low‐cost raw materials for scalable ammonia production under ambient conditions. For NO x − reduction to NH 3 , we present a surface boron‐rich core–shell nickel boride electrocatalyst. The surface boron‐rich feature is the key to boosting activity, selectivity, and stability via enhanced NO x − adsorption, and suppression of hydrogen evolution and surface Ni oxidation. A significant ammonia production of 198.3 μmol cm −2 h −1 was achieved, together with nearly 100 % Faradaic efficiency.
A simple strategy for tridoped porous carbon nanosheet as superior electrocatalyst for bifunctional oxygen reduction and hydrogen evolution reactions
Publisher: Elsevier BV
Date: 06-2020
The Hydrogen Evolution Reaction in Alkaline Solution: From Theory, Single Crystal Models, to Practical Electrocatalysts.
Publisher: Wiley
Date: 14-05-2018
Abstract: The hydrogen evolution reaction (HER) is a fundamental process in electrocatalysis and plays an important role in energy conversion for the development of hydrogen-based energy sources. However, the considerably slow rate of the HER in alkaline conditions has hindered advances in water splitting techniques for high-purity hydrogen production. Differing from well documented acidic HER, the mechanistic aspects of alkaline HER are yet to be settled. A critical appraisal of alkaline HER electrocatalysis is presented, with a special emphasis on the connection between fundamental surface electrochemistry on single-crystal models and the derived molecular design principle for real-world electrocatalysts. By presenting some typical ex les across theoretical calculations, surface characterization, and electrochemical experiments, we try to address some key ongoing debates to deliver a better understanding of alkaline HER at the atomic level.
Anomalous hydrogen evolution behavior in high-pH environment induced by locally generated hydronium ions
Publisher: Springer Science and Business Media LLC
Date: 25-10-2019
DOI: 10.1038/S41467-019-12773-7
Abstract: Most fundamental studies of electrocatalysis are based on the experimental and simulation results obtained for bulk model materials. Some of these mechanistic understandings are inapplicable for more active nanostructured electrocatalysts. Herein, considering the simplest and most typical electrocatalytic process, the hydrogen evolution reaction, an alternative reaction mechanism is proposed for nanomaterials based on the identification of a new intermediate, which differs from those commonly known for the bulk counterparts. In-situ Raman spectroscopy and electrochemical thermal/kinetic measurements were conducted on a series of nanomaterials under different conditions. In high-pH electrolytes with negligible hydronium (H 3 O + ) concentration in bulk phase, massive H 3 O + intermediates are found generating on the catalytic surface during water dissociation and hydrogen adsorption processes. These H 3 O + intermediates create a unique acid-like local reaction environment on nanostructured catalytic surfaces and cut the energy barrier of the overall reaction. Such phenomena on nanostructured electrocatalysts explain their widely observed anomalously high activity under high-pH conditions.
Highly active nickel–cobalt/nanocarbon thin films as efficient water splitting electrodes
Publisher: Royal Society of Chemistry (RSC)
Date: 2016
DOI: 10.1039/C6NR06961D
Abstract: Developing low cost, highly active and stable electrocatalysts for both the hydrogen evolution reaction (HER) and the oxygen evolution reaction (OER) using the same electrolyte has remained a major challenge. Herein, we report a novel and robust material comprised of nickel-cobalt nanoparticles coated on a porous nitrogen-doped carbon (NC) thin film synthesized via a two-step pulsed laser deposition technique. The optimized s le (Ni
Molecular Cleavage of Metal‐Organic Frameworks and Application to Energy Storage and Conversion
Publisher: Wiley
Date: 04-10-2021
Abstract: The physicochemical properties of metal‐organic frameworks (MOFs) significantly depend on composition, topology, and porosity, which can be tuned via synthesis. In addition to a classic direct synthesis, postsynthesis modulations of MOFs, including ion exchange, installation, and destruction, can significantly expand the application. Because of a limitation of the qualitative hard and soft acids and bases (HSAB) theory, posttreatment permits regulation of MOF structure by cleaving chemical bonds at the molecular level. Here, methods of coordination bond scission to tailor the structure are critically appraised and the application to energy storage and conversion is assessed. MOF structures synthesized by molecular‐level coordination bond cleavage are described and the corresponding MOFs for electrocatalysis and renewable battery applications are evaluated. Significant emphasis is placed on various coordination bond cleavage to tune properties, including chemical groups, electronic structures, and morphologies. The review concludes with a critical perspective on practical application, together with challenges and future outlook for this emerging field.
Oxidation Stability of Nanographite Materials
Publisher: Wiley
Date: 21-05-2013
Design of electrocatalysts for oxygen- and hydrogen-involving energy conversion reactions
Publisher: Royal Society of Chemistry (RSC)
Date: 2015
DOI: 10.1039/C4CS00470A
Abstract: This review provides insights into theoretical and experimental electrochemistry toward a better understanding of a series of key energy conversion reactions.
Nickel Ferrocyanide as High-Performance Next Generation Electrocatalyst for Urea Oxidation
Publisher: Research Square Platform LLC
Date: 10-09-2020
DOI: 10.21203/RS.3.RS-67358/V1
Abstract: Urea oxidation, a key process in energy and environmental science, faces challenges because of the insufficient understanding of its mechanism and the lack of efficient catalysts. Here we demonstrate that nickel ferrocyanide (Ni 2 Fe(CN) 6 ) molecular catalyst supported on Ni form can drive urea oxidation reaction (UOR) with the record electrochemical activity and stability among all supported catalysts reported so far. A combination of kinetics data, in-situ spectroscopic measurements and energy computations suggests a new UOR pathway that delivers such outstanding performance. Different from most studied Ni-based catalysts with NiOOH derivative as a real catalytically active site for UOR, Ni 2 Fe(CN) 6 appears to be a next-generation catalyst able to directly facilitate a two-step reaction pathway involving a critical reaction of intermediate ammonia’s production (on Ni site) and oxidation (on Fe site). Due to the alternative rate-determining step with a more favorable thermal energetics, Ni 2 Fe(CN) 6 broke the limiting activity of the reported so far UOR catalysts. As a result, the UOR process on Ni 2 Fe(CN) 6 can replace conventional water oxidation process in various energy-saving systems for hydrogen and hydrogen peroxide production.
Building Up a Picture of the Electrocatalytic Nitrogen Reduction Activity of Transition Metal Single-Atom Catalysts
Publisher: American Chemical Society (ACS)
Date: 30-05-2019
DOI: 10.1021/JACS.9B03811
Abstract: The lack of chemical understanding and efficient catalysts impedes the development of electrocatalytic nitrogen reduction reaction (eNRR) for ammonia production. In this work, we employed density functional theory calculations to build up a picture (activity trends, electronic origins, and design strategies) of single-atom catalysts (SACs) supported on nitrogen-doped carbons as eNRR electrocatalysts. To construct such a picture, this work presents systematic studies of the eNRR activity of SACs covering 20 different transition metal (TM) centers coordinated by nitrogen atoms contained in three types of nitrogen-doped carbon substrates, which gives 60 SACs. Our study shows that the intrinsic activity trends could be established on the basis of the nitrogen adatom adsorption energy (Δ E
C3 production from CO2 reduction by concerted *CO trimerization on a single-atom alloy catalyst
Publisher: Royal Society of Chemistry (RSC)
Date: 2021
DOI: 10.1039/D1TA09608G
Abstract: Embedding Ag single atoms onto densely arrayed Cu nanopyramids could optimize the *CO adsorption strength toward direct propanediol production via a one-step concerted *CO trimerization mechanism.
Boosting electrocatalytic CO2–to–ethanol production via asymmetric C–C coupling
Publisher: Springer Science and Business Media LLC
Date: 29-06-2022
DOI: 10.1038/S41467-022-31427-9
Abstract: Electroreduction of carbon dioxide (CO 2 ) into multicarbon products provides possibility of large-scale chemicals production and is therefore of significant research and commercial interest. However, the production efficiency for ethanol (EtOH), a significant chemical feedstock, is impractically low because of limited selectivity, especially under high current operation. Here we report a new silver–modified copper–oxide catalyst (dCu 2 O/Ag 2.3% ) that exhibits a significant Faradaic efficiency of 40.8% and energy efficiency of 22.3% for boosted EtOH production. Importantly, it achieves CO 2 –to–ethanol conversion under high current operation with partial current density of 326.4 mA cm −2 at −0.87 V vs reversible hydrogen electrode to rank highly significantly amongst reported Cu–based catalysts. Based on in situ spectra studies we show that significantly boosted production results from tailored introduction of Ag to optimize the coordinated number and oxide state of surface Cu sites, in which the * CO adsorption is steered as both atop and bridge configuration to trigger asymmetric C–C coupling for stablization of EtOH intermediates.
Emerging Two-Dimensional Nanomaterials for Electrocatalysis
Publisher: American Chemical Society (ACS)
Date: 19-03-2018
DOI: 10.1021/ACS.CHEMREV.7B00689
Abstract: Over the past few decades, the design and development of advanced electrocatalysts for efficient energy conversion technologies have been subjects of extensive study. With the discovery of graphene, two-dimensional (2D) nanomaterials have emerged as some of the most promising candidates for heterogeneous electrocatalysts due to their unique physical, chemical, and electronic properties. Here, we review 2D-nanomaterial-based electrocatalysts for selected electrocatalytic processes. We first discuss the unique advances in 2D electrocatalysts based on different compositions and functions followed by specific design principles. Following this overview, we discuss various 2D electrocatalysts for electrocatalytic processes involved in the water cycle, carbon cycle, and nitrogen cycle from their fundamental conception to their functional application. We place a significant emphasis on different engineering strategies for 2D nanomaterials and the influence these strategies have on intrinsic material performance, such as electronic properties and adsorption energetics. Finally, we feature the opportunities and challenges ahead for 2D nanomaterials as efficient electrocatalysts. By considering theoretical calculations, surface characterization, and electrochemical tests, we describe the fundamental relationships between electronic structure, adsorption energy, and apparent activity for a wide variety of 2D electrocatalysts with the goal of providing a better understanding of these emerging nanomaterials at the atomic level.
Co (II) Boron Imidazolate Framework with Rigid Auxiliary Linkers for Stable Electrocatalytic Oxygen Evolution Reaction
Publisher: Wiley
Date: 08-2019
An organic-inorganic hybrid strategy to fabricate highly dispersed Fe2C in porous N-Doped carbon for oxygen reduction reaction and rechargeable zinc-air battery
Publisher: Elsevier BV
Date: 08-2022
Electrochemical Reduction of CO 2 to Ethane through Stabilization of an Ethoxy Intermediate
Publisher: Wiley
Date: 25-05-2020
Abstract: Electrochemical conversion of CO 2 into ethane is seldom observed because of the generally higher selectivity towards methane, ethylene, and ethanol. Consequently, little experimental evidence for its reaction mechanism exists and thus remains largely unknown. Now, by combining electrochemistry with in situ X‐ray absorption fine‐structure and in situ Raman techniques, iodide‐derived copper (ID‐Cu) and oxide‐derived copper (OD‐Cu) systems were studied to obtain a deeper understanding of the CO 2 to ethane mechanism. With trace iodine species on the surface and positively charged Cu species, production of ethane is significantly more favored on ID‐Cu compared to OD‐Cu, with higher selectivity and faster kinetics. For the first time, it is experimentally found that the formation of ethane follows the same pathway to ethylene and ethanol, and better stabilization of the late stage ethoxy intermediate can steer the reaction to ethane over ethanol.
Mild Methane Electrochemical Oxidation Boosted via Plasma Pre-Activation
Publisher: Wiley
Date: 11-07-2023
Abstract: Obtaining partial methane oxidation reaction (MOR) with various oxygenates via a mild electrochemical method is practically difficult because of activation of stable C─H bond and consequent reaction pathway regulation. Here, a real‐time tandem MOR with cascaded plasma and electrocatalysis to activate and convert the methane (CH 4 ) synergistically is reported for the first time. Boosted CH 4 conversion is demonstrated toward value‐added products including, alcohols, carboxylates, and ketone via use of commercial Pd‐based electrocatalysts. Compared with hash industrial processes, a mild condition, that is, anode potential 1.0 V versus RHE (reversible hydrogen electrode) is used that mitigates overoxidation of oxygenates and obviates competing reaction(s). One evidence that Pd(II) sites and surface adsorbed hydroxyls are important in facilitating activated‐CH 4 species conversion, and establish a reaction mechanism for conversion(s) that involves coupling reactions between adsorbed hydroxyls, carbon monoxide and C 1 /C 2 alkyls. One conclude that pre‐activation is important in boosting electrochemical partial MOR under mild conditions and will be of benefit in the development of sustainable CH 4 conversion technology.
Well-crystallized mesoporous samaria-doped ceria from EDTA-citrate complexing process with in situ created NiO as recyclable template
Publisher: Elsevier BV
Date: 02-2010
Stabilizing Oxidation State of SnO2 for Highly Selective CO2 Electroreduction to Formate at Large Current Densities
Publisher: American Chemical Society (ACS)
Date: 16-02-2023
Characterization and optimization of La(0.8)Sr(0.2)Sc(0.1)Mn(0.9)O(3-delta)-based composite electrodes for intermediate-temperature solid-oxide fuel cells
Publisher: Elsevier BV
Date: 12-2008
Dynamic rhenium dopant boosts ruthenium oxide for durable oxygen evolution
Publisher: Springer Science and Business Media LLC
Date: 21-01-2023
DOI: 10.1038/S41467-023-35913-6
Abstract: Heteroatom-doping is a practical means to boost RuO 2 for acidic oxygen evolution reaction (OER). However, a major drawback is conventional dopants have static electron redistribution. Here, we report that Re dopants in Re 0.06 Ru 0.94 O 2 undergo a dynamic electron accepting-donating that adaptively boosts activity and stability, which is different from conventional dopants with static dopant electron redistribution. We show Re dopants during OER, (1) accept electrons at the on-site potential to activate Ru site, and (2) donate electrons back at large overpotential and prevent Ru dissolution. We confirm via in situ characterizations and first-principle computation that the dynamic electron-interaction between Re and Ru facilitates the adsorbate evolution mechanism and lowers adsorption energies for oxygen intermediates to boost activity and stability of Re 0.06 Ru 0.94 O 2 . We demonstrate a high mass activity of 500 A g cata. −1 (7811 A g Re-Ru −1 ) and a high stability number of S-number = 4.0 × 10 6 n oxygen n Ru −1 to outperform most electrocatalysts. We conclude that dynamic dopants can be used to boost activity and stability of active sites and therefore guide the design of adaptive electrocatalysts for clean energy conversions.
Pulsed laser deposition of porous N-carbon supported cobalt (oxide) thin films for highly efficient oxygen evolution
Publisher: Royal Society of Chemistry (RSC)
Date: 2016
DOI: 10.1039/C6CC04776A
Abstract: A robust porous N-carbon supported cobalt (oxide) film has been developed by pulsed laser deposition as a highly efficient OER electrode.
Activating cobalt(II) oxide nanorods for efficient electrocatalysis by strain engineering
Publisher: Springer Science and Business Media LLC
Date: 15-11-2017
DOI: 10.1038/S41467-017-01872-Y
Abstract: Designing high-performance and cost-effective electrocatalysts toward oxygen evolution and hydrogen evolution reactions in water–alkali electrolyzers is pivotal for large-scale and sustainable hydrogen production. Earth-abundant transition metal oxide-based catalysts are particularly active for oxygen evolution reaction however, they are generally considered inactive toward hydrogen evolution reaction. Here, we show that strain engineering of the outermost surface of cobalt(II) oxide nanorods can turn them into efficient electrocatalysts for the hydrogen evolution reaction. They are competitive with the best electrocatalysts for this reaction in alkaline media so far. Our theoretical and experimental results demonstrate that the tensile strain strongly couples the atomic, electronic structure properties and the activity of the cobalt(II) oxide surface, which results in the creation of a large quantity of oxygen vacancies that facilitate water dissociation, and fine tunes the electronic structure to weaken hydrogen adsorption toward the optimum region.
Tailoring Acidic Oxygen Reduction Selectivity on Single-Atom Catalysts via Modification of First and Second Coordination Spheres
Publisher: American Chemical Society (ACS)
Date: 13-05-2021
DOI: 10.1021/JACS.1C03135
Controlling the Cation Exsolution of Perovskite to Customize Heterostructure Active Site for Oxygen Evolution Reaction.
Publisher: American Chemical Society (ACS)
Date: 27-05-2022
Abstract: Perovskite oxides are an important class of oxygen evolution reaction (OER) catalysts offering an ordered atomic arrangement and a highly flexible electronic structure. Currently, understanding and adjusting the dynamic reconstruction of perovskite during the OER process remains a formidable challenge. Here, we report the artificial construction of a heterostructure by the cation exsolution of perovskite to control the active site formation and reconstruction. The deliberately made La deficiency in LaNiO
Plasma‐electrified up‐carbonization for low‐carbon clean energy
Publisher: Wiley
Date: 26-09-2022
DOI: 10.1002/CEY2.260
Abstract: Low‐value, renewable, carbon‐rich resources, with different biomass feedstocks and their derivatives as typical ex les, represent virtually inexhaustive carbon sources and carbon‐related energy on Earth. Upon conversion to higher‐value forms (referred to as “up‐carbonization” here), these abundant feedstocks provide viable opportunities for energy‐rich fuels and sustainable platform chemicals production. However, many of the current methods for such up‐carbonization still lack sufficient energy, cost, and material efficiency, which affect their economics and carbon‐emissions footprint. With external electricity precisely delivered, discharge plasmas enable many stubborn reactions to occur under mild conditions, by creating locally intensified and highly reactive environments. This technology emerges as a novel, versatile technology platform for integrated or stand‐alone conversion of carbon‐rich resources. The plasma‐based processes are compatible for integration with increasingly abundant and cost‐effective renewable electricity, making the whole conversion carbon‐neutral and further paving the plasma‐electrified up‐carbonization to be performance‐, environment‐, and economics‐viable. Despite the chief interest in this emerging area, no review article brings together the state‐of‐the‐art results from erse disciplines and underlies basic mechanisms and chemistry underpinned. As such, this review aims to fill this gap and provide basic guidelines for future research and transformation, by providing an overview of the application of plasma techniques for carbon‐rich resource conversion, with particular focus on the perspective of discharge plasmas, the fundamentals of why plasmas are particularly suited for up‐carbonization, and featured ex les of plasma‐enabled resource valorization. With parallels drawn and specificity highlighted, we also discuss the technique shortcomings, current challenges, and research needs for future work.
Electrocatalytic Refinery of Biomass-Based 5-Hydroxymethylfurfural to Fine Chemicals
Publisher: American Chemical Society (ACS)
Date: 10-08-2023
Directing the selectivity of CO2 electroreduction to target C2 products via non-metal doping on Cu surfaces
Publisher: Royal Society of Chemistry (RSC)
Date: 2021
DOI: 10.1039/D0TA11604A
Abstract: Understanding the late stages of C 2 pathways provides great opportunities for fully achieving a selective CO 2 electroreduction. The C 2 product selectivity can be directed by the active site's oxygen affinity on a range of non-metal doped Cu surfaces.
NiO as a Bifunctional Promoter for RuO2 toward Superior Overall Water Splitting
Publisher: Wiley
Date: 15-03-2018
Abstract: Conventional development of nanomaterials for efficient electrocatalysis is largely based on performance-oriented trial-and-error/iterative approaches, while a rational design approach at the atomic/molecular level is yet to be found. Here, inspired by a fundamental understanding of the mechanism for both oxygen and hydrogen evolution half reactions (OER/HER), a unique strategy is presented to engineer RuO
Electrochemical CO2 reduction in membrane-electrode assemblies
Publisher: Elsevier BV
Date: 03-2022
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View Funded ActivityLinkage Infrastructure, Equipment And Facilities - Grant ID: LE210100109
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Amount: $240,000.00
Funder: Australian Research Council
View Funded ActivityDiscovery Projects - Grant ID: DP190103472
Start Date: 2019
End Date: 12-2023
Amount: $350,000.00
Funder: Australian Research Council
View Funded ActivityLinkage Infrastructure, Equipment And Facilities - Grant ID: LE210100153
Start Date: 2021
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View Funded ActivityDiscovery Projects - Grant ID: DP170104464
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Amount: $410,500.00
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View Funded ActivityARC Future Fellowships - Grant ID: FT200100062
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End Date: 07-2025
Amount: $800,000.00
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End Date: 02-2031
Amount: $35,000,000.00
Funder: Australian Research Council
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