ORCID Profile
0000-0003-1531-2966
Current Organisation
University of Sydney
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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)
Functional materials | Bioinorganic chemistry | Materials engineering | Catalysis and mechanisms of reactions | Agriculture, Land and Farm Management | Catalytic Process Engineering | Catalysis and Mechanisms of Reactions | Chemical Engineering Design | Electrochemistry | Physical Chemistry (Incl. Structural) | Electrochemistry | Inorganic chemistry | Nanofabrication growth and self assembly | Physical chemistry | Sustainable Agricultural Development | Plasma Physics; Fusion Plasmas; Electrical Discharges | Solid state chemistry | Electrochemical energy storage and conversion
ANZSRC Socio-Economic Objective (SEO)
Management of Greenhouse Gas Emissions from Energy Activities (excl. Electricity Generation) | Chemical Fertilisers | Hydrogen Storage | Energy Storage (excl. Hydrogen) | Expanding Knowledge in the Chemical Sciences |
Related Links
Publications
Direct Detection of Electron Transfer Reactions Underpinning the Tin-Catalyzed Electrochemical Reduction of CO2 using Fourier-Transformed ac Voltammetry
Publisher: American Chemical Society (ACS)
Date: 23-06-2017
Constraining CO coverage on copper promotes high-efficiency ethylene electroproduction
Publisher: Springer Science and Business Media LLC
Date: 11-11-2019
Electrochemical upgrade of CO2 from amine capture solution
Publisher: Springer Science and Business Media LLC
Date: 07-12-2020
Materials and system design for direct electrochemical CO2 conversion in capture media
Publisher: Royal Society of Chemistry (RSC)
Date: 2021
DOI: 10.1039/D1TA02751D
Abstract: Integration of upstream CO 2 capture and downstream electrochemical conversion by direct electrolysis of CO 2 capture media offers a potential solution to energy- and cost-efficient utilisation of CO 2 .
Catalyst synthesis under CO2 electroreduction favours faceting and promotes renewable fuels electrosynthesis
Publisher: Springer Science and Business Media LLC
Date: 16-12-2019
Fabrication of ultra-fine nanostructures using edge transfer printing
Publisher: Royal Society of Chemistry (RSC)
Date: 2012
DOI: 10.1039/C2NR11829G
Abstract: The exploration of new methods and techniques for application in erse fields, such as photonics, microfluidics, biotechnology and flexible electronics is of increasing scientific and technical interest for multiple uses over distance of 10-100 nm. This article discusses edge transfer printing--a series of unconventional methods derived from soft lithography for nanofabrication. It possesses the advantages of easy fabrication, low-cost and great serviceability. In this paper, we show how to produce exposed edges and use various materials for edge transfer printing, while nanoskiving, nanotransfer edge printing and tunable cracking for nanogaps are introduced. Besides this, different functional materials, such as metals, inorganic semiconductors and polymers, as well as localised heating and charge patterning, are described here as unconventional "inks" for printing. Edge transfer printing, which can effectively produce sub-100 nm scale ultra-fine structures, has broad applications, including metallic nanowires as nanoelectrodes, semiconductor nanowires for chemical sensors, heterostructures of organic semiconductors, plasmonic devices and so forth.
Polyethylenimine promoted electrocatalytic reduction of CO2to CO in aqueous medium by graphene-supported amorphous molybdenum sulphide
Publisher: Royal Society of Chemistry (RSC)
Date: 2016
DOI: 10.1039/C5EE02879E
Abstract: Amorphous molybdenum sulphide immobilized on polyethylenimine modified reduced graphene oxide can catalyse the electroreduction of CO 2 to CO or “syngas” in aqueous media with high efficiency.
Electrohydrogenation of Carbon Dioxide using a Ternary Pd/Cu2O–Cu Catalyst
Publisher: Wiley
Date: 03-09-2019
Abstract: A simple one-pot method has been developed to synthesize a palladium/cuprous oxide-copper (Pd/Cu
Efficient electrocatalytic conversion of carbon monoxide to propanol using fragmented copper
Publisher: Springer Science and Business Media LLC
Date: 11-02-2019
Enhanced multi-carbon alcohol electroproduction from CO via modulated hydrogen adsorption
Publisher: Springer Science and Business Media LLC
Date: 23-07-2020
DOI: 10.1038/S41467-020-17499-5
Abstract: Multi-carbon alcohols such as ethanol are valued as fuels in view of their high energy density and ready transport. Unfortunately, the selectivity toward alcohols in CO 2 /CO electroreduction is diminished by ethylene production, especially when operating at high current densities ( mA cm −2 ). Here we report a metal doping approach to tune the adsorption of hydrogen at the copper surface and thereby promote alcohol production. Using density functional theory calculations, we screen a suite of transition metal dopants and find that incorporating Pd in Cu moderates hydrogen adsorption and assists the hydrogenation of C 2 intermediates, providing a means to favour alcohol production and suppress ethylene. We synthesize a Pd-doped Cu catalyst that achieves a Faradaic efficiency of 40% toward alcohols and a partial current density of 277 mA cm −2 from CO electroreduction. The activity exceeds that of prior reports by a factor of 2.
Structure‐Based Enhanced Capacitance: In Situ Growth of Highly Ordered Polyaniline Nanorods on Reduced Graphene Oxide Patterns
Publisher: Wiley
Date: 19-01-2012
Efficient upgrading of CO to C3 fuel using asymmetric C-C coupling active sites
Publisher: Springer Science and Business Media LLC
Date: 29-11-2019
DOI: 10.1038/S41467-019-13190-6
Abstract: The electroreduction of C 1 feedgas to high-energy-density fuels provides an attractive avenue to the storage of renewable electricity. Much progress has been made to improve selectivity to C 1 and C 2 products, however, the selectivity to desirable high-energy-density C 3 products remains relatively low. We reason that C 3 electrosynthesis relies on a higher-order reaction pathway that requires the formation of multiple carbon-carbon (C-C) bonds, and thus pursue a strategy explicitly designed to couple C 2 with C 1 intermediates. We develop an approach wherein neighboring copper atoms having distinct electronic structures interact with two adsorbates to catalyze an asymmetric reaction. We achieve a record n -propanol Faradaic efficiency (FE) of (33 ± 1)% with a conversion rate of (4.5 ± 0.1) mA cm −2 , and a record n -propanol cathodic energy conversion efficiency (EE cathodic half-cell ) of 21%. The FE and EE cathodic half-cell represent a 1.3× improvement relative to previously-published CO-to- n -propanol electroreduction reports.
Recent advances in the nanoengineering of electrocatalysts for CO2reduction
Publisher: Royal Society of Chemistry (RSC)
Date: 2018
DOI: 10.1039/C7NR09620H
Abstract: Go nano, go active: the performance of catalysts for electrocatalytic CO 2 reduction can be improved by a range of nanoengineering strategies. Through these strategies, the catalyst's morphology, electronic structures and surrounding environment are finely tuned on a nanoscale.
Copper adparticle enabled selective electrosynthesis of n-propanol
Publisher: Springer Science and Business Media LLC
Date: 05-11-2018
DOI: 10.1038/S41467-018-07032-0
Abstract: The electrochemical reduction of carbon monoxide is a promising approach for the renewable production of carbon-based fuels and chemicals. Copper shows activity toward multi-carbon products from CO reduction, with reaction selectivity favoring two-carbon products however, efficient conversion of CO to higher carbon products such as n-propanol, a liquid fuel, has yet to be achieved. We hypothesize that copper adparticles, possessing a high density of under-coordinated atoms, could serve as preferential sites for n-propanol formation. Density functional theory calculations suggest that copper adparticles increase CO binding energy and stabilize two-carbon intermediates, facilitating coupling between adsorbed *CO and two-carbon intermediates to form three-carbon products. We form adparticle-covered catalysts in-situ by mediating catalyst growth with strong CO chemisorption. The new catalysts exhibit an n-propanol Faradaic efficiency of 23% from CO reduction at an n-propanol partial current density of 11 mA cm −2 .
High‐Rate and Selective CO2 Electrolysis to Ethylene via Metal–Organic‐Framework‐Augmented CO2 Availability
Publisher: Wiley
Date: 16-11-2022
Abstract: High‐rate conversion of carbon dioxide (CO 2 ) to ethylene (C 2 H 4 ) in the CO 2 reduction reaction (CO 2 RR) requires fine control over the phase boundary of the gas diffusion electrode (GDE) to overcome the limit of CO 2 solubility in aqueous electrolytes. Here, a metal–organic framework (MOF)‐functionalized GDE design is presented, based on a catalysts:MOFs:hydrophobic substrate materials layered architecture, that leads to high‐rate and selective C 2 H 4 production in flow cells and membrane electrode assembly (MEA) electrolyzers. It is found that using electroanalysis and operando X‐ray absorption spectroscopy (XAS), MOF‐induced organic layers in GDEs augment the local CO 2 concentration near the active sites of the Cu catalysts. MOFs with different CO 2 adsorption abilities are used, and the stacking ordering of MOFs in the GDE is varied. While sputtering Cu on poly(tetrafluoroethylene) (PTFE) (Cu/PTFE) exhibits 43% C 2 H 4 Faradaic efficiency (FE) at a current density of 200 mA cm − 2 in a flow cell, 49% C 2 H 4 FE at 1 A cm − 2 is achieved on MOF‐augmented GDEs in CO 2 RR. MOF‐augmented GDEs are further evaluated in an MEA electrolyzer, achieving a C 2 H 4 partial current density of 220 mA cm −2 for CO 2 RR and 121 mA cm −2 for the carbon monoxide reduction reaction (CORR), representing 2.7‐fold and 15‐fold improvement in C 2 H 4 production rate, compared to those obtained on bare Cu/PTFE.
Enhanced Nitrate-to-Ammonia Activity on Copper–Nickel Alloys via Tuning of Intermediate Adsorption
Publisher: American Chemical Society (ACS)
Date: 02-03-2020
DOI: 10.1021/JACS.9B13347
A metal-supported single-atom catalytic site enables carbon dioxide hydrogenation
Publisher: Springer Science and Business Media LLC
Date: 10-02-2022
DOI: 10.1038/S41467-022-28456-9
Abstract: Nitrogen-doped graphene-supported single atoms convert CO 2 to CO, but fail to provide further hydrogenation to methane – a finding attributable to the weak adsorption of CO intermediates. To regulate the adsorption energy, here we investigate the metal-supported single atoms to enable CO 2 hydrogenation. We find a copper-supported iron-single-atom catalyst producing a high-rate methane. Density functional theory calculations and in-situ Raman spectroscopy show that the iron atoms attract surrounding intermediates and carry out hydrogenation to generate methane. The catalyst is realized by assembling iron phthalocyanine on the copper surface, followed by in-situ formation of single iron atoms during electrocatalysis, identified using operando X-ray absorption spectroscopy. The copper-supported iron-single-atom catalyst exhibits a CO 2 -to-methane Faradaic efficiency of 64% and a partial current density of 128 mA cm −2 , while the nitrogen-doped graphene-supported one produces only CO. The activity is 32 times higher than a pristine copper under the same conditions of electrolyte and bias.
Interfacial energy band engineered CsPbBr3/NiFe-LDH heterostructure catalysts with tunable visible light driven photocatalytic CO2 reduction capability
Publisher: Royal Society of Chemistry (RSC)
Date: 2023
DOI: 10.1039/D2CY01982E
Abstract: CsPbBr 3 /NiFe-LDH heterostructure photocatalysts are developed with tuneable Z-scheme reduction capability for efficient CO 2 reduction performance.
A comprehensive biomedical variant catalogue based on whole genome sequences of 582 dogs and eight wolves
Publisher: Wiley
Date: 05-09-2019
DOI: 10.1111/AGE.12834
Promoting electrocatalytic CO2 methanation using a molecular modifier on Cu surfaces
Publisher: Royal Society of Chemistry (RSC)
Date: 2022
DOI: 10.1039/D2TA07266A
Abstract: A benzenethiol molecule modulates the electronic structure of copper surfaces and thus tunes the coverage of key reaction intermediates, boosting electrochemical CO 2 methanation.
Molecular tuning of CO2-to-ethylene conversion
Publisher: Springer Science and Business Media LLC
Date: 20-11-2019
DOI: 10.1038/S41586-019-1782-2
Abstract: The electrocatalytic reduction of carbon dioxide, powered by renewable electricity, to produce valuable fuels and feedstocks provides a sustainable and carbon-neutral approach to the storage of energy produced by intermittent renewable sources
Size-tunable, highly sensitive microelectrode arrays enabled by polymer pen lithography
Publisher: Royal Society of Chemistry (RSC)
Date: 2017
DOI: 10.1039/C6SM02791A
Abstract: By combining polymer pen lithography (PPL) patterning with in situ polymerization, we report a straightforward and bottom-up approach for bench-top fabrication of microelectrode arrays (MEAs) with well-controlled dimensions. The as-fabricated MEAs can be used to electrodeposit prussian blue in situ and work as a biosensor for H
Chloride-mediated selective electrosynthesis of ethylene and propylene oxides at high current density
Publisher: American Association for the Advancement of Science (AAAS)
Date: 12-06-2020
Abstract: Ethylene oxide is a strained, reactive molecule produced on a vast scale as a plastics precursor. The current method of synthesis involves the direct reaction of ethylene and oxygen at high temperature, but the original protocol relied on the reduction of chlorine to produce a chlorohydrin intermediate. Leow et al. report a room temperature method that returns to the chlorine route but uses electrochemistry to generate it catalytically from chloride (see the Perspective by Barton). This efficient process uses water in place of oxygen and can be integrated with the electrochemical generation of ethylene from carbon dioxide. Propylene oxide can be produced using the same method. Science , this issue p. 1228 see also p. 1181
Tuning OH binding energy enables selective electrochemical oxidation of ethylene to ethylene glycol
Publisher: Springer Science and Business Media LLC
Date: 06-01-2020
Electrochemical Reduction of Carbon Dioxide in a Monoethanolamine Capture Medium
Publisher: Wiley
Date: 19-09-2017
Abstract: The electrocatalytic reduction of CO
Ultra-small Cu nanoparticles embedded in N-doped carbon arrays for electrocatalytic CO2 reduction reaction in dimethylformamide
Publisher: Springer Science and Business Media LLC
Date: 07-2018
Towards a better Sn: Efficient electrocatalytic reduction of CO 2 to formate by Sn/SnS 2 derived from SnS 2 nanosheets
Publisher: Elsevier BV
Date: 2017
Electrochemical Reduction of CO2 at Metal Electrodes in a Distillable Ionic Liquid
Publisher: Wiley
Date: 10-05-2016
Abstract: The electroreduction of CO2 in the distillable ionic liquid dimethylammonium dimethylcarbamate (dimcarb) has been investigated with 17 metal electrodes. Analysis of the electrolysis products reveals that aluminum, bismuth, lead, copper, nickel, palladium, platinum, iron, molybdenum, titanium and zirconium electroreduce the available protons in dimcarb to hydrogen rather than reducing CO2 . Conversely, indium, tin, zinc, silver and gold are able to catalyze the reduction of CO2 to predominantly carbon monoxide (CO) and to a lesser extent, formate ([HCOO](-) ). In all cases, the applied potential was found to have a minimal influence on the distribution of the reduction products. Overall, indium was found to be the best electrocatalyst for CO2 reduction in dimcarb, with faradaic efficiencies of approximately 45 % and 40 % for the generation of CO and [HCOO](-) , respectively, at a potential of -1.34 V versus Cc(+/0) (Cc(+) =cobaltocenium) employing a dimethylamine to CO2 ratio of less than 1.8:1.
Stretchable Supercapacitor with Adjustable Volumetric Capacitance Based on 3D Interdigital Electrodes
Publisher: Wiley
Date: 15-06-2015
Facile Patterning of Reduced Graphene Oxide Film into Microelectrode Array for Highly Sensitive Sensing
Publisher: American Chemical Society (ACS)
Date: 27-07-2011
DOI: 10.1021/AC200939G
Abstract: In this study, we develop a new technique to fabricate a reduced graphene oxide (rGO)-based microelectrode array (MEA) with low-cost soft lithography. To prepare patterned rGO, a polydimethylsiloxane (PDMS) mold with an array of microwells on its surface is fabricated using soft lithography, and GO is assembled on an indium tin oxide (ITO) electrode with a layer-by-layer method. The rGO pattern is formed by closely contacting the assembled GO film onto the ITO electrode with the PDMS mold filled with hydrazine solution in the microwells to selectively reduce the localized GO into the rGO. The MEA with patterned rGO as the microelectrode is characterized with Kelvin probe force microscopy (KFM), atomic force microscopy (AFM), and cyclic voltammetry (CV) with ferricyanide in aqueous solution as the redox probe. The KFM and AFM results demonstrate that each rGO pattern prepared under the present conditions is 3 μm in diameter, which is close to that of the PDMS mold we use. The CV results show that the rGO patterned onto the ITO exhibits a sigmoid-shaped voltammogram up to 200 mVs(-1) with a micro ere level current response, suggesting that the rGO-based electrode fabricated with soft lithography behalves like a MEA. To demonstrate the potential electroanalytical application of the rGO-based MEA, prussian blue (PB) is electrodeposited onto the rGO-based MEA to form the PB/rGO-based MEA. Electrochemical studies on the formed PB/rGO-based MEA reveal that MEA shows a lower detection limit and a larger current density for the detection of H(2)O(2), as compared with the macroscopic rGO electrode. The method demonstrated here provides a simple and low-cost strategy for the fabrication of graphene-based MEA that are useful for electroanalytical applications.
Publisher Correction: Copper adparticle enabled selective electrosynthesis of n-propanol
Publisher: Springer Science and Business Media LLC
Date: 20-02-2020
DOI: 10.1038/S41467-020-14883-Z
Abstract: An amendment to this paper has been published and can be accessed via a link at the top of the paper.
Facile electrochemical co-deposition of metal (Cu, Pd, Pt, Rh) nanoparticles on reduced graphene oxide for electrocatalytic reduction of nitrate/nitrite
Publisher: Elsevier BV
Date: 04-2018
CO 2 electrolysis to multicarbon products at activities greater than 1 A cm −2
Publisher: American Association for the Advancement of Science (AAAS)
Date: 07-02-2020
Abstract: One challenge for efficient electrochemical reduction of carbon dioxide (CO 2 ) is that the gas is hydrophobic, but many of its desirable reactions require water (H 2 O). García de Arquer et al. addressed this problem by combining a copper electrocatalyst with an ionomer assembly that intersperses sulfonate-lined paths for the H 2 O with fluorocarbon channels for the CO 2 . The electrode architecture enables production of two-carbon products such as ethylene and ethanol at current densities just over an ere per square centimeter. Science , this issue p. 661
Advanced Composite 2D Energy Materials by Simultaneous Anodic and Cathodic Exfoliation
Publisher: Wiley
Date: 22-01-2018
Abstract: Composite materials based on graphene and other 2D materials are of considerable interest in the fields of catalysis, electronics, and energy conversion and storage because of the unique structural features and electronic properties of each component and the synergetic effects brought about by the compositing. Approaches to the mass production of 2D materials and their composites in a facile and affordable way are urgently needed to enable their implementation in practical applications. Here a novel electrochemical exfoliation approach to prepare 2D composites is proposed, which combines simultaneous anodic exfoliation of graphite and cathodic exfoliation of other 2D materials (namely MoS 2 , MnO 2 , and graphitic carbon nitride). The synthesis is carried out in a single‐compartment electrochemical cell to in situ produce functional 2D composite materials. Applications of the as‐prepared 2D composites are demonstrated as (i) effective hydrogen evolution catalysts and (ii) supercapacitor electrode materials. The method enables the compositing of semiconductive, or even insulating, 2D materials with conductive graphene in an easy, cheap, ecofriendly, yet efficient way, liberating the intrinsic functions of 2D materials, which are usually hindered by their poor conductivity. The method is believed to be widely applicable to the family of 2D materials.
Promoting CO2 methanation via ligand-stabilized metal oxide clusters as hydrogen-donating motifs
Publisher: Springer Science and Business Media LLC
Date: 03-12-2020
DOI: 10.1038/S41467-020-20004-7
Abstract: Electroreduction uses renewable energy to upgrade carbon dioxide to value-added chemicals and fuels. Renewable methane synthesized using such a route stands to be readily deployed using existing infrastructure for the distribution and utilization of natural gas. Here we design a suite of ligand-stabilized metal oxide clusters and find that these modulate carbon dioxide reduction pathways on a copper catalyst, enabling thereby a record activity for methane electroproduction. Density functional theory calculations show adsorbed hydrogen donation from clusters to copper active sites for the *CO hydrogenation pathway towards *CHO. We promote this effect via control over cluster size and composition and demonstrate the effect on metal oxides including cobalt(II), molybdenum(VI), tungsten(VI), nickel(II) and palladium(II) oxides. We report a carbon dioxide-to-methane faradaic efficiency of 60% at a partial current density to methane of 135 milli ere per square centimetre. We showcase operation over 18 h that retains a faradaic efficiency exceeding 55%.
Binding Site Diversity Promotes CO2 Electroreduction to Ethanol
Publisher: American Chemical Society (ACS)
Date: 08-05-2019
DOI: 10.1021/JACS.9B02945
Abstract: The electrochemical reduction of CO
Intermediate Binding Control Using Metal–Organic Frameworks Enhances Electrochemical CO2 Reduction
Publisher: American Chemical Society (ACS)
Date: 15-12-2020
DOI: 10.1021/JACS.0C10774
Dopant-tuned stabilization of intermediates promotes electrosynthesis of valuable C3 products
Publisher: Springer Science and Business Media LLC
Date: 22-10-2019
DOI: 10.1038/S41467-019-12788-0
Abstract: The upgrading of CO 2 /CO feedstocks to higher-value chemicals via energy-efficient electrochemical processes enables carbon utilization and renewable energy storage. Substantial progress has been made to improve performance at the cathodic side whereas less progress has been made on improving anodic electro-oxidation reactions to generate value. Here we report the efficient electroproduction of value-added multi-carbon dimethyl carbonate (DMC) from CO and methanol via oxidative carbonylation. We find that, compared to pure palladium controls, boron-doped palladium (Pd-B) tunes the binding strength of intermediates along this reaction pathway and favors DMC formation. We implement this doping strategy and report the selective electrosynthesis of DMC experimentally. We achieve a DMC Faradaic efficiency of 83 ± 5%, fully a 3x increase in performance compared to the corresponding pure Pd electrocatalyst.
Hierarchical Mesoporous SnO2 Nanosheets on Carbon Cloth: A Robust and Flexible Electrocatalyst for CO2 Reduction with High Efficiency and Selectivity
Publisher: Wiley
Date: 07-12-2016
Abstract: Electrochemical reduction of CO
Copper nanocavities confine intermediates for efficient electrosynthesis of C3 alcohol fuels from carbon monoxide
Publisher: Springer Science and Business Media LLC
Date: 29-10-2018
In situ characterisation for nanoscale structure–performance studies in electrocatalysis
Publisher: Royal Society of Chemistry (RSC)
Date: 2023
DOI: 10.1039/D2NH00447J
Abstract: We focus on the new horizons in operando / in situ characterisation techniques in electrocatalysis, providing a critical analysis of how advanced in situ techniques help us to deepen our understanding of reaction mechanisms and material evolution.
Hydroxide promotes carbon dioxide electroreduction to ethanol on copper via tuning of adsorbed hydrogen
Publisher: Springer Science and Business Media LLC
Date: 20-12-2019
DOI: 10.1038/S41467-019-13833-8
Abstract: Producing liquid fuels such as ethanol from CO 2 , H 2 O, and renewable electricity offers a route to store sustainable energy. The search for efficient electrocatalysts for the CO 2 reduction reaction relies on tuning the adsorption strength of carbonaceous intermediates. Here, we report a complementary approach in which we utilize hydroxide and oxide doping of a catalyst surface to tune the adsorbed hydrogen on Cu. Density functional theory studies indicate that this doping accelerates water dissociation and changes the hydrogen adsorption energy on Cu. We synthesize and investigate a suite of metal-hydroxide-interface-doped-Cu catalysts, and find that the most efficient, Ce(OH) x -doped-Cu, exhibits an ethanol Faradaic efficiency of 43% and a partial current density of 128 mA cm −2 . Mechanistic studies, wherein we combine investigation of hydrogen evolution performance with the results of operando Raman spectroscopy, show that adsorbed hydrogen hydrogenates surface *HCCOH, a key intermediate whose fate determines branching to ethanol versus ethylene.
Towards Carbon‐Neutral Methanol Production from Carbon Dioxide Electroreduction
Publisher: Wiley
Date: 29-04-2021
Abstract: Electrochemical conversion of CO 2 into liquid fuels and chemicals powered by renewable energy is a promising method to reduce concentration of CO 2 in the atmosphere. Methanol, a value‐added fuel and raw industrial material, can potentially derive from CO 2 electroreduction. However, this route has been plagued by insufficient selectivity, activity, and efficiency. This review summarizes recent advances of electrochemical CO 2 ‐to‐methanol conversion, highlighting mechanistic studies, materials innovations, and reactor designs that aim for improving selectivity, activity, and efficiency of the reaction. The potential challenges and prospects are discussed to guide future advances of this emerging field.
CO2 Electroreduction to Methane at Production Rates Exceeding 100 mA/cm2
Publisher: American Chemical Society (ACS)
Date: 14-09-2020
Conversion of CO2 to multicarbon products in strong acid by controlling the catalyst microenvironment
Publisher: Springer Science and Business Media LLC
Date: 09-02-2023
Electrochemical maps and movies of the hydrogen evolution reaction on natural crystals of molybdenite (MoS2): basal vs. edge plane activity
Publisher: Royal Society of Chemistry (RSC)
Date: 2017
DOI: 10.1039/C7SC02545A
Abstract: In this work, we report the first spatially-resolved voltammetric measurements of the hydrogen evolution reaction on natural crystals of molybdenite, unequivocally demonstrating enhanced catalytic activity on the edge plane relative to the basal plane.
CO 2 electrolysis to multicarbon products in strong acid
Publisher: American Association for the Advancement of Science (AAAS)
Date: 04-06-2021
Abstract: Electrochemical reduction of carbon dioxide (CO 2 ) is a promising means of converting this greenhouse gas into valuable fuels and chemicals. However, two competing reactions restrict the efficiency of this process. In base, much of the CO 2 is trapped as carbonate before reduction in acid, protons outpace CO 2 at catching electrons from the cathode. Huang et al. report that a high dose of potassium ions can help to solve the latter problem. By concentrating potassium ions at the electrode, high selectivity toward CO 2 reduction at high current in acid is possible, which the authors attribute to electrostatic stabilization of the desired adsorbates. Science , abg6582, this issue p. 1074
Electrochemical reduction of CO2on defect-rich Bi derived from Bi2S3with enhanced formate selectivity
Publisher: Royal Society of Chemistry (RSC)
Date: 2018
DOI: 10.1039/C8TA00023A
Abstract: An urchin-like sulphide-derived bismuth electrocatalyst was synthesised for CO 2 reduction and a maximum of 84.0% faradaic efficiency for formate formation was achieved. The origin of the activity of the sulphide-derived bismuth catalyst was explored and its defect-rich structure was responsible for the high formate selectivity.
Facile fabrication of regular Au microband electrode arrays for voltammetric detection down to submicromolar level by hydrogel etching
Publisher: Elsevier BV
Date: 05-2013
Molecular enhancement of heterogeneous CO2 reduction
Publisher: Springer Science and Business Media LLC
Date: 25-02-2020
Bias-Adaptable CO2-to-CO Conversion via Tuning the Binding of Competing Intermediates
Publisher: American Chemical Society (ACS)
Date: 19-08-2021
High‐Oriented Polypyrrole Nanotubes for Next‐Generation Gas Sensor
Publisher: Wiley
Date: 07-07-2016
Abstract: Highly oriented PPy nanotubes are grown by in situ vapor phase polymerization within a nanoscale template under low temperature. As-fabricated PPy nanotubes are used for gas sensing, where an ultralow detection limit (0.05 ppb) and very fast response are achieved. Such an in situ mass-productive method for synthesizing highly oriented conducting polymers may pave a new step toward next-generation gas sensors.
Gradual-order enhanced stability: a frozen section of electrospun nanofibers for energy storage
Publisher: Royal Society of Chemistry (RSC)
Date: 2015
DOI: 10.1039/C5NR01502B
Abstract: The combination of electrospinning and a frozen section has been used to fabricate homodisperse nanoparticle electrodes with high electrochemical performances.
Porous nitrogen–doped carbon derived from biomass for electrocatalytic reduction of CO2 to CO
Publisher: Elsevier BV
Date: 08-2017
Efficient Enzymatic Oxidation of Glucose Mediated by Ferrocene Covalently Attached to Polyethylenimine Stabilized Gold Nanoparticles
Publisher: Wiley
Date: 15-07-2016
Seeing is believing: In-situ visualising dynamic evolution in CO2 electrolysis
Publisher: Elsevier BV
Date: 02-2022
Copper/alkaline earth metal oxide interfaces for electrochemical CO2-to-alcohol conversion by selective hydrogenation
Publisher: Springer Science and Business Media LLC
Date: 24-11-2022
Unlocking the Electrocatalytic Activity of Antimony for CO2 Reduction by Two‐Dimensional Engineering of the Bulk Material
Publisher: Wiley
Date: 17-10-2017
Abstract: Two-dimensional (2D) materials are known to be useful in catalysis. Engineering 3D bulk materials into the 2D form can enhance the exposure of the active edge sites, which are believed to be the origin of the high catalytic activity. Reported herein is the production of 2D "few-layer" antimony (Sb) nanosheets by cathodic exfoliation. Application of this 2D engineering method turns Sb, an inactive material for CO
Superconductivity above 30 K in alkali-metal-doped hydrocarbon
Publisher: Springer Science and Business Media LLC
Date: 30-04-2012
DOI: 10.1038/SREP00389
Efficient electrically powered CO2-to-ethanol via suppression of deoxygenation
Publisher: Springer Science and Business Media LLC
Date: 11-05-2020
Facile regrowth of Mg-Fe2O3/P-Fe2O3 homojunction photoelectrode for efficient solar water oxidation
Publisher: Royal Society of Chemistry (RSC)
Date: 2018
DOI: 10.1039/C8TA05194A
Abstract: In this article, we applied a facile regrowth strategy to prepare Mg-Fe 2 O 3 /P-Fe 2 O 3 NRs photoanode with homojunction structure, which shown high PEC water oxidation efficiency. Experimental and theoretical results reveal that the origin of the superior PEC performance is dependent on P-doping and Mg-Fe 2 O 3 coating.
Cooperative CO2-to-ethanol conversion via enriched intermediates at molecule–metal catalyst interfaces
Publisher: Springer Science and Business Media LLC
Date: 18-12-2019
Detection of Various Microplastics in Patients Undergoing Cardiac Surgery
Publisher: American Chemical Society (ACS)
Date: 13-07-2023
Copper-on-nitride enhances the stable electrosynthesis of multi-carbon products from CO2
Publisher: Springer Science and Business Media LLC
Date: 20-09-2018
DOI: 10.1038/S41467-018-06311-0
Abstract: Copper-based materials are promising electrocatalysts for CO 2 reduction. Prior studies show that the mixture of copper (I) and copper (0) at the catalyst surface enhances multi-carbon products from CO 2 reduction however, the stable presence of copper (I) remains the subject of debate. Here we report a copper on copper (I) composite that stabilizes copper (I) during CO 2 reduction through the use of copper nitride as an underlying copper (I) species. We synthesize a copper-on-nitride catalyst that exhibits a Faradaic efficiency of 64 ± 2% for C 2+ products. We achieve a 40-fold enhancement in the ratio of C 2+ to the competing CH 4 compared to the case of pure copper. We further show that the copper-on-nitride catalyst performs stable CO 2 reduction over 30 h. Mechanistic studies suggest that the use of copper nitride contributes to reducing the CO dimerization energy barrier—a rate-limiting step in CO 2 reduction to multi-carbon products.
Polyoxometalate-Promoted Electrocatalytic CO2 Reduction at Nanostructured Silver in Dimethylformamide
Publisher: American Chemical Society (ACS)
Date: 27-03-2018
Abstract: Electrochemical reduction of CO
Controllable Synthesis of Few-Layer Bismuth Subcarbonate by Electrochemical Exfoliation for Enhanced CO2 Reduction Performance
Publisher: Wiley
Date: 03-09-2018
Abstract: Two‐dimensional (2D) engineering of materials has been recently explored to enhance the performance of electrocatalysts by reducing their dimensionality and introducing more catalytically active ones. In this work, controllable synthesis of few‐layer bismuth subcarbonate nanosheets has been achieved via an electrochemical exfoliation method. These nanosheets catalyse CO 2 reduction to formate with high faradaic efficiency and high current density at a low overpotential owing to the 2D structure and co‐existence of bismuth subcarbonate and bismuth metal under catalytic turnover conditions. Two underlying fast electron transfer processes revealed by Fourier‐transformed alternating current voltammetry (FTacV) are attributed to CO 2 reduction at bismuth subcarbonate and bismuth metal. FTacV results also suggest that protonation of CO 2 .− is the rate determining step for bismuth catalysed CO 2 reduction.
Assessing the economic potential of large-scale carbonate-formation-free CO2 electrolysis
Publisher: Royal Society of Chemistry (RSC)
Date: 2022
DOI: 10.1039/D2CY00045H
Abstract: A techno-economic assessment unraveling the quantitative correlation between carbonate formation and the cost of CO 2 electroreduction.
Quenching of the Electrochemiluminescence of Tris(2,2′-bipyridine)ruthenium(II)/Tri-n-propylamine by Pristine Carbon Nanotube and Its Application to Quantitative Detection of DNA
Publisher: American Chemical Society (ACS)
Date: 24-01-2013
DOI: 10.1021/AC303025Y
Abstract: In this study, we describe the quenching of electrochemiluminescence (ECL) of tris(2,2'-bipyridine)-ruthenium(II)(Ru(bpy)(3)(2+))/tri-n-propylamine(TPA) at pristine multiwall carbon nanotube (MWNT) modified glassy carbon (GC) electrode. Even though the faradic current of the Ru(bpy)(3)(2+)/TPA system and the oxidation of TPA obtained at pristine MWNT-modified GC electrode is enhanced compared with those at the bare GC electrode, the intensity of ECL produced at MWNT electrode is smaller than that at GC electrode. For testing the possible reason of quenching, a comparison of ECL behavior of Ru(bpy)(3)(2+)/TPA at pristine MWNT and acid-treated, heat-treated, and polyethylene glycol (PEG)-wrapped MWNT-modified GC electrode is studied. The results demonstrate that the oxygen-containing groups at the surface of MWNT and the intrinsic electron properties of MWNT are considered to be the major reason for the suppression of ECL. The comparison also demonstrates that this quenching is related to the distance between MWNT and Ru(bpy)(3)(2+)/TPA. Utilizing this essential quenching mechanism, a new signal-on DNA hybridization assay is proposed on the basis of the MWNT modified electrode, where single-stranded DNA (ssDNA) labeled with Ru(bpy)(3)(2+) derivatives probe (Ru-ssDNA) at the distal end is covalently attached onto the MWNT electrode. ECL signal is quenched where Ru-ssDNA is self-organized on the surface of MWNT electrode however, the quenched ECL signal returns in case of the presence of complementary ssDNA. The developed approach for sequence-specific DNA detection has good selectivity, sensitivity, and signal-to-background ratio. Therefore, the quenching of the ECL of Ru(bpy)(3)(2+)/TPA system by the pristine MWNT can be an excellent platform for nucleic acid studies and molecular sensing.
Electrochemical, spectroscopic and theoretical studies of a simple bifunctional cobalt corrole catalyst for oxygen evolution and hydrogen production
Publisher: Royal Society of Chemistry (RSC)
Date: 2014
DOI: 10.1039/C3CP54361G
Abstract: Six cobalt and manganese corrole complexes were synthesized and examined as single-site catalysts for water splitting. The simple cobalt corrole [Co(tpfc)(py)2] (1, tpfc = 5,10,15-tris(pentafluorophenyl)corrole, py = pyridine) catalyzed both water oxidation and proton reduction efficiently. By coating complex 1 onto indium tin oxide (ITO) electrodes, the turnover frequency for electrocatalytic water oxidation was 0.20 s(−1) at 1.4 V (vs. Ag/AgCl, pH = 7), and it was 1010 s(−1) for proton reduction at −1.0 V (vs. Ag/AgCl, pH = 0.5). The stability of 1 for catalytic oxygen evolution and hydrogen production was evaluated by electrochemical, UV-vis and mass measurements, scanning electron microscope (SEM) and energy dispersive X-ray spectroscopy (EDX), which confirmed that 1 was the real molecular catalyst. Titration and UV-vis experiments showed that the pyridine group on Co dissociated at the beginning of catalysis, which was critical to subsequent activation of water. A proton-coupled electron transfer process was involved based on the pH dependence of the water oxidation reaction catalyzed by 1. As for manganese corroles 2–6, although their oxidizing powers were comparable to that of 1, they were not as stable as 1 and underwent decomposition at the electrode. Density functional theory (DFT) calculations indicated that water oxidation by 1 was feasible through a proposed catalytic cycle. The formation of an O–O bond was suggested to be the rate-determining step, and the calculated activation barrier of 18.1 kcal mol(−1) was in good agreement with that obtained from experiments.
Stannate derived bimetallic nanoparticles for electrocatalytic CO2 reduction
Publisher: Royal Society of Chemistry (RSC)
Date: 2018
DOI: 10.1039/C8TA02429D
Abstract: Stannate derived bimetallic systems can achieve highly efficient electrocatalytic CO 2 reduction to formate.
Stabilizing copper sites in coordination polymers toward efficient electrochemical C-C coupling
Publisher: Springer Science and Business Media LLC
Date: 30-01-2023
DOI: 10.1038/S41467-023-35993-4
Abstract: Electroreduction of carbon dioxide with renewable electricity holds promise for achieving net-zero carbon emissions. Single-site catalysts have been reported to catalyze carbon-carbon (C-C) coupling—the indispensable step for more valuable multi-carbon (C 2+ ) products—but were proven to be transformed in situ to metallic agglomerations under working conditions. Here, we report a stable single-site copper coordination polymer (Cu(OH)BTA) with periodic neighboring coppers and it exhibits 1.5 times increase of C 2 H 4 selectivity compared to its metallic counterpart at 500 mA cm − 2 . In-situ/operando X-ray absorption, Raman, and infrared spectroscopies reveal that the catalyst remains structurally stable and does not undergo a dynamic transformation during reaction. Electrochemical and kinetic isotope effect analyses together with computational calculations show that neighboring Cu in the polymer provides suitably-distanced dual sites that enable the energetically favorable formation of an *OCCHO intermediate post a rate-determining step of CO hydrogenation. Accommodation of this intermediate imposes little changes of conformational energy to the catalyst structure during the C-C coupling. We stably operate full-device CO 2 electrolysis at an industry-relevant current of one ere for 67 h in a membrane electrode assembly. The coordination polymers provide a perspective on designing molecularly stable, single-site catalysts for electrochemical CO 2 conversion.
Electrochemical Reduction of CO2 with an Oxide‐Derived Lead Nano‐Coralline Electrode in Dimcarb
Publisher: Wiley
Date: 04-04-2017
Gas Sensors: High‐Oriented Polypyrrole Nanotubes for Next‐Generation Gas Sensor (Adv. Mater. 37/2016)
Publisher: Wiley
Date: 10-2016
Ultralow-limit gas detection in nano-dumbbell polymer sensor via electrospinning
Publisher: Royal Society of Chemistry (RSC)
Date: 2013
DOI: 10.1039/C3NR34090B
Abstract: Nano-dumbbells via electrospinning: controllable nano-dumbbells are fabricated via electrospinning. The weight block parts and the length of nanowires between them can be adjusted through changing the experimental conditions. This nanostructure enables ultralow-limit gas sensing properties of the resulting polypyrrole-based microsensor.
Silica-copper catalyst interfaces enable carbon-carbon coupling towards ethylene electrosynthesis
Publisher: Springer Science and Business Media LLC
Date: 14-05-2021
DOI: 10.1038/S41467-021-23023-0
Abstract: Membrane electrode assembly (MEA) electrolyzers offer a means to scale up CO 2 -to-ethylene electroconversion using renewable electricity and close the anthropogenic carbon cycle. To date, excessive CO 2 coverage at the catalyst surface with limited active sites in MEA systems interferes with the carbon-carbon coupling reaction, diminishing ethylene production. With the aid of density functional theory calculations and spectroscopic analysis, here we report an oxide modulation strategy in which we introduce silica on Cu to create active Cu-SiO x interface sites, decreasing the formation energies of OCOH* and OCCOH*—key intermediates along the pathway to ethylene formation. We then synthesize the Cu-SiO x catalysts using one-pot coprecipitation and integrate the catalyst in a MEA electrolyzer. By tuning the CO 2 concentration, the Cu-SiO x catalyst based MEA electrolyzer shows high ethylene Faradaic efficiencies of up to 65% at high ethylene current densities of up to 215 mA cm −2 and features sustained operation over 50 h.
Low coordination number copper catalysts for electrochemical CO2 methanation in a membrane electrode assembly
Publisher: Springer Science and Business Media LLC
Date: 18-05-2021
DOI: 10.1038/S41467-021-23065-4
Abstract: The electrochemical conversion of CO 2 to methane provides a means to store intermittent renewable electricity in the form of a carbon-neutral hydrocarbon fuel that benefits from an established global distribution network. The stability and selectivity of reported approaches reside below technoeconomic-related requirements. Membrane electrode assembly-based reactors offer a known path to stability however, highly alkaline conditions on the cathode favour C-C coupling and multi-carbon products. In computational studies herein, we find that copper in a low coordination number favours methane even under highly alkaline conditions. Experimentally, we develop a carbon nanoparticle moderator strategy that confines a copper-complex catalyst when employed in a membrane electrode assembly. In-situ XAS measurements confirm that increased carbon nanoparticle loadings can reduce the metallic copper coordination number. At a copper coordination number of 4.2 we demonstrate a CO 2 -to-methane selectivity of 62%, a methane partial current density of 136 mA cm −2 , and 110 hours of stable operation.
Mitigating carbonate formation in CO2 electrolysis
Publisher: Elsevier BV
Date: 09-2023
Efficient Methane Electrosynthesis Enabled by Tuning Local CO2 Availability
Publisher: American Chemical Society (ACS)
Date: 28-01-2020
DOI: 10.1021/JACS.9B12445
Abstract: The electroreduction of carbon dioxide (CO
A tandem effect of atomically isolated copper–nitrogen sites and copper clusters enhances CO2 electroreduction to ethylene
Publisher: Royal Society of Chemistry (RSC)
Date: 2023
DOI: 10.1039/D2NR06009D
Abstract: A Cu-based tandem catalyst shows high ethylene selectivity from the electrochemical CO 2 reduction reaction. In the catalyst, high-concentration CO is generated at one site and then converted with low energy barrier to ethylene at another site.
Reactor design for electrochemical CO2 conversion toward large-scale applications
Publisher: Elsevier BV
Date: 02-2021
Two‐Dimensional Electrocatalysts for Efficient Reduction of Carbon Dioxide
Publisher: Wiley
Date: 10-10-2020
Abstract: Two-dimensional (2D) materials are attractive catalysts for the electrochemical reduction of carbon dioxide reaction (eCO
High-Rate and Efficient Ethylene Electrosynthesis Using a Catalyst/Promoter/Transport Layer
Publisher: American Chemical Society (ACS)
Date: 14-08-2020
Oxomolybdate anchored on copper for electrocatalytic hydrogen production over the entire pH range
Publisher: Elsevier BV
Date: 07-2019
Electrochemical CO2reduction to ethanol: from mechanistic understanding to catalyst design
Publisher: Royal Society of Chemistry (RSC)
Date: 2021
DOI: 10.1039/D1TA01115D
Abstract: Mechanistic understanding has enabled the design of high-performance electrocatalysts. Reaction pathways and electrocatalyst design strategies for CO 2 -to-ethanol conversion are reviewed, and remaining challenges and future directions are discussed.
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