ORCID Profile
0000-0002-9448-6771
Current Organisation
University of Adelaide
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Nanomaterials | Nanotechnology | Functional materials | Electrochemical energy storage and conversion |
Publisher: Wiley
Date: 17-05-2020
Publisher: Wiley
Date: 22-08-2019
Abstract: Simultaneously achieving high Faradaic efficiency, current density, and stability at low overpotentials is essential for industrial applications of electrochemical CO
Publisher: American Chemical Society (ACS)
Date: 16-06-2021
Publisher: Royal Society of Chemistry (RSC)
Date: 2023
DOI: 10.1039/D2EE03482D
Abstract: By tailoring the microenvironments of a Ni–N–C catalyst in an acidic MEA electrolyzer, we achieve a CO faradaic efficiency of 95% at 500 mA cm −2 , and the CO 2 loss is reduced by 86% at 300 mA cm −2 at pH 0.5, compared to alkaline CO 2 electrolysis.
Publisher: Royal Society of Chemistry (RSC)
Date: 2018
DOI: 10.1039/C8EE00133B
Abstract: Coordinatively unsaturated Ni–N active sites facilitate CO 2 electroreduction and inhibit the competitive hydrogen evolution reaction, demonstrating selective and high-rate CO 2 electroreduction.
Publisher: American Chemical Society (ACS)
Date: 13-03-2023
DOI: 10.1021/JACS.2C13590
Publisher: Wiley
Date: 03-05-2022
Abstract: Electrocatalysts for high‐rate hydrogen evolution reaction (HER) are crucial to clean fuel production. Nitrogen‐rich 2D transition metal nitride, designated “nitridene”, has shown promising HER performance because of its unique physical/chemical properties. However, its synthesis is hindered by the sluggish growth kinetics. Here for the first time using a catalytic molten‐salt method, we facilely synthesized a V−Mo bimetallic nitridene solid solution, V 0.2 Mo 0.8 N 1.2 , with tunable electrocatalytic property. The molten‐salt synthesis reduces the growth barrier of V 0.2 Mo 0.8 N 1.2 and facilitates V dissolution via a monomer assembly, as confirmed by synchrotron spectroscopy and ex situ electron microscopy. Furthermore, by merging computational simulations, we confirm that the V doping leads to an optimized electronic structure for fast protons coupling to produce hydrogen. These findings offer a quantitative engineering strategy for developing analogues of MXenes for clean energy conversions.
Publisher: American Chemical Society (ACS)
Date: 10-08-2022
Publisher: Elsevier BV
Date: 10-2023
Publisher: American Chemical Society (ACS)
Date: 14-01-2019
DOI: 10.1021/ACS.JPCLETT.8B03448
Abstract: A number of experiments have demonstrated that electrochemical reactions are feasible in confined nanoscale reactors, while what the fundamentals of confined electrochemistry are is not clear. Using first-principles calculations and electrochemical modeling, we find that the capacitance in the confined nanoscale reactors can be significantly enhanced, compared to an open electrode interface, essentially promoting the electrochemical reactions and charge transfer efficiency in nanoscale reactors. More importantly, this is a general character, as found in a variety of electrochemical and thermochemical reactions. At the end, we use the recently defined new concept of "confinement energy" for understanding the nature of confined electrochemistry from both thermochemical and electrochemical points of view.
Publisher: Royal Society of Chemistry (RSC)
Date: 2017
DOI: 10.1039/C7SC01615H
Abstract: The confinement effect of h-BN shells helps to maintain active metallic Ni cores and strengthen the HOR processes occurring at h-BN/Ni interfaces.
Publisher: American Chemical Society (ACS)
Date: 23-04-2015
DOI: 10.1021/ACS.NANOLETT.5B01205
Abstract: In heterogeneous catalysis molecule-metal interaction is often modulated through structural modifications at the surface or under the surface of the metal catalyst. Here, we suggest an alternative way toward this modulation by placing a two-dimensional (2D) cover on the metal surface. As an illustration, CO adsorption on Pt(111) surface has been studied under 2D hexagonal boron nitride (h-BN) overlayer. Dynamic imaging data from surface electron microscopy and in situ surface spectroscopic results under near ambient pressure conditions confirm that CO molecules readily intercalate monolayer h-BN sheets on Pt(111) in CO atmosphere but desorb from the h-BN/Pt(111) interface even around room temperature in ultrahigh vacuum. The interaction of CO with Pt has been strongly weakened due to the confinement effect of the h-BN cover, and consequently, CO oxidation at the h-BN/Pt(111) interface was enhanced thanks to the alleviated CO poisoning effect.
Publisher: Springer Science and Business Media LLC
Date: 05-2018
Publisher: American Chemical Society (ACS)
Date: 22-05-2019
Publisher: American Chemical Society (ACS)
Date: 29-11-2022
DOI: 10.1021/ACS.JPCLETT.2C02767
Abstract: Synthesis of large-area uniform bilayer graphene (BLG) with different twisted angles has gathered extensive interest but remains a challenge, hindered by the ubiquitous layer-plus-island growth and the uncontrollable layer rotation. Herein, using real-time surface imaging, film uniformity and stacking structures in BLG were well controlled by a two-step carbon segregation on Ni(111) films following the layer-by-layer growth mode. The aligned first graphene layers formed at 850 °C through a thermodynamics-limit process, followed by decreasing temperatures to grow the second layers, eventually enabling the extremely uniform 15°-twisted BLG at 790 °C and AB-stacked BLG at 720 °C, respectively. Essentially, the growth dynamics is perceived to determine that for the different stacking structures, nonaligned second layers are more kinetically preferable than aligned ones at relatively high temperatures, but the case reverses at low temperatures. This work conveys a fundamental dynamic understanding of the controllable integration of uniform BLG and tuning stacking structures.
Publisher: American Chemical Society (ACS)
Date: 17-09-2020
Publisher: Elsevier BV
Date: 10-2018
Publisher: Elsevier BV
Date: 04-2019
Publisher: American Association for the Advancement of Science (AAAS)
Date: 04-12-2015
Abstract: A coordinatively unsaturated single iron site confined in a graphene matrix shows an ultrahigh activity for catalytic oxidation.
Publisher: Elsevier BV
Date: 07-2017
Publisher: Royal Society of Chemistry (RSC)
Date: 2023
DOI: 10.1039/D3EE01981K
Publisher: Royal Society of Chemistry (RSC)
Date: 2022
DOI: 10.1039/D1EE02013G
Abstract: Direct synthesis of Ni 3 N/Ni catalyst enriched with N-vacancies using one-step reactive magnetron sputtering with enhanced performance for the hydrogen evolution reaction in photoelectrochemical cells and electrolysers.
Publisher: American Chemical Society (ACS)
Date: 14-09-2020
DOI: 10.1021/JACS.0C08139
Publisher: American Chemical Society (ACS)
Date: 07-04-2021
Publisher: Wiley
Date: 07-10-2010
Abstract: The size- and shape-controlled synthesis of Sb(2)S(3) nanostructures has been successfully realized by a facile hydrothermal route. A range of dimensional nanostructures, such as one-dimensional nanorods, two-dimensional nanowire bundles, three dimensional sheaf-like superstructures, dumbbell-shaped superstructures, and urchin-like microspheres, could be obtained through introducing different organic complex reagents or ionic liquids to the reaction system. The formation mechanisms of various Sb(2)S(3) nanostructures have been rationally proposed based on the crystal structure and the nature of the complex reagents and the ionic liquid. The effects of experimental parameters on the final product are also discussed in detail. In addition, electrochemical measurements demonstrate that the as-synthesized Sb(2)S(3) nanostructures have higher initial Li intercalation capacity and excellent cyclic performances, which indicates that the as-synthesized Sb(2)S(3) nanostructures could have potential applications in commercial batteries.
Publisher: Elsevier BV
Date: 08-2017
Publisher: American Chemical Society (ACS)
Date: 09-10-2017
Publisher: Royal Society of Chemistry (RSC)
Date: 2011
DOI: 10.1039/C0DT01212B
Abstract: CdSe nanospheres and dendrites have been successfully synthesized via an ionic liquid-assisted hydrothermal synthetic method. The s les are characterized by X-ray diffraction (XRD), energy-dispersive X-ray spectroscopy (EDS), transmission electron microscopy (TEM) and high-resolution transmission electron microscopy (HRTEM). Our experimental results demonstrate that the CdSe dendrites are obtained by self-assembly from nanospheres under the driving force of oriented attachment process. Moreover, we found that the sizes and morphologies of the crystals depended on the concentration of the ionic liquid, and we obtained the CdSe nanospheres with low concentration of [BMIm][SeO(2)(OCH(3))] and CdSe dendrites with high concentration of [BMIm][SeO(2)(OCH(3))]. The effects of [BMIm][SeO(2)(OCH(3))] on the formation of the CdSe have been investigated systematically. This method is expected to be a useful technique to prepare other metal selenides for controlling the erse shapes and sizes.
Publisher: Springer Science and Business Media LLC
Date: 18-05-2023
DOI: 10.1038/S41467-023-38497-3
Abstract: Acidic CO 2 -to-HCOOH electrolysis represents a sustainable route for value-added CO 2 transformations. However, competing hydrogen evolution reaction (HER) in acid remains a great challenge for selective CO 2 -to-HCOOH production, especially in industrial-level current densities. Main group metal sulfides derived S-doped metals have demonstrated enhanced CO 2 -to-HCOOH selectivity in alkaline and neutral media by suppressing HER and tuning CO 2 reduction intermediates. Yet stabilizing these derived sulfur dopants on metal surfaces at large reductive potentials for industrial-level HCOOH production is still challenging in acidic medium. Herein, we report a phase-engineered tin sulfide pre-catalyst (π-SnS) with uniform rhombic dodecahedron structure that can derive metallic Sn catalyst with stabilized sulfur dopants for selective acidic CO 2 -to-HCOOH electrolysis at industrial-level current densities. In situ characterizations and theoretical calculations reveal the π-SnS has stronger intrinsic Sn-S binding strength than the conventional phase, facilitating the stabilization of residual sulfur species in the Sn subsurface. These dopants effectively modulate the CO 2 RR intermediates coverage in acidic medium by enhancing *OCHO intermediate adsorption and weakening *H binding. As a result, the derived catalyst (Sn(S)-H) demonstrates significantly high Faradaic efficiency (92.15 %) and carbon efficiency (36.43 %) to HCOOH at industrial current densities (up to −1 A cm −2 ) in acidic medium.
Publisher: Research Square Platform LLC
Date: 10-05-2023
DOI: 10.21203/RS.3.RS-2798507/V1
Abstract: Ternary metal (hydro)oxide amorphous catalysts are attractive oxygen evolution reaction (OER) catalysts due to their high performance and cost-effectiveness, but a fundamental understanding of their structure-property relationships remains elusive. Herein, we fabricate a highly active ternary metal (hydro)oxide (NiFeCo) OER catalyst, showing an overpotential of 146 mV at 10 mAcm-2 and ~300 hours durability in 1M KOH. Inspired by this finding, a dataset with first-principles adsorption energies of reaction intermediates at over 300 active-site structures for both oxides and hydroxides is computed and used to train a machine-learning model for screening the dominating factors and unveiling their intrinsic contributions. The computational work confirms that adding Fe and Co makes the original Ni (hydro)oxide reach ultra-low overpotentials below 200 mV through the modulation from hydroxide towards oxide and the formation of active-sites of ternary metallic components. A series of physical properties of the Fe, Co and Ni atoms in the active-sites are further included in the analysis, and it is found that the magnetic moment (mag) plays an important role in the OER activity. This work demonstrates the application of machine-learning methods in atomic-scale active-site engineering to understand the activity mechanism of ternary metal (hydro)oxide amorphous catalysts for water oxidation, and it has the potential to be extended to wider applications.
Publisher: Royal Society of Chemistry (RSC)
Date: 2015
DOI: 10.1039/C5EE00751H
Abstract: Doping single-atom metals into MoS 2 matrix can efficiently trigger the electrocatalytic hydrogen evolution activity of inert S atoms on 2D MoS 2 surface and meanwhile enhance catalytic stability and anti-poison ability.
Publisher: Wiley
Date: 09-01-2023
Abstract: The design of heterogeneous catalysts is necessarily surface‐focused, generally achieved via optimization of adsorption energy and microkinetic modelling. A prerequisite is to ensure the adsorption energy is physically meaningful is the stable existence of the conceived active‐site structure on the surface. The development of improved understanding of the catalyst surface, however, is challenging practically because of the complex nature of dynamic surface formation and evolution under in‐situ reactions. We propose therefore data‐driven machine‐learning (ML) approaches as a solution. In this Minireview we summarize recent progress in using machine‐learning to search and predict (meta)stable structures, assist operando simulation under reaction conditions and micro‐environments, and critically analyze experimental characterization data. We conclude that ML will become the new norm to lower costs associated with discovery and design of optimal heterogeneous catalysts.
Publisher: Proceedings of the National Academy of Sciences
Date: 22-05-2017
Abstract: Small spaces in nanoreactors may have big implications in chemistry, because the chemical nature of molecules and reactions within the nanospaces can be changed significantly due to the nanoconfinement effect. Two-dimensional (2D) nanoreactor formed under 2D materials can provide a well-defined model system to explore the confined catalysis. We demonstrate a general tendency for weakened surface adsorption under the confinement of graphene overlayer, illustrating the feasible modulation of surface reactions by placing a 2D cover on top of the surface. The developed concept “catalysis under cover” can be applied to reactions between two opposite 2D walls interacting with each other through van der Waals force, which helps to design high-performance nanocatalysts interfacing with 2D material overlayers.
Publisher: American Chemical Society (ACS)
Date: 13-04-2023
Publisher: Elsevier BV
Date: 12-2018
Publisher: American Chemical Society (ACS)
Date: 21-06-2023
DOI: 10.1021/JACS.3C03022
Publisher: Wiley
Date: 15-04-2010
Publisher: Elsevier BV
Date: 08-2018
Publisher: Wiley
Date: 02-11-2018
Publisher: American Chemical Society (ACS)
Date: 09-11-2018
Publisher: American Chemical Society (ACS)
Date: 16-11-2017
Publisher: Wiley
Date: 07-07-2023
Abstract: The systematical understanding of metal‐dependent activity in electrocatalyzing oxygen reduction reaction (ORR), a vital reaction with sluggish kinetics for zinc‐air batteries, remains quite unclear. An atomic and spatial engineering modulating ORR activity over hollow carbon quasi‐sphere (HCS) confined in a series of single M‐N (M = Cu, Mn, Ni) sites is reported here. Based on the theoretical prediction and experimental validation, Cu‐N 4 site with the lowest overpotential shows a better ORR kinetics than Mn‐N 4 and Ni‐N 4 . The ORR activity of single‐atom Cu center can be further improved by decreasing the coordination number of N to two, namely Cu‐N 2 , due to the enhancement of electrons with lower coordination structure. Benefitting from the unique spatial confinement effect of the HCS structure in modulating electronic feature of active sites, the Cu‐N 2 site confined in HCS also delivers highly improved ORR kinetics and activity relative to that on planner graphene. Additionally, the best catalyst holds excellent promise in the application of zinc‐air batteries. The findings will pave a new way to atomically and electronically tune active sites with high efficiency for other single‐atom catalysts.
Publisher: Wiley
Date: 03-05-2022
Abstract: Electrocatalysts for high-rate hydrogen evolution reaction (HER) are crucial to clean fuel production. Nitrogen-rich 2D transition metal nitride, designated "nitridene", has shown promising HER performance because of its unique physical/chemical properties. However, its synthesis is hindered by the sluggish growth kinetics. Here for the first time using a catalytic molten-salt method, we facilely synthesized a V-Mo bimetallic nitridene solid solution, V
Publisher: American Chemical Society (ACS)
Date: 06-07-2023
DOI: 10.1021/JACS.3C05171
Publisher: Elsevier BV
Date: 12-2016
Publisher: Wiley
Date: 08-11-2021
Abstract: Reaction temperature is an important parameter to tune the selectivity and activity of electrochemical CO 2 reduction reaction (CO 2 RR) due to different thermodynamics of CO 2 RR and competitive hydrogen evolution reaction (HER). In this work, temperature‐dependent CO 2 RR over Fe‐N‐C and Ni‐N‐C single‐atom catalysts are investigated from 303 to 343 K. Increasing the reaction temperature improves and decreases CO Faradaic efficiency over Fe‐N‐C and Ni‐N‐C catalysts at high overpotentials, respectively. CO current density over Fe‐N‐C catalyst increases with temperature, then gets into a plateau at 323 K, finally reaches the maximum value of 185.8 mA cm −2 at 343 K. While CO current density over Ni‐N‐C catalyst achieves the maximum value of 252.5 mA cm −2 at 323 K, and then drops significantly to 202.9 mA cm −2 at 343 K. Temperature programmed desorption results and density functional theory calculations reveal that the difference of temperature‐dependent variation on CO Faradaic efficiency and current density between Fe‐N‐C and Ni‐N‐C catalysts results from the varied adsorption strength of key reaction intermediates during CO 2 RR.
Publisher: Wiley
Date: 24-11-2012
Publisher: Royal Society of Chemistry (RSC)
Date: 2010
DOI: 10.1039/B921787H
Abstract: gamma-Aluminium oxide (gamma-Al(2)O(3)) mesoporous nanoflakes, showing interesting optical properties, have been successfully synthesized via a one-step ionothermal synthetic method under mild conditions using an ionic liquid [bdmim][Cl] as multifunctional material in terms of solvent and template.
Publisher: Elsevier BV
Date: 09-2019
Start Date: 2024
End Date: 12-2026
Amount: $439,237.00
Funder: Australian Research Council
View Funded ActivityStart Date: 2023
End Date: 12-2025
Amount: $714,888.00
Funder: Australian Research Council
View Funded Activity