ORCID Profile
0000-0001-7858-0533
Current Organisation
University of Melbourne
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Chemical engineering | Electrochemistry | Electrochemical energy storage and conversion
Publisher: American Chemical Society (ACS)
Date: 17-06-2022
Publisher: American Chemical Society (ACS)
Date: 12-01-2017
Abstract: Susceptibility to CO
Publisher: Wiley
Date: 07-07-2020
Publisher: Royal Society of Chemistry (RSC)
Date: 2015
DOI: 10.1039/C5TA07178J
Abstract: The crystal geometry factor was constrained for the first time to study the non-geometry factors that may affect the oxygen reduction reaction at the operating temperature of solid oxide fuel cells.
Publisher: Elsevier BV
Date: 10-2019
Publisher: Wiley
Date: 09-04-2023
Abstract: The electrochemical CO 2 reduction reaction (CO 2 RR) is an attractive method to produce renewable fuel and chemical feedstock using clean energy sources. Formate production represents one of the most economical target products from CO 2 RR but is primarily produced using post‐transition metal catalysts that require comparatively high overpotentials. Here a composition of bimetallic Cu–Pd is formulated on 2D Ti 3 C 2 T x (MXene) nanosheets that are lyophilized into a highly porous 3D aerogel, resulting in formate production much more efficient than post‐transition metals. Using a membrane electrode assembly (MEA), formate selectivities % are achieved with a current density of 150 mA cm −2 resulting in the highest ever reported overall energy efficiency of 47% (cell potentials of −2.8 V), over 5 h of operation. A comparable Cu‐Pd aerogel achieves near‐unity CO production without the MXene templating. This simple strategy represents an important step toward the experimental demonstration of 3D‐MXenes‐based electrocatalysts for CO 2 RR application and opens a new platform for the fabrication of macroscale aerogel MXene‐based electrocatalysts.
Publisher: Elsevier BV
Date: 12-2021
Publisher: Research Square Platform LLC
Date: 09-08-2022
DOI: 10.21203/RS.3.RS-1874150/V1
Abstract: Oxygen-ion conducting perovskite oxides are important functional materials for solid oxide fuel cells and oxygen permeable membranes operating at high temperatures ( 500 ºC). Co-doped perovskites have recently shown their potential to boost oxygen-related kinetics, but challenges remain to understand the underlying mechanisms. This work unveils the local cation arrangement as a new key factor controlling oxygen kinetics in perovskite oxides. By single- and co-doping Nb5+ and Ta5+ into SrCoO3-δ, we control dominant factors affecting oxygen kinetics such as lattice geometry, cobalt states, and oxygen vacancies, which are confirmed by neutron and synchrotron X-ray diffraction as well as high-temperature X-ray absorption spectroscopy. Our combined experimental and theoretical study unveils that co-doping likely leads to higher cation dispersion at the B-site compared to single-doping. Consequently, a high-entropy configuration enhances oxygen ion migration in the lattice, translating to improved oxygen reduction activity.
Publisher: MDPI AG
Date: 29-04-2021
DOI: 10.3390/MEMBRANES11050328
Abstract: Nanodiamonds (ND) have recently emerged as excellent candidates for various applications including membrane technology due to their nanoscale size, non-toxic nature, excellent mechanical and thermal properties, high surface areas and tuneable surface structures with functional groups. However, their non-porous structure and strong tendency to aggregate are hindering their potential in gas separation membrane applications. To overcome those issues, this study proposes an efficient approach by decorating the ND surface with polyethyleneimine (PEI) before embedding it into the polymer matrix to fabricate MMMs for CO2/N2 separation. Acting as both interfacial binder and gas carrier agent, the PEI layer enhances the polymer/filler interfacial interaction, minimising the agglomeration of ND in the polymer matrix, which is evidenced by the focus ion beam scanning electron microscopy (FIB-SEM). The incorporation of PEI into the membrane matrix effectively improves the CO2/N2 selectivity compared to the pristine polymer membranes. The improvement in CO2/N2 selectivity is also modelled by calculating the interfacial permeabilities with the Felske model using the gas permeabilities in the MMM. This study proposes a simple and effective modification method to address both the interface and gas selectivity in the application of nanoscale and non-porous fillers in gas separation membranes.
Publisher: Wiley
Date: 17-06-2021
Abstract: Single‐phase perovskite oxides that contain nonprecious metals have long been pursued as candidates for catalyzing the oxygen evolution reaction, but their catalytic activity cannot meet the requirements for practical electrochemical energy conversion technologies. Here a cation deficiency‐promoted phase separation strategy to design perovskite‐based composites with significantly enhanced water oxidation kinetics compared to single‐phase counterparts is reported. These composites, self‐assembled from perovskite precursors, comprise strongly interacting perovskite and related phases, whose structure, composition, and concentration can be accurately controlled by tailoring the stoichiometry of the precursors. The composite catalyst with optimized phase composition and concentration outperforms known perovskite oxide systems and state‐of‐the‐art catalysts by 1–3 orders of magnitude. It is further demonstrated that the strong interfacial interaction of the composite catalysts plays a key role in promoting oxygen ionic transport to boost the lattice‐oxygen participated water oxidation. These results suggest a simple and viable approach to developing high‐performance, perovskite‐based composite catalysts for electrochemical energy conversion.
Publisher: Springer Science and Business Media LLC
Date: 14-09-2022
DOI: 10.1038/S41467-022-33145-8
Abstract: Integrating carbon dioxide (CO 2 ) electrolysis with CO 2 capture provides exciting new opportunities for energy reductions by simultaneously removing the energy-demanding regeneration step in CO 2 capture and avoiding critical issues faced by CO 2 gas-fed electrolysers. However, understanding the potential energy advantages of an integrated process is not straightforward due to the interconnected processes which require knowledge of both capture and electrochemical conversion processes. Here, we identify the upper limits of the integrated process from an energy perspective by comparing the working principles and performance of integrated and sequential approaches. Our high-level energy analyses unveil that an integrated electrolyser must show similar performance to the gas-fed electrolyser to ensure an energy benefit of up to 44% versus the sequential route. However, such energy benefits diminish if future gas-fed electrolysers resolve the CO 2 utilisation issue and if an integrated electrolyser shows lower conversion efficiencies than the gas-fed system.
Publisher: Wiley
Date: 05-2016
DOI: 10.1002/APJ.2009
Publisher: Wiley
Date: 03-02-2023
Abstract: The electrochemical reduction of carbon dioxide (CO 2 ) to value‐added chemicals is a promising strategy to mitigate climate change. Metalloporphyrins have been used as a promising class of stable and tunable catalysts for the electrochemical reduction reaction of CO 2 (CO 2 RR) but have been primarily restricted to single‐carbon reduction products. Here, we utilize functionalized earth‐abundant manganese tetraphenylporphyrin‐based (Mn‐TPP) molecular electrocatalysts that have been immobilized via electrografting onto a glassy carbon electrode (GCE) to convert CO 2 with overall 94 % Faradaic efficiencies, with 62 % being converted to acetate. Tuning of Mn‐TPP with electron‐withdrawing sulfonate groups (Mn‐TPPS) introduced mechanistic changes arising from the electrostatic interaction between the sulfonate groups and water molecules, resulting in better surface coverage, which facilitated higher conversion rates than the non‐functionalized Mn‐TPP. For Mn‐TPP only carbon monoxide and formate were detected as CO 2 reduction products. Density‐functional theory (DFT) calculations confirm that the additional sulfonate groups could alter the C−C coupling pathway from *CO→*COH→*COH‐CO to *CO→*CO‐CO→*COH‐CO, reducing the free energy barrier of C−C coupling in the case of Mn‐TPPS. This opens a new approach to designing metalloporphyrin catalysts for two carbon products in CO 2 RR.
Publisher: Wiley
Date: 18-06-2021
Abstract: Electrochemical recovery of the cobalt in deep eutectic solvent shows its promise in recycling and recovery of valuable elements from the spent lithium‐ion battery due to its high selectivity and minimal environmental impacts. This work unveiled the roles of the substrates, applied potentials, and operating temperatures on the performance of cobalt electrochemical recovery in a deep eutectic choline chloride+urea solvent. The solvent contains cobalt and lithium ions extracted from lithium cobalt oxides – 3an essential lithium‐ion battery cathode material. Our results highlight that the substrate predetermines the cobalt recovery modes via substrate–cobalt interactions, which could be predicted by the cobalt surface segregation energies and crystallographic misfits. We also show that a moderate cathode potential under −1.0 V vs. silver quasi‐reference electrode at 94–104 °C is essential to ensure a selective cobalt recovery at an optimal rate. We also found that the stainless‐steel mesh is an optimal substrate for cobalt recovery due to its relatively high selectivity, fast recovery rate, and easy cobalt collection. Our work provides new insights on metal recovery in deep eutectic solvents and offers a new avenue to control the metal electrodeposition modes via modulation of substrate compositions and crystal structures.
Publisher: American Chemical Society (ACS)
Date: 12-2021
DOI: 10.26434/CHEMRXIV-2021-7CHQX
Abstract: Electrochemical conversion of CO2 to chemicals and fuels can potentially play a role in reducing CO2 emissions from industrial processes and providing non-fossil fuel routes to important chemical feedstocks. Most of the recent research on electrocatalysts for CO2 reduction (CO2R) focuses on achieving maximum selectivity for desired products at the highest possible current density. This approach assumes that maximising current density leads to the lowest cost of CO2R (e.g. $·kg-1 CO2 converted) because it requires the lowest catalyst loadings and electrode area per kg of CO2 treated and thus minimising the electrolyser equipment cost. Using a techno-economic analysis (TEA) model with experimental data from a two-cell vapor fed electrolyser, we show this assumption is not valid for CO2 conversion to CO if the process model accounts for relationships between current density, selectivity, cell voltage, ohmic losses, and product separation costs. Instead, our model predicts the lowest CO production costs at current densities from 500 – 700 A·m-2. At current densities above 1000 A·m-2, growing ohmic losses in the electrolyser lead to increasing power costs that become much larger than any capital savings related to reduced electrode area at the higher current density. Further, we investigate different opportunities that could bring down the CO production cost, however, in all the cases, the lowest CO production cost was found at current densities between 600 – 1400 A·m-2. This work also provides insights that can help identify feasible design spaces for both catalysts and electrolysers to develop CO2 conversion technologies that could soon compete on a cost basis with the natural reforming technologies to produce CO (0.60 $·kg-1 market price).
Publisher: American Chemical Society (ACS)
Date: 14-09-2023
Publisher: Wiley
Date: 25-11-2021
Abstract: The melting behaviour of metal–organic frameworks (MOFs) has aroused significant research interest in the areas of materials science, condensed matter physics and chemical engineering. This work first introduces a novel method to fabricate a bimetallic MOF glass, through melt‐quenching of the cobalt‐based zeolitic imidazolate framework (ZIF) [ZIF‐62(Co)] with an adsorbed ferric coordination complex. The high‐temperature chemically reactive ZIF‐62(Co) liquid facilitates the formation of coordinative bonds between Fe and imidazolate ligands, incorporating Fe nodes into the framework after quenching. The resultant Co–Fe bimetallic MOF glass therefore shows a significantly enhanced oxygen evolution reaction performance. The novel bimetallic MOF glass, when combined with the facile and scalable mechanochemical synthesis technique for both discrete powders and surface coatings on flexible substrates, enables significant opportunities for catalytic device assembly.
Publisher: American Chemical Society (ACS)
Date: 05-01-2021
Publisher: Elsevier BV
Date: 06-2021
Publisher: Royal Society of Chemistry (RSC)
Date: 2021
DOI: 10.1039/D0RE00396D
Abstract: Catalyst dimensionality is essential for the reactivity and selectivity of gas-diffusion electrodes for CO 2 electrochemical reduction to produce formate.
Publisher: American Chemical Society (ACS)
Date: 17-12-2021
DOI: 10.26434/CHEMRXIV-2021-33K4D
Abstract: Integrating carbon dioxide (CO2) electrolysis with CO2 capture provides new exciting opportunities for energy reductions by simultaneously removing the energy-demanding regeneration step in CO2 capture and avoiding critical issues faced by CO2 gas-fed electrolysers. However, understanding the potential energy advantages of an integrated capture and conversion process is not straightforward. There are only early-stage demonstrations of CO2 conversion from capture media very recently, and an evaluation of the broader process is paramount before claiming any energy gains from the integration. Here we identify the upper limits of the integrated capture and conversion from an energy perspective by comparing the working principles and performance of integrated and sequential CO2 conversion approaches. Our high-level energy analyses unveil that an integrated electrolysis unit must operate below 1000 kJ/molCO2 to ensure an energy benefit of up to 44% versus the existing state-of-the-art sequential route. However, such energy benefits diminish if future gas-fed electrolysers resolve the carbonation issue and if an integrated electrolyser has poor conversion efficiencies. We conclude with opportunities and limitations to develop industrially relevant integrated electrolysis, providing performance targets for novel integrated electrolysis processes.
Publisher: Wiley
Date: 19-01-2020
Abstract: Invited for this month's cover is the group of Tom Rufford at the University of Queensland. The image shows how choline chloride and urea in a reline solution interact with the surface of a silver cathode to enhance the selectivity of electrochemical CO
Publisher: Wiley
Date: 19-01-2020
Publisher: Elsevier BV
Date: 06-2020
Publisher: Elsevier BV
Date: 06-2021
Publisher: American Chemical Society (ACS)
Date: 08-2022
Abstract: We report a new strategy to improve the reactivity and durability of a membrane electrode assembly (MEA)-type electrolyzer for CO
Publisher: Elsevier BV
Date: 02-2019
Publisher: Royal Society of Chemistry (RSC)
Date: 2020
DOI: 10.1039/D0CC00664E
Abstract: In situ vitrification of MOF within polymer can rigidify the polymer chains and remove interfacial defects, leading to a significantly enhanced membrane selectivity.
Publisher: American Chemical Society (ACS)
Date: 20-04-2020
Publisher: American Chemical Society (ACS)
Date: 28-11-2022
Publisher: Elsevier BV
Date: 12-2019
Publisher: Wiley
Date: 16-04-2020
Publisher: Springer Science and Business Media LLC
Date: 24-04-2020
DOI: 10.1038/S41467-020-15873-X
Abstract: The development of oxygen evolution reaction (OER) electrocatalysts remains a major challenge that requires significant advances in both mechanistic understanding and material design. Recent studies show that oxygen from the perovskite oxide lattice could participate in the OER via a lattice oxygen-mediated mechanism, providing possibilities for the development of alternative electrocatalysts that could overcome the scaling relations-induced limitations found in conventional catalysts utilizing the adsorbate evolution mechanism. Here we distinguish the extent to which the participation of lattice oxygen can contribute to the OER through the rational design of a model system of silicon-incorporated strontium cobaltite perovskite electrocatalysts with similar surface transition metal properties yet different oxygen diffusion rates. The as-derived silicon-incorporated perovskite exhibits a 12.8-fold increase in oxygen diffusivity, which matches well with the 10-fold improvement of intrinsic OER activity, suggesting that the observed activity increase is dominantly a result of the enhanced lattice oxygen participation.
Publisher: Wiley
Date: 04-05-2020
Publisher: American Chemical Society (ACS)
Date: 03-07-2019
Abstract: Development of low-cost and cobalt-free efficient cathode materials for oxygen reduction reaction (ORR) remains one of the paramount motivations for material researchers at a low temperature (<650 °C). In particular, iron-based perovskite oxides show promise as electrocatalysts for ORR because Fe metal is cheaper and naturally abundant, exhibit matched thermal expansion with contacting components such as electrolytes, and show high tolerance in a CO
Publisher: Elsevier BV
Date: 10-2011
Publisher: Elsevier BV
Date: 10-2019
DOI: 10.1016/J.JCIS.2019.06.054
Abstract: Pursuing efficient and low-cost catalysts for the sluggish oxygen evolution reaction (OER) is imperative for the large-scale deployment of promising electrochemical technologies such as water splitting and CO
Publisher: American Chemical Society (ACS)
Date: 27-04-2020
Publisher: Inter-Research Science Center
Date: 08-03-2012
DOI: 10.3354/MEPS09541
Publisher: Elsevier BV
Date: 06-2021
Publisher: Wiley
Date: 11-06-2015
Abstract: Amorphous nickel carbonate particles are catalysts for the oxygen evolution reaction (OER), which plays a critical role in the electrochemical splitting of water. The amorphous nickel carbonate particles can be prepared at a temperature as low as 60 °C by an evaporation-induced precipitation (EIP) method. The products feature hierarchical pore structures. The mass-normalized activity of the catalysts, measured at an overpotential of 0.35 V, was 55.1 A g(-1) , with a Tafel slope of only 60 mV dec(-1) . This catalytic activity is superior to the performance of crystalline NiOx particles and β-Ni(OH)2 particles, and compares favorably to state-of-the-art RuO2 catalysts. The activity of the amorphous nickel carbonate is remarkably stable during a 10 000 s chrono erometry test. Further optimization of synthesis parameters reveals that the amorphous structure can be tuned by adjusting the H2 O/Ni ratio in the precursor mixture. These results suggest the potential application of easily prepared hierarchical basic nickel carbonate particles as cheap and robust OER catalysts with high activity.
Publisher: Elsevier BV
Date: 02-2022
Publisher: Wiley
Date: 07-07-2020
Publisher: Wiley
Date: 17-06-2015
Publisher: Royal Society of Chemistry (RSC)
Date: 2021
DOI: 10.1039/D1TA03636J
Abstract: This review provides an in-depth analysis of essential role of electrode wettability in improving CO 2 electrochemical reduction.
Publisher: Royal Society of Chemistry (RSC)
Date: 2013
DOI: 10.1039/C3TA12781H
Publisher: American Chemical Society (ACS)
Date: 30-08-2022
DOI: 10.26434/CHEMRXIV-2021-33K4D-V2
Abstract: Integrating carbon dioxide (CO2) electrolysis with CO2 capture provides exciting new opportunities for energy reductions by simultaneously removing the energy-demanding regeneration step in CO2 capture and avoiding critical issues faced by CO2 gas-fed electrolysers. However, understanding the potential energy advantages of an integrated process is not straightforward due to the interconnected processes which require knowledge of both capture and electrochemical conversion processes. Here, we identify the upper limits of the integrated process from an energy perspective by comparing the working principles and performance of integrated and sequential approaches. Our high-level energy analyses unveil that an integrated electrolyser must show similar performance to the gas-fed electrolyser to ensure an energy benefit of up to 44% versus the sequential route. However, such energy benefits diminish if future gas-fed electrolysers resolve the CO2 utilisation issue and if an integrated electrolyser shows lower conversion efficiencies than the gas-fed system.
Publisher: Wiley
Date: 20-05-2021
Abstract: Interactions of electrolyte ions at electrocatalyst surfaces influence the selectivity of electrochemical CO 2 reduction (CO 2 R) to chemical feedstocks like CO. We investigated the effects of anion type in aqueous choline halide solutions (ChCl, ChBr, and ChI) on the selectivity of CO 2 R to CO over an Ag foil cathode. Using an H‐type cell, we observed that halide‐specific adsorption at the Ag surface limits CO faradaic efficiency (FE CO ) at potentials more positive than −1.0 V vs. reversible hydrogen electrode (RHE). At these conditions, FE CO increased from I − Br − Cl − , that is, in the opposite order to the strength of specific adsorption of the halide ions (Cl − Br − I − ). At potentials of −1.0 to −1.3 V vs. RHE, restructuring of the Ag surface in ChI and ChCl via dissolution and re‐electrodeposition led to more CO‐selective Ag facets ([220], [311], and [222]) than in ChBr. This mechanism allowed very high faradaic efficiencies for CO of 97±2 % in ChI and 94±2 % in ChCl to be achieved simultaneously with high current densities at −1.3 V vs. RHE. We also demonstrate that high selectivity to CO (FE CO %) in ChCl (at −0.75±0.06 Vvs. RHE) and ChI (at −0.78±0.17 V vs. RHE) could be achieved at a current density of 150 mA cm −2 in a continuous flow‐cell electrolyser with Ag nanoparticles on a commercial gas diffusion electrode. This study provides new insights to understand the interactions of anions with catalysts and offers a new method to modify electrocatalyst surfaces.
Publisher: Royal Society of Chemistry (RSC)
Date: 2022
DOI: 10.1039/D2NR03310K
Abstract: This review paper provides an overview of the fundamental and applied aspects of advancing carbon dioxide electrolysis for the integrated amine-based CO 2 capture and conversion.
Publisher: Springer Science and Business Media LLC
Date: 03-01-2017
DOI: 10.1038/NCOMMS13990
Abstract: The slow activity of cathode materials is one of the most significant barriers to realizing the operation of solid oxide fuel cells below 500 °C. Here we report a niobium and tantalum co-substituted perovskite SrCo 0.8 Nb 0.1 Ta 0.1 O 3−δ as a cathode, which exhibits high electroactivity. This cathode has an area-specific polarization resistance as low as ∼0.16 and ∼0.68 Ω cm 2 in a symmetrical cell and peak power densities of 1.2 and 0.7 W cm −2 in a Gd 0.1 Ce 0.9 O 1.95 -based anode-supported fuel cell at 500 and 450 °C, respectively. The high performance is attributed to an optimal balance of oxygen vacancies, ionic mobility and surface electron transfer as promoted by the synergistic effects of the niobium and tantalum. This work also points to an effective strategy in the design of cathodes for low-temperature solid oxide fuel cells.
Publisher: Wiley
Date: 28-11-2018
Abstract: Rational design and synthesis of hetero-coordinated moieties at the atomic scale can significantly raise the performance of the catalyst and obtain mechanistic insight into the oxygen-involving electrocatalysis. Here, a facile plasma-photochemical strategy is applied to construct atomically coordinated Pt-Co-Se moieties in defective CoSe
Publisher: Wiley
Date: 06-11-2020
Abstract: Achieving high product selectivities is one challenge that limits viability of electrochemical CO
Publisher: Elsevier BV
Date: 08-2018
Publisher: Elsevier BV
Date: 05-2017
Publisher: American Chemical Society (ACS)
Date: 18-06-2021
DOI: 10.1021/JACS.1C03441
Publisher: The Electrochemical Society
Date: 05-2020
DOI: 10.1149/MA2020-01361518MTGABS
Abstract: Electrochemical CO 2 reduction (CO 2 R) could potentially be used with electricity from renewable sources to convert CO 2 into various products such as CO, formic acid (HCOOH), methane (CH 4 ), ethylene (C 2 H 6 ), etc. The overall efficiency of the CO 2 R process is largely linked to the catalyst on which CO 2 is being reduced. However, the local environment surrounding the catalyst is generally subjected to reaction-driven changes during CO 2 R which play a significant role in affecting the overall efficiency, product selectivity, and reaction rate. Therefore, the understanding of catalyst-electrolyte interactions during CO 2 R could be effective in further improving the performance of the catalyst. For ex le, the potential buffering effects of different alkali cations at the catalyst surface due to variations in cation hydrolysis can influence the local proton concentration and thus CO 2 R. 1 The surface tethering of catalyst surface with functional additives such as glycine 2 , poly(acrylamine) 3 , thiol group 4 , etc. have been shown to improve product selectivity by affecting the binding strength with CO 2 R intermediates. In our recent work 5 , we uncovered that the interactions between a polycrystalline Ag foil and reline solution including (i) in-situ nano-structuring of Ag foil by electrodeposition of dissolute native Ag oxide layer, (ii) HER suppression by specifically adsorbed choline ions which restrict the protons availability at the interface, and (iii) stabilization of CO 2 R intermediates by hydrogen bonding with amino group of urea led to a remarkable CO selectivity of (96±8)% at - 0.884 V vs. RHE. Anions of the electrolyte especially halide ions (Cl - , Br - , and I - ) have been reported to affect both the selectivity and activity of CO 2 R. 6, 7 Specifically adsorbed halide ions can modulate the coverage of adsorbed CO on the catalyst surface by stabilizing the intermediates. 8 Moreover, halide ions can induce morphological changes of the catalyst surface during CO 2 R which have demonstrated to enhance the selectivity of CO over Ag catalysts. 9 Inspired by the effect of halide ions, we are investigating the role of different halide ions such as Cl - , Br - and I - in choline based electrolytes over Ag foil for CO 2 R. Our initial experiments have shown that at less negative potentials (between – 1.0 to – 0.7 V vs RHE), I - exhibited the lowest selectivity for CO, and we attribute this result to I - having the highest specific adsorption at the Ag surface and adsorbed I - may restrict the active sites for CO 2 R. However, at larger negative potentials the electrostatic repulsion between the Ag surface and specifically halide ions increases causing the interactions of the catalyst-halide ions to be weakened and thus improving the CO selectivity. SEM characterization of the Ag foil after CO 2 R has confirmed the change in morphology of the Ag surface (more-rougher). Moreover, we performed several flow-cell CO 2 R experiments over Ag-based gas diffusion electrodes (GDEs) and could achieve a CO selectivity over 90% at 150 mA·cm -2 in all three electrolytes. Therefore, altering the interactions between the Ag catalyst and choline-based halide ions during CO 2 R could be a potential approach to enhance the catalytic activity of Ag-metal or Ag nanoparticles. References 1. M. R. Singh, Y. Kwon, Y. Lum, J. W. Ager and A. T. Bell, J. Am. Chem. Soc. , 2016, 138 , 13006-13012. 2. M. S. Xie, B. Y. Xia, Y. Li, Y. Yan, Y. Yang, Q. Sun, S. H. Chan, A. Fisher and X. Wang, Energy Environ. Sci. , 2016, 9 , 1687-1695. 3. S. Ahn, K. Klyukin, R. J. Wakeham, J. A. Rudd, A. R. Lewis, S. Alexander, F. Carla, V. Alexandrov and E. Andreoli, ACS Catalysis , 2018, 8 , 4132-4142. 4. C. Kim, H. S. Jeon, T. Eom, M. S. Jee, H. Kim, C. M. Friend, B. K. Min and Y. J. Hwang, Journal of the American Chemical Society , 2015, 137 , 13844-13850. 5. S. Garg, M. Li, T. E. Rufford, L. Ge, V. Rudolph, R. Knibbe, M. Konarova and G. G. X. Wang, ChemSusChem , 2019, n/a . 6. K. Ogura, J. R. Ferrell, A. V. Cugini, E. S. Smotkin and M. D. Salazar-Villalpando, Electrochim. Acta , 2010, 56 , 381-386. 7. Y. Huang, C. W. Ong and B. S. Yeo, ChemSusChem , 2018, 11 , 3299-3306. 8. A. S. Varela, W. Ju, T. Reier and P. Strasser, ACS Catal. , 2016, 6 , 2136-2144. 9. D. Gao, R. M. Arán-Ais, H. S. Jeon and B. Roldan Cuenya, Nature Catalysis , 2019, 2 , 198-210.
Publisher: American Chemical Society (ACS)
Date: 11-11-2021
Publisher: American Chemical Society (ACS)
Date: 05-08-2022
Publisher: Royal Society of Chemistry (RSC)
Date: 2021
DOI: 10.1039/D0EE03756G
Abstract: Opportunities, challenges and design criteria associated with Gas diffusion electrodes (GDEs) for various electrochemical applications.
Publisher: Wiley
Date: 15-10-2019
Publisher: Wiley
Date: 21-10-2014
Publisher: Elsevier BV
Date: 2019
Publisher: Royal Society of Chemistry (RSC)
Date: 2020
DOI: 10.1039/C9TA13298H
Abstract: This review of design and operating conditions of electrochemical CO 2 reduction covers electrolytes, electrodes, reactors, temperature, pressure, and pH effects.
Publisher: Elsevier BV
Date: 05-2021
Publisher: Elsevier BV
Date: 02-2022
Publisher: American Chemical Society (ACS)
Date: 04-11-2019
Abstract: Metal-organic frameworks (MOFs) have recently emerged as promising electrocatalysts because of their atomically dispersed metal sites and porous structures. The active sites of MOF catalysts largely exist as coordinatively unsaturated metal sites (CUMSs). In this study, facile microwave-induced plasma engraving is applied to fine-tune the CUMSs of cobalt-based MOF (Co-MOF-74) without destroying its phase integrity by controlling the plasma-engraving species, intensity, and duration. The electrochemical activity of the engraved MOF is found to be quantitatively correlated to the coordination geometry of the metal centers corresponding to CUMSs. Specifically, the hydrogen plasma-engraved Co-MOF-74 shows an enhanced catalytic activity of oxygen evolution reaction, which exhibits a low overpotential (337 mV at 15 mA cm
Publisher: Springer Science and Business Media LLC
Date: 09-04-2021
Publisher: Wiley
Date: 08-08-2019
Abstract: Metal-organic framework (MOFs) two-dimensional (2D) nanosheets have many coordinatively unsaturated metal sites that act as active centres for catalysis. To date, limited numbers of 2D MOFs nanosheets can be obtained through top-down or bottom-up synthesis strategies. Herein, we report a 2D oxide sacrifice approach (2dOSA) to facilely synthesize ultrathin MOF-74 and BTC MOF nanosheets with a flexible combination of metal sites, which cannot be obtained through the delamination of their bulk counterparts (top-down) or the conventional solvothermal method (bottom-up). The ultrathin iron-cobalt MOF-74 nanosheets prepared are only 2.6 nm thick. The s le enriched with surface coordinatively unsaturated metal sites, exhibits a significantly higher oxygen evolution reaction reactivity than bulk FeCo MOF-74 particles and the state-of-the-art MOF catalyst. It is believed that this 2dOSA could provide a new and simple way to synthesize various ultrathin MOF nanosheets for wide applications.
Publisher: Inter-Research Science Center
Date: 30-07-2013
DOI: 10.3354/MEPS10364
Publisher: Elsevier BV
Date: 03-2022
Publisher: Wiley
Date: 27-02-2017
Abstract: Electrochemical water splitting is a promising method for storing light/electrical energy in the form of H
Publisher: Research Square Platform LLC
Date: 25-01-2022
DOI: 10.21203/RS.3.RS-1274022/V1
Abstract: The electrochemical reduction of carbon dioxide (CO2) to value-added materials has received considerable attention. Both bulk transition metal catalysts, and molecular catalysts affixed to conductive non-catalytic solid supports, represents a promising approach towards electroreduction of CO2. Here, we report a combined silver (Ag) and pyridine catalyst through a green and irreversible electrografting process, which demonstrates enhanced CO2 conversion versus the in idual counterparts. We find by tailoring the pyridine carbon chain length, a 200 mV shift in the onset potential is obtainable compared to the bare silver electrode. A 10-fold activity enhancement at -0.7 V vs RHE is then observed with demonstratable higher partial current densities for CO indicating a co-catalytic effect is attainable through the integration of the two different catalytic structures. We extended performance to a flow cell operating at 150 mA/cm2, demonstrating the approach’s potential for substantial adaption with various transition metals as supports, and electrografted molecular co-catalysts.
Start Date: 08-2023
End Date: 08-2026
Amount: $428,154.00
Funder: Australian Research Council
View Funded Activity