ORCID Profile
0000-0001-9641-9815
Current Organisation
Queen's University
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Publisher: Springer Science and Business Media LLC
Date: 06-01-2020
Publisher: Springer Science and Business Media LLC
Date: 18-12-2019
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.
Publisher: Springer Science and Business Media LLC
Date: 29-10-2018
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.
Publisher: Springer Science and Business Media LLC
Date: 11-11-2019
Publisher: Springer Science and Business Media LLC
Date: 16-12-2019
Publisher: American Chemical Society (ACS)
Date: 14-09-2020
Publisher: Springer Science and Business Media LLC
Date: 11-02-2019
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.
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
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.
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
Publisher: American Chemical Society (ACS)
Date: 08-05-2019
DOI: 10.1021/JACS.9B02945
Abstract: The electrochemical reduction of CO
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 .
Publisher: American Chemical Society (ACS)
Date: 02-03-2020
DOI: 10.1021/JACS.9B13347
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
Publisher: Springer Science and Business Media LLC
Date: 11-05-2020
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.
No related grants have been discovered for Cao-Thang Dinh.