A silver–copper oxide catalyst for acetate electrosynthesis from carbon monoxide

Roham Dorakhan; Ivan Grigioni; Byoung Hoon Lee; Pengfei Ou; Jehad Abed; Colin O’Brien; Armin Sedighian Rasouli; Milivoj Plodinec; Rui Kai Miao; Erfan Shirzadi; Joshua Wicks; Sungjin Park; Geonhui Lee; Jinqiang Zhang; David Sinton; Edward H. Sargent

doi:10.1038/s44160-023-00259-w

A silver–copper oxide catalyst for acetate electrosynthesis from carbon monoxide

Roham Dorakhan, Ivan Grigioni, Byoung Hoon Lee, Pengfei Ou, Jehad Abed, Colin O’Brien, Armin Sedighian Rasouli, Milivoj Plodinec, Rui Kai Miao, Erfan Shirzadi, Joshua Wicks, Sungjin Park, Geonhui Lee, Jinqiang Zhang, David Sinton, Edward H. Sargent^*

^*Corresponding author for this work

Chemistry

Research output: Contribution to journal › Article › peer-review

22 Scopus citations

Abstract

Acetic acid is an important chemical feedstock. The electrocatalytic synthesis of acetic acid from CO₂ offers a low-carbon alternative to traditional synthetic routes, but the direct reduction from CO₂ comes with a CO₂ crossover energy penalty. CO electroreduction bypasses this, which motivates the interest in a cascade synthesis approach of CO₂ to CO followed by CO to acetic acid. Here we report a catalyst design strategy in which off-target intermediates (such as ethylene and ethanol) in the reduction of CO to acetate are destabilized. On the optimized Ag–CuO₂ catalyst, this destabilization of off-target intermediates leads to an acetate Faradaic efficiency of 70% at 200 mA cm⁻². We demonstrate 18 hours of stable operation in a membrane electrode assembly; the system produced 5 wt% acetate at 100 mA cm⁻² and a full-cell energy efficiency of 25%, a twofold improvement on the highest energy-efficient electrosynthesis in prior reports. [Figure not available: see fulltext.]

Original language	English (US)
Pages (from-to)	448-457
Number of pages	10
Journal	Nature Synthesis
Volume	2
Issue number	5
DOIs	https://doi.org/10.1038/s44160-023-00259-w
State	Published - May 2023

Funding

We acknowledge the support of this work by the Ontario Research Foundation—Research Excellence Program (no. ORF-RE08-034, E.H.S.), the Natural Sciences and Engineering Research Council (NSERC) of Canada (no. RGPIN-2017-06477, E.H.S.) and Suncor Canada. I.G. acknowledges the European Union’s Horizon 2020 research and innovation programme under a Marie Sklodowska-Curie grant (agreement no. 846107). DFT calculations were performed on the Niagara supercomputer at the SciNet HPC Consortium. We acknowledge the computational resources supported by SciNet, which is funded by the University of Toronto, the Ontario Research Fund—Research Excellence Program, the Government of Ontario and the Canada Foundation for Innovation. This research used resources of the Advanced Photon Source, an Office of Science User Facility operated for the US Department of Energy (DOE) Office of Science by Argonne National Laboratory and was supported by the US DOE under contract no. DE-AC02-06CH11357, and the Canadian Light Source and its funding partners. This research used resources of the European Synchrotron Radiation Facility at beamline ID26 during the experimental session MA5352 ( https://doi.org/10.15151/ESRF-ES-744180074 ). We thank D. Motta Meira from the 20BM beamline for assistance in collecting the XAS data. We thank R. Wolowiec and D. Kopilovic for their kind technical assistance, S. Boccia from the Ontario Centre for the Characterization of Advanced Materials (OCCAM) of the University of Toronto for the electron microscopy imaging and A. Ip for general input on the paper. We thank Y.-C. Chu and H. M. Chen in the National Taiwan University for conducting in situ XAS experiments. We thank C.-W. Bao in TPS 44A1, National Synchrotron Radiation Research Center, Taiwan, for help with tuning the incident beam of the XAS. We acknowledge support from the Ministry of Science and Technology, Taiwan (contract nos. MOST 110-2628-M-002-001-RSP and 110-2113-M-153-001). We acknowledge the support of this work by the Ontario Research Foundation—Research Excellence Program (no. ORF-RE08-034, E.H.S.), the Natural Sciences and Engineering Research Council (NSERC) of Canada (no. RGPIN-2017-06477, E.H.S.) and Suncor Canada. I.G. acknowledges the European Union’s Horizon 2020 research and innovation programme under a Marie Sklodowska-Curie grant (agreement no. 846107). DFT calculations were performed on the Niagara supercomputer at the SciNet HPC Consortium. We acknowledge the computational resources supported by SciNet, which is funded by the University of Toronto, the Ontario Research Fund—Research Excellence Program, the Government of Ontario and the Canada Foundation for Innovation. This research used resources of the Advanced Photon Source, an Office of Science User Facility operated for the US Department of Energy (DOE) Office of Science by Argonne National Laboratory and was supported by the US DOE under contract no. DE-AC02-06CH11357, and the Canadian Light Source and its funding partners. This research used resources of the European Synchrotron Radiation Facility at beamline ID26 during the experimental session MA5352 (https://doi.org/10.15151/ESRF-ES-744180074). We thank D. Motta Meira from the 20BM beamline for assistance in collecting the XAS data. We thank R. Wolowiec and D. Kopilovic for their kind technical assistance, S. Boccia from the Ontario Centre for the Characterization of Advanced Materials (OCCAM) of the University of Toronto for the electron microscopy imaging and A. Ip for general input on the paper. We thank Y.-C. Chu and H. M. Chen in the National Taiwan University for conducting in situ XAS experiments. We thank C.-W. Bao in TPS 44A1, National Synchrotron Radiation Research Center, Taiwan, for help with tuning the incident beam of the XAS. We acknowledge support from the Ministry of Science and Technology, Taiwan (contract nos. MOST 110-2628-M-002-001-RSP and 110-2113-M-153-001).

ASJC Scopus subject areas

Chemistry (miscellaneous)
Inorganic Chemistry
Organic Chemistry
Materials Chemistry

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Dorakhan, R., Grigioni, I., Lee, B. H., Ou, P., Abed, J., O’Brien, C., Sedighian Rasouli, A., Plodinec, M., Miao, R. K., Shirzadi, E., Wicks, J., Park, S., Lee, G., Zhang, J., Sinton, D., & Sargent, E. H. (2023). A silver–copper oxide catalyst for acetate electrosynthesis from carbon monoxide. Nature Synthesis, 2(5), 448-457. https://doi.org/10.1038/s44160-023-00259-w

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AU - Dorakhan, Roham

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AU - Abed, Jehad

AU - O’Brien, Colin

AU - Sedighian Rasouli, Armin

AU - Plodinec, Milivoj

AU - Miao, Rui Kai

AU - Shirzadi, Erfan

AU - Wicks, Joshua

AU - Park, Sungjin

AU - Lee, Geonhui

AU - Zhang, Jinqiang

AU - Sinton, David

AU - Sargent, Edward H.

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N2 - Acetic acid is an important chemical feedstock. The electrocatalytic synthesis of acetic acid from CO2 offers a low-carbon alternative to traditional synthetic routes, but the direct reduction from CO2 comes with a CO2 crossover energy penalty. CO electroreduction bypasses this, which motivates the interest in a cascade synthesis approach of CO2 to CO followed by CO to acetic acid. Here we report a catalyst design strategy in which off-target intermediates (such as ethylene and ethanol) in the reduction of CO to acetate are destabilized. On the optimized Ag–CuO2 catalyst, this destabilization of off-target intermediates leads to an acetate Faradaic efficiency of 70% at 200 mA cm−2. We demonstrate 18 hours of stable operation in a membrane electrode assembly; the system produced 5 wt% acetate at 100 mA cm−2 and a full-cell energy efficiency of 25%, a twofold improvement on the highest energy-efficient electrosynthesis in prior reports. [Figure not available: see fulltext.]

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A silver–copper oxide catalyst for acetate electrosynthesis from carbon monoxide

Abstract

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ASJC Scopus subject areas

UN SDGs

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