High carbon utilization in CO2 reduction to multi-carbon products in acidic media

Tsz Woon Benedict Lo; Yi  Xie; Pengfei  Qu; Wang Xue; Zhangyou Xu; Yuguang C. Li; Ziyun Wang; Jianan Erick Huang; Joshua Wicks; Christopher McCallum; Ning Wang; Yuhang Wang; Tianxiang Chen; David Sinton; Jimmy C. Yu; Ying Wang; Edward H.  Sargent

doi:https://doi.org/10.1038/s41929-022-00788-1

High carbon utilization in CO2 reduction to multi-carbon products in acidic media

Tsz Woon Benedict Lo, Yi Xie, Pengfei Qu, Wang Xue, Zhangyou Xu, Yuguang C. Li, Ziyun Wang, Jianan Erick Huang, Joshua Wicks, Christopher McCallum, Ning Wang, Yuhang Wang, Tianxiang Chen, David Sinton, Jimmy C. Yu, Ying Wang, Edward H. Sargent

Research output: Journal article publication › Journal article › Academic research › peer-review

16 Citations (Scopus)

Abstract

Renewable electricity-powered CO ₂ reduction to multi-carbon (C ₂₊) products offers a promising route to realization of low-carbon-footprint fuels and chemicals. However, a major fraction of input CO ₂ (>85%) is consumed by the electrolyte through reactions with hydroxide to form carbonate/bicarbonate in both alkaline and neutral reactors. Acidic conditions offer a solution to overcoming this limitation, but also promote the hydrogen evolution reaction. Here we report a design strategy that suppresses hydrogen evolution reaction activity by maximizing the co-adsorption of CO and CO ₂ on Cu-based catalysts to weaken H* binding. Using density functional theory studies, we found Pd–Cu promising for selective C ₂₊ production over C ₁, with the lowest ∆G _OCCOH* and ∆G _OCCOH* - ∆G _CHO*. We synthesized Pd–Cu catalysts and report a crossover-free system (liquid product crossover <0.05%) with a Faradaic efficiency of 89 ± 4% for CO ₂ to C ₂₊ at 500 mA cm ⁻², simultaneous with single-pass CO ₂ utilization of 60 ± 2% to C ₂₊. [Figure not available: see fulltext.]

Original language	English
Pages (from-to)	564-570
Number of pages	7
Journal	Nature Catalysis
Volume	5
Issue number	6
DOIs	https://doi.org/10.1038/s41929-022-00788-1
Publication status	Published - 9 Jun 2022

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https://doi.org/10.1038/s41929-022-00788-1

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@article{923c104b3bdc4be3850279918f118cf1,

title = "High carbon utilization in CO2 reduction to multi-carbon products in acidic media",

abstract = "Renewable electricity-powered CO 2 reduction to multi-carbon (C 2+) products offers a promising route to realization of low-carbon-footprint fuels and chemicals. However, a major fraction of input CO 2 (>85%) is consumed by the electrolyte through reactions with hydroxide to form carbonate/bicarbonate in both alkaline and neutral reactors. Acidic conditions offer a solution to overcoming this limitation, but also promote the hydrogen evolution reaction. Here we report a design strategy that suppresses hydrogen evolution reaction activity by maximizing the co-adsorption of CO and CO 2 on Cu-based catalysts to weaken H* binding. Using density functional theory studies, we found Pd–Cu promising for selective C 2+ production over C 1, with the lowest ∆G OCCOH* and ∆G OCCOH* - ∆G CHO*. We synthesized Pd–Cu catalysts and report a crossover-free system (liquid product crossover <0.05%) with a Faradaic efficiency of 89 ± 4% for CO 2 to C 2+ at 500 mA cm −2, simultaneous with single-pass CO 2 utilization of 60 ± 2% to C 2+. [Figure not available: see fulltext.]",

author = "Lo, {Tsz Woon Benedict} and Yi Xie and Pengfei Qu and Wang Xue and Zhangyou Xu and Li, {Yuguang C.} and Ziyun Wang and Huang, {Jianan Erick} and Joshua Wicks and Christopher McCallum and Ning Wang and Yuhang Wang and Tianxiang Chen and David Sinton and Yu, {Jimmy C.} and Ying Wang and Sargent, {Edward H.}",

note = "Funding Information: Ying Wang, Y.X. and Z.X. acknowledge the support of the Research Grants Council of the Hong Kong Special Administrative Region (project no. 24304920). E.H.S., P.O., X.W., J.E.H., J.W., N.W. and Yuhang Wang acknowledge the support of the Natural Sciences and Engineering Research Council of Canada and the Ontario Research Fund – Research Excellence programme. Z.W. wishes to acknowledge the Marsden Fund Council from Government funding, managed by Royal Society Te Apārangi and the eScience Infrastructure (NeSI) high performance computing facilities. All DFT calculations were performed with support from the Niagara supercomputer at the SciNet HPC Consortium. SciNet is funded by the Canada Foundation for Innovation, the Government of Ontario, Ontario Research Fund – Research Excellence, and the University of Toronto. Publisher Copyright: {\textcopyright} 2022, The Author(s), under exclusive licence to Springer Nature Limited.",

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month = jun,

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T1 - High carbon utilization in CO2 reduction to multi-carbon products in acidic media

AU - Lo, Tsz Woon Benedict

AU - Xie, Yi

AU - Qu, Pengfei

AU - Xue, Wang

AU - Xu, Zhangyou

AU - Li, Yuguang C.

AU - Wang, Ziyun

AU - Huang, Jianan Erick

AU - Wicks, Joshua

AU - McCallum, Christopher

AU - Wang, Ning

AU - Wang, Yuhang

AU - Chen, Tianxiang

AU - Sinton, David

AU - Yu, Jimmy C.

AU - Wang, Ying

AU - Sargent, Edward H.

N1 - Funding Information: Ying Wang, Y.X. and Z.X. acknowledge the support of the Research Grants Council of the Hong Kong Special Administrative Region (project no. 24304920). E.H.S., P.O., X.W., J.E.H., J.W., N.W. and Yuhang Wang acknowledge the support of the Natural Sciences and Engineering Research Council of Canada and the Ontario Research Fund – Research Excellence programme. Z.W. wishes to acknowledge the Marsden Fund Council from Government funding, managed by Royal Society Te Apārangi and the eScience Infrastructure (NeSI) high performance computing facilities. All DFT calculations were performed with support from the Niagara supercomputer at the SciNet HPC Consortium. SciNet is funded by the Canada Foundation for Innovation, the Government of Ontario, Ontario Research Fund – Research Excellence, and the University of Toronto. Publisher Copyright: © 2022, The Author(s), under exclusive licence to Springer Nature Limited.

PY - 2022/6/9

Y1 - 2022/6/9

N2 - Renewable electricity-powered CO 2 reduction to multi-carbon (C 2+) products offers a promising route to realization of low-carbon-footprint fuels and chemicals. However, a major fraction of input CO 2 (>85%) is consumed by the electrolyte through reactions with hydroxide to form carbonate/bicarbonate in both alkaline and neutral reactors. Acidic conditions offer a solution to overcoming this limitation, but also promote the hydrogen evolution reaction. Here we report a design strategy that suppresses hydrogen evolution reaction activity by maximizing the co-adsorption of CO and CO 2 on Cu-based catalysts to weaken H* binding. Using density functional theory studies, we found Pd–Cu promising for selective C 2+ production over C 1, with the lowest ∆G OCCOH* and ∆G OCCOH* - ∆G CHO*. We synthesized Pd–Cu catalysts and report a crossover-free system (liquid product crossover <0.05%) with a Faradaic efficiency of 89 ± 4% for CO 2 to C 2+ at 500 mA cm −2, simultaneous with single-pass CO 2 utilization of 60 ± 2% to C 2+. [Figure not available: see fulltext.]

AB - Renewable electricity-powered CO 2 reduction to multi-carbon (C 2+) products offers a promising route to realization of low-carbon-footprint fuels and chemicals. However, a major fraction of input CO 2 (>85%) is consumed by the electrolyte through reactions with hydroxide to form carbonate/bicarbonate in both alkaline and neutral reactors. Acidic conditions offer a solution to overcoming this limitation, but also promote the hydrogen evolution reaction. Here we report a design strategy that suppresses hydrogen evolution reaction activity by maximizing the co-adsorption of CO and CO 2 on Cu-based catalysts to weaken H* binding. Using density functional theory studies, we found Pd–Cu promising for selective C 2+ production over C 1, with the lowest ∆G OCCOH* and ∆G OCCOH* - ∆G CHO*. We synthesized Pd–Cu catalysts and report a crossover-free system (liquid product crossover <0.05%) with a Faradaic efficiency of 89 ± 4% for CO 2 to C 2+ at 500 mA cm −2, simultaneous with single-pass CO 2 utilization of 60 ± 2% to C 2+. [Figure not available: see fulltext.]

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U2 - https://doi.org/10.1038/s41929-022-00788-1

DO - https://doi.org/10.1038/s41929-022-00788-1

M3 - Journal article

SN - 2520-1158

VL - 5

SP - 564

EP - 570

JO - Nature Catalysis

JF - Nature Catalysis

IS - 6

ER -

High carbon utilization in CO2 reduction to multi-carbon products in acidic media

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