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

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

doi:10.1038/s41929-022-00788-1

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

Yi Xie, Pengfei Ou, Xue Wang, Zhanyou Xu, Yuguang C. Li, Ziyun Wang, Jianan Erick Huang, Joshua Wicks, Christopher McCallum, Ning Wang, Yuhang Wang, Tianxiang Chen, Benedict T. W. Lo, David Sinton, Jimmy C. Yu, Ying Wang^*, Edward H. Sargent^*

^*Corresponding author for this work

Research output: Journal Publications and Reviews › RGC 21 - Publication in refereed journal › peer-review

483 Citations (Scopus)

Abstract

Renewable electricity-powered CO₂ reduction to multi-carbon (C₂₊) products offers a promising route to realization of low-carbon-footprint fuels and chemicals. However, a major fraction of input CO₂ (>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 CO₂ on Cu-based catalysts to weaken H* binding. Using density functional theory studies, we found Pd–Cu promising for selective C₂₊ production over C₁, 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 CO₂ to C₂₊ at 500 mA cm⁻², simultaneous with single-pass CO₂ utilization of 60 ± 2% to C₂₊.

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

Funding

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.

RGC Funding Information

RGC-funded

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

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Cite this

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

abstract = "Renewable electricity-powered CO2 reduction to multi-carbon (C2+) products offers a promising route to realization of low-carbon-footprint fuels and chemicals. However, a major fraction of input CO2 (>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 CO2 on Cu-based catalysts to weaken H* binding. Using density functional theory studies, we found Pd–Cu promising for selective C2+ production over C1, with the lowest ∆GOCCOH* and ∆GOCCOH* - ∆GCHO*. We synthesized Pd–Cu catalysts and report a crossover-free system (liquid product crossover <0.05%) with a Faradaic efficiency of 89 ± 4% for CO2 to C2+ at 500 mA cm−2, simultaneous with single-pass CO2 utilization of 60 ± 2% to C2+.",

author = "Yi Xie and Pengfei Ou and Xue Wang and Zhanyou 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 Lo, {Benedict T. W.} and David Sinton and Yu, {Jimmy C.} and Ying Wang and Sargent, {Edward H.}",

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language = "English",

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

AU - Xie, Yi

AU - Ou, Pengfei

AU - Wang, Xue

AU - Xu, Zhanyou

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 - Lo, Benedict T. W.

AU - Sinton, David

AU - Yu, Jimmy C.

AU - Wang, Ying

AU - Sargent, Edward H.

PY - 2022/6

Y1 - 2022/6

N2 - Renewable electricity-powered CO2 reduction to multi-carbon (C2+) products offers a promising route to realization of low-carbon-footprint fuels and chemicals. However, a major fraction of input CO2 (>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 CO2 on Cu-based catalysts to weaken H* binding. Using density functional theory studies, we found Pd–Cu promising for selective C2+ production over C1, with the lowest ∆GOCCOH* and ∆GOCCOH* - ∆GCHO*. We synthesized Pd–Cu catalysts and report a crossover-free system (liquid product crossover <0.05%) with a Faradaic efficiency of 89 ± 4% for CO2 to C2+ at 500 mA cm−2, simultaneous with single-pass CO2 utilization of 60 ± 2% to C2+.

AB - Renewable electricity-powered CO2 reduction to multi-carbon (C2+) products offers a promising route to realization of low-carbon-footprint fuels and chemicals. However, a major fraction of input CO2 (>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 CO2 on Cu-based catalysts to weaken H* binding. Using density functional theory studies, we found Pd–Cu promising for selective C2+ production over C1, with the lowest ∆GOCCOH* and ∆GOCCOH* - ∆GCHO*. We synthesized Pd–Cu catalysts and report a crossover-free system (liquid product crossover <0.05%) with a Faradaic efficiency of 89 ± 4% for CO2 to C2+ at 500 mA cm−2, simultaneous with single-pass CO2 utilization of 60 ± 2% to C2+.

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