Asymmetrical electro-hydrogenation of CO2 to ethanol with Copper-Gold heterojunctions

Siyu Kuang; Ya-Qiong Su; Minglu Li; Hai Liu; Hongyuan Chuai; Emiel J.M. Hensen; Thomas Meyer; Sheng Zhang; Xinbin Ma; Xiaoyi Chen

doi:10.1073/pnas.2214175120

Asymmetrical electro-hydrogenation of CO2 to ethanol with Copper-Gold heterojunctions

Siyu Kuang
, Ya-Qiong Su
, Minglu Li
, Hai Liu
, Hongyuan Chuai
, Emiel J.M. Hensen
, Thomas Meyer
, Sheng Zhang (Corresponding author)
, Xinbin Ma (Corresponding author)
, Xiaoyi Chen (Corresponding author)

Inorganic Materials & Catalysis

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

100 Citations (Scopus)

268 Downloads (Pure)

Abstract

Copper is distinctive in electrocatalyzing reduction of CO2 into various energy-dense forms, but it often suffers from limited product selectivity including ethanol in competi-tion with ethylene. Here, we describe systematically designed, bimetallic electrocatalysts based on copper/gold heterojunctions with a faradaic efficiency toward ethanol of 60% at currents in excess of 500 mA cm−2. In the modified catalyst, the ratio of ethanol to ethylene is enhanced by a factor of 200 compared to copper catalysts. Analysis by ATR-IR measurements under operating conditions, and by computational simulations, suggests that reduction of CO2 at the copper/gold heterojunction is dominated by generation of the intermediate OCCOH*. The latter is a key contributor in the overall, asymmetrical electrohydrogenation of CO2 giving ethanol rather than ethylene

Original language	English
Article number	e2214175120
Number of pages	6
Journal	Proceedings of the National Academy of Sciences of the United States of America
Volume	120
Issue number	4
DOIs	https://doi.org/10.1073/pnas.2214175120
Publication status	Published - 17 Jan 2023

Funding

We are grateful to the financial support from the National Nature Science Foundation of China (Grant nos. 22078232 and 21938008) and the Science and Technology Major Project of Tianjin (Grant nos. 19ZXNCGX00030 and 20JCYBJC00870). Y. S. acknowledges the “Young Talent Support Plan” of Xi'an Jiaotong University. Supercomputing facilities were provided by Hefei Advanced Computing Center.

Funders	Funder number
National Natural Science Foundation of China	21938008, 22078232
Xi’an Jiaotong University

Keywords

copper
ethanol
heterojunction
CO2
hydrogenation
CO

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title = "Asymmetrical electro-hydrogenation of CO2 to ethanol with Copper-Gold heterojunctions",

abstract = "Copper is distinctive in electrocatalyzing reduction of CO2 into various energy-dense forms, but it often suffers from limited product selectivity including ethanol in competi-tion with ethylene. Here, we describe systematically designed, bimetallic electrocatalysts based on copper/gold heterojunctions with a faradaic efficiency toward ethanol of 60\% at currents in excess of 500 mA cm−2. In the modified catalyst, the ratio of ethanol to ethylene is enhanced by a factor of 200 compared to copper catalysts. Analysis by ATR-IR measurements under operating conditions, and by computational simulations, suggests that reduction of CO2 at the copper/gold heterojunction is dominated by generation of the intermediate OCCOH*. The latter is a key contributor in the overall, asymmetrical electrohydrogenation of CO2 giving ethanol rather than ethylene",

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author = "Siyu Kuang and Ya-Qiong Su and Minglu Li and Hai Liu and Hongyuan Chuai and Hensen, \{Emiel J.M.\} and Thomas Meyer and Sheng Zhang and Xinbin Ma and Xiaoyi Chen",

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T1 - Asymmetrical electro-hydrogenation of CO2 to ethanol with Copper-Gold heterojunctions

AU - Kuang, Siyu

AU - Su, Ya-Qiong

AU - Li, Minglu

AU - Liu, Hai

AU - Chuai, Hongyuan

AU - Hensen, Emiel J.M.

AU - Meyer, Thomas

AU - Zhang, Sheng

AU - Ma, Xinbin

AU - Chen, Xiaoyi

PY - 2023/1/17

Y1 - 2023/1/17

N2 - Copper is distinctive in electrocatalyzing reduction of CO2 into various energy-dense forms, but it often suffers from limited product selectivity including ethanol in competi-tion with ethylene. Here, we describe systematically designed, bimetallic electrocatalysts based on copper/gold heterojunctions with a faradaic efficiency toward ethanol of 60% at currents in excess of 500 mA cm−2. In the modified catalyst, the ratio of ethanol to ethylene is enhanced by a factor of 200 compared to copper catalysts. Analysis by ATR-IR measurements under operating conditions, and by computational simulations, suggests that reduction of CO2 at the copper/gold heterojunction is dominated by generation of the intermediate OCCOH*. The latter is a key contributor in the overall, asymmetrical electrohydrogenation of CO2 giving ethanol rather than ethylene

AB - Copper is distinctive in electrocatalyzing reduction of CO2 into various energy-dense forms, but it often suffers from limited product selectivity including ethanol in competi-tion with ethylene. Here, we describe systematically designed, bimetallic electrocatalysts based on copper/gold heterojunctions with a faradaic efficiency toward ethanol of 60% at currents in excess of 500 mA cm−2. In the modified catalyst, the ratio of ethanol to ethylene is enhanced by a factor of 200 compared to copper catalysts. Analysis by ATR-IR measurements under operating conditions, and by computational simulations, suggests that reduction of CO2 at the copper/gold heterojunction is dominated by generation of the intermediate OCCOH*. The latter is a key contributor in the overall, asymmetrical electrohydrogenation of CO2 giving ethanol rather than ethylene

KW - copper

KW - ethanol

KW - heterojunction

KW - CO2

KW - hydrogenation

KW - CO

UR - https://www.scopus.com/pages/publications/85146404300

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ER -

Asymmetrical electro-hydrogenation of CO2 to ethanol with Copper-Gold heterojunctions

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