Boosting C2+ Alcohols Selectivity and Activity in High-Current CO Electroreduction using Synergistic Cu/Zn Co-Catalysts

Zhitan Wu; Nannan Meng; Rong Yang; Maoxin Chen; Jinhui Pan; Sijia Chi; Chao Wu; Shibo Xi; Yuan Liu; Yingqing Ou; Wenya Wu; Shuhe Han; Bin Zhang; Quan-Hong Yang; Kian Ping Loh

doi:10.1002/anie.202420283

Boosting C₂₊ Alcohols Selectivity and Activity in High-Current CO Electroreduction using Synergistic Cu/Zn Co-Catalysts

Angew Chem Int Ed Engl. 2024 Dec 9:e202420283. doi: 10.1002/anie.202420283. Online ahead of print.

Authors

Zhitan Wu^{1

2

3}, Nannan Meng², Rong Yang⁴, Maoxin Chen^{1

2

3}, Jinhui Pan^{1

2}, Sijia Chi³, Chao Wu⁵, Shibo Xi⁵, Yuan Liu², Yingqing Ou², Wenya Wu⁶, Shuhe Han⁷, Bin Zhang⁴, Quan-Hong Yang^{1

3}, Kian Ping Loh^{1

2}

Affiliations

¹ Joint School of National University of Singapore and Tianjin University, International Campus of Tianjin University, Binhai New City, Fuzhou 350207, China.
² Department of Chemistry, National University of Singapore, 3 Science Drive 3, Singapore, 117543, Singapore.
³ Nanoyang Group, Tianjin Key Laboratory of Advanced Carbon and Electrochemical Energy Storage, State Key Laboratory of Chemical Engineering, School of Chemical Engineering and Technology, Tianjin University, Tianjin, 300072, China.
⁴ Department of Chemistry, School of Science, Tianjin University, Tianjin, 300072, China.
⁵ Institute of Chemical and Engineering Sciences, Agency of Science Technology and Research, 1, Pesek Road, Jurong Island, Singapore, 627833, Singapore.
⁶ Institute of Materials Research and Engineering, Agency of Science Technology and Research, 2, Fusionopolis Way, #08-03, Innovis, 138634, Singapore.
⁷ Department of Applied Physics, The Hong Kong Polytechnic University, Hung Hom, Kowloon, 100872, Hong Kong.

PMID: 39653651
DOI: 10.1002/anie.202420283

Abstract

The electrosynthesis of multi-carbon (C₂₊) alcohols, specifically ethanol and n-propanol through CO electroreduction (CORR) in H₂O, presents a sustainable pathway for intermittent renewable energy storage and a low-carbon economy. However, achieving high selectivity for alcohol production at industrial current densities is kinetically hampered by side reactions such as ethylene generation and hydrogen evolution reaction, which result from competing adsorption of *CO and *H. In this study, we developed a Cu/Zn alloy catalyst to simultaneously enhance the activity and selectivity for alcohol production by increasing CO capture capacity and enriching active hydrogen on Cu sites. Our findings demonstrate that the Cu/5Zn alloy with a molar ratio of Cu to Zn of 95 : 5 exhibits a Faradaic efficiency of 50 % for the selective electrosynthesis of C₂₊ alcohols during ampere-level CO electrolysis. Mechanistic investigations revealed that the Cu/Zn alloy promotes polarized Cu sites, enhancing CO adsorption while facilitating the spillover of hydrogen atoms from Zn to Cu sites, contributing to selective alcohol formation.

Keywords: CO electroreduction; Cu/Zn catalyst; alcohol production; hydrogen spillover; in situ Raman.

Abstract

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