Boosting electrocatalytic CO2-to-ethanol production via asymmetric C-C coupling

Pengtang Wang; Hao Yang; Cheng Tang; Yu Wu; Yao Zheng; Tao Cheng; Kenneth Davey; Xiaoqing Huang; Shi-Zhang Qiao

doi:10.1038/s41467-022-31427-9

Boosting electrocatalytic CO₂-to-ethanol production via asymmetric C-C coupling

Nat Commun. 2022 Jun 29;13(1):3754. doi: 10.1038/s41467-022-31427-9.

Authors

Pengtang Wang^#^{1

2}, Hao Yang^#³, Cheng Tang¹, Yu Wu³, Yao Zheng¹, Tao Cheng³, Kenneth Davey¹, Xiaoqing Huang⁴, Shi-Zhang Qiao⁵

Affiliations

¹ School of Chemical Engineering and Advanced Materials, The University of Adelaide, Adelaide, SA, 5005, Australia.
² State Key Laboratory of Physical Chemistry of Solid Surfaces, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, 361005, China.
³ Institute of Functional Nano & Soft Materials (FUNSOM), Jiangsu Key Laboratory for Carbon-Based Functional Materials & Devices, Joint International Research Laboratory of Carbon-Based Functional Materials and Devices, Soochow University, Suzhou, 215123, China.
⁴ State Key Laboratory of Physical Chemistry of Solid Surfaces, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, 361005, China. hxq006@xmu.edu.cn.
⁵ School of Chemical Engineering and Advanced Materials, The University of Adelaide, Adelaide, SA, 5005, Australia. s.qiao@adelaide.edu.au.

^# Contributed equally.

Abstract

Electroreduction of carbon dioxide (CO₂) into multicarbon products provides possibility of large-scale chemicals production and is therefore of significant research and commercial interest. However, the production efficiency for ethanol (EtOH), a significant chemical feedstock, is impractically low because of limited selectivity, especially under high current operation. Here we report a new silver-modified copper-oxide catalyst (dCu₂O/Ag_2.3%) that exhibits a significant Faradaic efficiency of 40.8% and energy efficiency of 22.3% for boosted EtOH production. Importantly, it achieves CO₂-to-ethanol conversion under high current operation with partial current density of 326.4 mA cm^-2 at -0.87 V vs reversible hydrogen electrode to rank highly significantly amongst reported Cu-based catalysts. Based on in situ spectra studies we show that significantly boosted production results from tailored introduction of Ag to optimize the coordinated number and oxide state of surface Cu sites, in which the ^*CO adsorption is steered as both atop and bridge configuration to trigger asymmetric C-C coupling for stablization of EtOH intermediates.