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Vol. 14 (2022)

Hetero-Interfaces on Cu Electrode for Enhanced Electrochemical Conversion of CO2 to Multi-Carbon Products

https://doi.org/10.1007/s40820-022-00879-5
Xiaotong Li
Institute for Composites Science Innovation (InCSI) and State Key Laboratory of Silicon Materials, School of Materials Science and Engineering, Zhejiang University, Hangzhou 310027, People’s Republic of China
Jianghao Wang
Institute for Composites Science Innovation (InCSI) and State Key Laboratory of Silicon Materials, School of Materials Science and Engineering, Zhejiang University, Hangzhou 310027, People’s Republic of China
Xiangzhou Lv
Institute for Composites Science Innovation (InCSI) and State Key Laboratory of Silicon Materials, School of Materials Science and Engineering, Zhejiang University, Hangzhou 310027, People’s Republic of China
Yue Yang
Institute for Composites Science Innovation (InCSI) and State Key Laboratory of Silicon Materials, School of Materials Science and Engineering, Zhejiang University, Hangzhou 310027, People’s Republic of China
Yifei Xu
Institute for Composites Science Innovation (InCSI) and State Key Laboratory of Silicon Materials, School of Materials Science and Engineering, Zhejiang University, Hangzhou 310027, People’s Republic of China
Qian Liu
Institute for Composites Science Innovation (InCSI) and State Key Laboratory of Silicon Materials, School of Materials Science and Engineering, Zhejiang University, Hangzhou 310027, People’s Republic of China
Hao Bin Wu
Institute for Composites Science Innovation (InCSI) and State Key Laboratory of Silicon Materials, School of Materials Science and Engineering, Zhejiang University, Hangzhou 310027, People’s Republic of China

Corresponding Author: Hao Bin Wu

hbwu@zju.edu.cn

Nano-Micro Letters, Vol. 14 (2022), Article Number: 134

Abstract

Electrochemical CO2 reduction reaction (CO2RR) to multi-carbon products would simultaneously reduce CO2 emission and produce high-value chemicals. Herein, we report Cu electrodes modified by metal–organic framework (MOF) exhibiting enhanced electrocatalytic performance to convert CO2 into ethylene and ethanol. The Zr-based MOF, UiO-66 would in situ transform into amorphous ZrOx nanoparticles (a-ZrOx), constructing a-ZrOx/Cu hetero-interface as a dual-site catalyst. The Faradaic efficiency of multi-carbon (C2+) products for optimal UiO-66-coated Cu (0.5-UiO/Cu) electrode reaches a high value of 74% at − 1.05 V versus RHE. The intrinsic activity for C2+ products on 0.5-UiO/Cu electrode is about two times higher than that of Cu foil. In situ surface-enhanced Raman spectra demonstrate that UiO-66-derived a-ZrOx coating can promote the stabilization of atop-bound CO* intermediates on Cu surface during CO2 electrolysis, leading to increased CO* coverage and facilitating the C–C coupling process. The present study gives new insights into tailoring the adsorption configurations of CO2RR intermediate by designing dual-site electrocatalysts with hetero-interfaces.


Highlights:


1 Dual-site electrocatalysts with in situ formed metal-oxide interfaces are proposed and demonstrated to enhance the formation of multi-carbon products from electrochemical CO2 reduction.
2 The 0.5-UiO/Cu delivers a high C2+ Faradaic efficiency of over 74% with notably boosted formation rate and durability, surpassing most reported electrocatalysts.
3 A unique mechanism of UiO-66 to induce in situ reconstruction of Cu surface and formation of UiO-66-derived amorphous ZrOx/Cu interface is uncovered, which improves the selectivity and productivity toward C2+ products.

Keywords

CO2 reduction reaction Metal–organic frameworks Copper Hetero-interfaces Multi-carbon products
Li, Xiaotong, Jianghao Wang, Xiangzhou Lv, Yue Yang, Yifei Xu, Qian Liu, and Hao Bin Wu. 2022. “Hetero-Interfaces on Cu Electrode for Enhanced Electrochemical Conversion of CO2 to Multi-Carbon Products”. Nano-Micro Letters 14 (June):134. https://doi.org/10.1007/s40820-022-00879-5.
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