Localized geometry determined selectivity of iodide-derived copper for electrochemical CO2 reduction

doi:10.1002/aenm.202203896

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Title:	Localized geometry determined selectivity of iodide-derived copper for electrochemical CO2 reduction
Authors:	Yuchuan Shi, Yiqing Wang, Chung-Li Dong, Ta Thi Thuy Nga, Daixing Wei, Jialin Wang, Xiaoli Zhao, Miao Wang, Kaini Zhang, Mingtao Li, Fan Dong, Shaohua Shen
Date:	2023-01-29
Issue Date:	2024-07-31 12:10:49 (UTC+8)
Publisher:	Wiley-VCH
Abstract:	Two iodide-derived copper (ID-Cu) electrocatalysts (E-ID-Cu and W-ID-Cu) are prepared by electrochemical/wet chemical iodination of Cu foil and subsequent in situ electrochemical reduction reaction. In comparison to electropolished Cu (EP-Cu), both E-ID-Cu and W-ID-Cu can produce multicarbon (C2+) products with much-improved selectivity, with Faradic efficiency (FE) reaching 64.39% for E-ID-Cu and 71.16% for W-ID-Cu at −1.1 V versus reversible hydrogen electrodes (RHE), which can be attributed to their localized geometry features with high defect density and high surface roughness. Given the well-determined FEs towards C2+ products, the partial current densities for C2+ production can be estimated to be 251.8 mA cm−2 for E-ID-Cu and 290.0 mA cm−2 for W-ID-Cu at −1.2 V versus RHE in a flow cell. In situ characterizations and theoretical calculations reveal that the high-density defects and high surface roughness can promote CO adsorption by raising the d band center and then facilitate C–C coupling, contributing to the high selectivity of C2+ products for ID-Cu. Interestingly, the high surface roughness can increase the residence time of C–H intermediates and decrease the formation energy of the OCCO andCH3CH2O intermediates, thus favoring C2+ production, with a unique C2H6 product observed over W-ID-Cu with FE of 10.14% at −0.7 V versus RHE.
Relation:	Advanced Energy Materials 13(11), 2203896
DOI:	10.1002/aenm.202203896
Appears in Collections:	[Graduate Institute & Department of Electrical Engineering] Journal Article

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