Switching CO2 Electroreduction Selectivity Between C1 and C2 Hydrocarbons on Cu Gas-Diffusion Electrodes

Zhang, Jianfang; Li, Zhengyuan Y.; Cai, Rui; Zhang, Tianyu; Yang, Shize; Ma, Lu; Wang, Yan; Wu, Yucheng; Wu, Jingjie J.

doi:10.1002/eem2.12307

Switching CO₂ Electroreduction Selectivity Between C₁ and C₂ Hydrocarbons on Cu Gas-Diffusion Electrodes

Journal Article · Tue Nov 02 00:00:00 EDT 2021 · Energy & Environmental Materials

DOI:https://doi.org/10.1002/eem2.12307· OSTI ID:1890212

^[1]; Li, Zhengyuan Y. ^[2]; Cai, Rui ^[3]; Zhang, Tianyu ^[2]; Yang, Shize ^[4]; Ma, Lu ^[5]; Wang, Yan ^[3]; ^[3]; Wu, Jingjie J. ^[2]

Hefei University of Technology (China); University of Cincinnati, OH (United States)
University of Cincinnati, OH (United States)
Hefei University of Technology (China)
Arizona State University, Tempe, AZ (United States)
Brookhaven National Lab. (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)

We report that regulating the selectivity toward a target hydrocarbon product is still the focus of CO₂ electroreduction. Here, we discover that the original surface Cu species in Cu gas-diffusion electrodes plays a more important role than the surface roughness, local pH, and facet in governing the selectivity toward C₁ or C₂ hydrocarbons. The selectivity toward C₂H₄ progressively increases, while CH₄ decreases steadily upon lowering the Cu oxidation species fraction. At a relatively low electrodeposition voltage of 1.5 V, the Cu gas-diffusion electrode with the highest Cu^δ+/Cu⁰ ratio favors the pathways of hydrogenation to form CH₄ with maximum Faradaic efficiency of 65.4% and partial current density of 228 mA cm^-2 at -0.83 V vs RHE. At 2.0 V, the Cu gas-diffusion electrode with the lowest Cu^δ+/Cu⁰ ratio prefers C–C coupling to form C₂₊ products with Faradaic efficiency topping 80.1% at -0.75 V vs RHE, where the Faradaic efficiency of C₂H₄ accounts for 46.4% and the partial current density of C₂H₄ achieves 279 mA cm^-2. This work demonstrates that the selectivity from CH₄ to C₂H₄ is switchable by tuning surface Cu species composition of Cu gas-diffusion electrodes.

View Accepted Manuscript (DOE)

Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF); National Natural Science Foundation of China; Central Universities; Key R&D Projects of Anhui Province; Arizona State University

Grant/Contract Number:: SC0012704

OSTI ID:: 1890212

Report Number(s):: BNL-223518-2022-JAAM

Journal Information:: Energy & Environmental Materials, Journal Name: Energy & Environmental Materials Journal Issue: 2 Vol. 6; ISSN 2575-0356

Publisher:: Wiley - Zhengzhou UniversityCopyright Statement

Country of Publication:: United States

Language:: English

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