Confined Intermediates Boost C2+Selectivity in CO2 Electroreduction

被引：14

作者：

Li, Wanhe ^{[1
]}

Chen, Yahui ^{[1
]}

Guo, Chengqi ^{[1
]}

Jia, Shuhan ^{[1
]}

Zhou, Yiying ^{[1
]}

Liu, Zhonghuan ^{[1
]}

Jiang, Enhui ^{[1
]}

Chen, Xiaoke ^{[1
]}

Zou, Yue ^{[1
]}

Huo, Pengwei ^{[1
]}

Yan, Yongshneg ^{[1
]}

Zhu, Zhi ^{[1
]}

Ng, Yun Hau ^{[2
]}

Gong, Yanjun

Crittenden, John Charles

Yan, Yan ^{[1
]}

机构：

[1] Jiangsu Univ, Sch Chem & Chem Engn, Zhenjiang 212013, Peoples R China

[2] City Univ Hong Kong, Sch Energy & Environm, Hong Kong 999077, Peoples R China

来源：

ACS CATALYSIS | 2024年 / 14卷 / 17期

基金：

中国国家自然科学基金;

关键词：

CO2; reduction; Cu2O; confinement space; in situFTIR; molecular dynamics; CARBON-DIOXIDE; ELECTROCHEMICAL REDUCTION; ETHYLENE; COPPER; SELECTIVITY; CATALYSTS;

D O I：

10.1021/acscatal.4c02823

中图分类号：

O64 [物理化学（理论化学）、化学物理学];

学科分类号：

070304 ; 081704 ;

摘要：

Addressing the efficient electrochemical conversion of CO2 (CO2RR) into valuable multicarbon (C2+) products necessitates innovative strategies to boost carbon (C1) intermediate coupling on catalyst surfaces. In this work, we introduce a surface-confinement strategy on Cu2O nanoparticles by long alkyl chain grafting to create a spatially confined environment, impeding C1 intermediate detachment and promoting C-C coupling in the CO2RR. The optimized C12-Cu2O sample exhibits a Faradaic efficiency (FE) over 63.0% for C2H4, more than double the yield of pristine Cu2O (FE = 25.7%). In situ ATR-FTIR spectroscopy provides direct evidence of rapid C1 intermediate enrichment and restricted diffusion within the surface-confined environment. Molecular dynamics simulations further support these findings by identifying a prolonged residency time that is proportionate to the alkyl chain length, thereby maximizing C2+ selectivity. This surface-confinement approach marks a previously overlooked but immensely promising paradigm in the catalyst design for the CO2RR.

引用

页码：13400 / 13407

页数：8

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