Chiral Nanostructured Ag Films for Multicarbon Products from CO2 Electroreduction

被引：0

作者：

Zhang, Wanning ^{[1
]}

Ai, Jing ^{[2
]}

Ouyang, Tianwei ^{[1
]}

Yu, Lu ^{[3
,4
]}

Liu, Aokun ^{[3
,4
]}

Han, Lu ^{[5
]}

Duan, Yingying ^{[5
]}

Tian, Changlin ^{[3
,4
]}

Chu, Chaoyang ^{[6
]}

Ma, Yanhang ^{[6
]}

Che, Shunai ^{[1
]}

Fang, Yuxi ^{[1
]}

机构：

[1] School of Chemistry and Chemical Engineering, Frontiers Science Center for Transformative Molecules, State Key Laboratory of Metal Matrix Composites, Shanghai Key Laboratory for Molecular Engineering of Chiral Drugs, Shanghai Jiao Tong University, 800 Dong

[2] Sinopec Shanghai Research Institute of Petrochemical Technology, 1658 Pudong Beilu, Shanghai,201208, China

[3] High Magnetic Field Laboratory, Hefei Institutes of Physical Science, Chinese Academy of Sciences, 350 Shushanhu Road, Anhui, Hefei,230031, China

[4] Division of Life Sciences and Medicine, Anhui Engineering Laboratory of Peptide Drug, Anhui Laboratory of Advanced Photonic Science and Technology, University of Science and Technology of China, 96 Jinzhai Road, Anhui, Hefei,230026, China

[5] School of Chemical Science and Engineering, Tongji University, 1239 Siping Road, Shanghai,200092, China

[6] Centre for High Resolution Electron Microscopy, Shanghai Key Lab of High-Resolution Microscopy, ShanghaiTech University, Shanghai,201210, China

来源：

Journal of the American Chemical Society | 2024年

关键词：

The formation of multicarbon products from CO2 electroreduction is challenging on materials other than Cu-based catalysts. Ag has been known to be a typical metal catalyst; producing CO in CO2 electroreduction. The formation of C2+ products by Ag has never been reported because the carbon-carbon (C-C) coupling is an unfavorable process due to the high reaction barrier energy of *OCCO. Here; we propose that the chirality-induced spin polarization of chiral nanostructured Ag films (CNAFs) can promote the formation of triplet OCCO by regulating its parallel electron spin alignment; and the helical lattice distortion of nanostructures can decrease the reaction energy of *OCCO; which triggers C-C coupling and promotes subsequent *OCCO hydrogenation to facilitate the generation of C2+ products. The CNAFs with helically lattice-distorted nanoflakes were fabricated via electrodeposition using phenylalanine as the symmetry-breaking agent. C2+ products (C2H4; C2H6; C3H8; C2H5OH; and CH3COOH) with a Faradaic efficiency of ∼4.7% and a current density of ∼22 mA/cm2 were generated in KHCO3 electrolytes under 12.5 atm of CO2 (g). Our findings propose that the chiral nanostructured materials can regulate the multifunctionality of catalytic performance in the catalytic reactions with triplet intermediates and products. © 2024 American Chemical Society;

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摘要：

Article in Press

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