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;

D O I：

暂无

中图分类号：

学科分类号：

摘要：

Article in Press

引用

共 50 条

[31] CO2 transformation to multicarbon products by photocatalysis and electrocatalysis
Du, C.
Wang, X.
Chen, W.
Feng, S.
Wen, J.
Wu, Y. A.
MATERIALS TODAY ADVANCES, 2020, 6
[32] Promoting Cu-catalysed CO2 electroreduction to multicarbon products by tuning the activity of H2O
Zhang, Hao
Gao, Jiaxin
Raciti, David
Hall, Anthony Shoji
NATURE CATALYSIS, 2023, 6 (09) : 807 - 817
[33] Direct low concentration CO2 electroreduction to multicarbon products via rate-determining step tuning
Xie, Liangyiqun
Cai, Yanming
Jiang, Yujing
Shen, Meikun
Lam, Jason Chun-Ho
Zhu, Jun-jie
Zhu, Wenlei
NATURE COMMUNICATIONS, 2024, 15 (01)
[34] Metal-Organic Frameworks-Based Copper Catalysts for CO2 Electroreduction Toward Multicarbon Products
Qin, Chen
Li, Xuheng
Wang, Ting
Xu, Zhen
Chen, Kai-Jie
Pan, Fuping
EXPLORATION, 2025,
[35] Activity and Selectivity Control in CO2 Electroreduction to Multicarbon Products over CuOx Catalysts via Electrolyte Design
Gao, Dunfeng
McCrum, Ian T.
Deo, Shyam
Choi, Yong-Wook
Scholten, Fabian
Wan, Weiming
Chen, Jingguang G.
Janik, Michael J.
Roldan Cuenya, Beatriz
ACS CATALYSIS, 2018, 8 (11): : 10012 - +
[36] Fluorine Doping-Assisted Reconstruction of Isolated Cu Sites for CO2 Electroreduction Toward Multicarbon Products
Jia, Chen
Tan, Xin
Sun, Qian
Liu, Ruirui
Hocking, Rosalie K.
Wang, Shuhao
Zhong, Li
Shi, Zhun
Smith, Sean
Zhao, Chuan
ADVANCED MATERIALS, 2025, 37 (09)
[37] Mechanistic Insights into CO2 Electroreduction on Ni2P: Understanding Its Selectivity toward Multicarbon Products
Banerjee, Sayan
Kakekhani, Arvin
Wexler, Robert B.
Rappe, Andrew M.
ACS CATALYSIS, 2021, 11 (18) : 11706 - 11715
[38] Enhancing CO2 Electroreduction Selectivity toward Multicarbon Products via Tuning the Local H2O/CO2 Molar Ratio
Kong, Xiangdong
Wang, Cheng
Xu, Zifan
Zhong, Yongzhi
Liu, Yan
Qin, Lang
Zeng, Jie
Geng, Zhigang
NANO LETTERS, 2022, 22 (19) : 8000 - 8007
[39] Accelerating CO2 Electroreduction to Multicarbon Products via Synergistic Electric-Thermal Field on Copper Nanoneedles
Yang, Baopeng
Liu, Kang
Li, HuangJingWei
Liu, Changxu
Fu, Junwei
Li, Hongmei
Huang, Jianan Erick
Ou, Pengfei
Alkayyali, Tartela
Cai, Chao
Duan, Yuxia
Liu, Hui
An, Pengda
Zhang, Ning
Li, Wenzhang
Qiu, Xiaoqing
Jia, Chuankun
Hu, Junhua
Chai, Liyuan
Lin, Zhang
Gao, Yongli
Miyauchi, Masahiro
Cortes, Emiliano
Maier, Stefan A.
Liu, Min
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2022, 144 (07) : 3039 - 3049
[40] Tandem engineering for CO2 electrolysis toward multicarbon products
Yang, Tinghui
Kuang, Min
Yang, Jianping
NANO RESEARCH, 2023, 16 (07) : 8670 - 8683

← 1 2 3 4 5 →