Nanoconfinement Effects of Yolk-Shell Cu2O Catalyst for Improved C2+ Selectivity and Cu+ Stability in Electrocatalytic CO2 Reduction

被引：19

作者：

Lu, Jinghao ^{[1
]}

Yang, Lili ^{[1
]}

Zhang, Yishuai ^{[1
]}

Wang, Chao ^{[1
]}

Zhang, Chuanhui ^{[1
]}

Zhao, Xiu Song ^{[1
]}

机构：

[1] Qingdao Univ, Inst Mat Energy & Environm, Coll Mat Sci & Engn, Qingdao 266071, Peoples R China

来源：

ACS APPLIED NANO MATERIALS | 2023年 / 6卷 / 22期

基金：

中国国家自然科学基金;

关键词：

Cu2O; yolk-shellstructure; CO2; reduction; nanoconfinement; selectivity; in situ ATR-SEIRAS; ELECTROCHEMICAL REDUCTION; OXIDATION-STATE; COPPER; ELECTROREDUCTION; ELECTRODES; OPERANDO; SURFACE;

D O I：

10.1021/acsanm.3c03645

中图分类号：

TB3 [工程材料学];

学科分类号：

0805 ; 080502 ;

摘要：

Electrocatalytic conversion of carbon dioxide (CO2) to value-added hydrocarbon products provides an industrially viable approach to utilizing carbon resources and the storage of renewable energy. Monovalent copper (Cu+) has been demonstrated to be indispensable for the formation of C2+ products via C-C coupling. However, the C2+ selectivity and stability of Cu+ at the cathodic potential remain a great challenge. In this work, we investigated the electrochemical properties of three Cu-based catalysts with different structures in the electrocatalytic reduction of the CO2 reaction (eCO(2)RR). Results showed that a Cu2O catalyst with a yolk-shell microstructure having a distance between the shell internal surface and the core external surface of 25 nm displays the best performance. It exhibits a C2+ Faradaic efficiency of 80.2% and a FEC2+ to FEC1 ratio of similar to 8.9. Both in situ ATR-SEIRAS and ex situ XPS characterization results reveal that Cu+ is stable under the experimental conditions, and the coverage of adsorbed carbon monoxide (*CO) on the Cu+ active site is enhanced due to nanoconfinement effects. The increased *CO surface coverage significantly promotes C-C coupling, leading to enhanced C2+ selectivity.

引用

页码：20746 / 20756

页数：11

共 63 条

[1] Structure of the catalytically active copper-ceria interfacial perimeter [J].

Chen, Aling ;

Yu, Xiaojuan ;

Zhou, Yan ;

Miao, Shu ;

Li, Yong ;

Kuld, Sebastian ;

Sehested, Jens ;

Liu, Jingyue ;

Aoki, Toshihiro ;

Hong, Song ;

Camellone, Matteo Farnesi ;

Fabris, Stefano ;

Ning, Jing ;

Jin, Chuanchuan ;

Yang, Chengwu ;

Nefedov, Alexei ;

Woell, Christof ;

Wang, Yuemin ;

Shen, Wenjie .

NATURE CATALYSIS, 2019, 2 (04) :334-341

[2] Mechanically induced Cu active sites for selective C-C coupling in CO2 electroreduction [J].

Chen, Zhao ;

Song, Yao ;

Zhang, Zhenyu ;

Cai, Yafeng ;

Liu, Huan ;

Xie, Wenxiang ;

Deng, Dehui .

JOURNAL OF ENERGY CHEMISTRY, 2022, 74 :198-202

[3] Nature of the Active Sites for CO Reduction on Copper Nanoparticles; Suggestions for Optimizing Performance [J].

Cheng, Tao ;

Xiao, Hai ;

Goddard, William A. .

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2017, 139 (34) :11642-11645

[4] Controlling the Oxidation State of the Cu Electrode and Reaction Intermediates for Electrochemical CO2 Reduction to Ethylene [J].

Chou, Tsu-Chin ;

Chang, Chiao-Chun ;

Yu, Hung-Ling ;

Yu, Wen-Yueh ;

Dong, Chung-Li ;

Velasco-Velez, Juan Jesus ;

Chuang, Cheng-Hao ;

Chen, Li-Chyong ;

Lee, Jyh-Fu ;

Chen, Jin-Ming ;

Wu, Heng-Liang .

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2020, 142 (06) :2857-2867

[5] Facet-Dependent Selectivity of Cu Catalysts in Electrochemical CO2 Reduction at Commercially Viable Current Densities [J].

De Gregorio, Gian Luca ;

Burdyny, Tom ;

Loiudice, Anna ;

Iyengar, Pranit ;

Smith, Wilson A. ;

Buonsanti, Raffaella .

ACS CATALYSIS, 2020, 10 (09) :4854-4862

[6] Catalyst electro-redeposition controls morphology and oxidation state for selective carbon dioxide reduction [J].

De Luna, Phil ;

Quintero-Bermudez, Rafael ;

Cao-Thang Dinh ;

Ross, Michael B. ;

Bushuyev, Oleksandr S. ;

Todorovic, Petar ;

Regier, Tom ;

Kelley, Shana O. ;

Yang, Peidong ;

Sargent, Edward H. .

NATURE CATALYSIS, 2018, 1 (02) :103-110

[7] CO2 electroreduction to ethylene via hydroxide-mediated copper catalysis at an abrupt interface [J].

Dinh, Cao-Thang ;

Burdyny, Thomas ;

Kibria, Md Golam ;

Seifitokaldani, Ali ;

Gabardo, Christine M. ;

de Arquer, F. Pelayo Garcia ;

Kiani, Amirreza ;

Edwards, Jonathan P. ;

De Luna, Phil ;

Bushuyev, Oleksandr S. ;

Zou, Chengqin ;

Quintero-Bermudez, Rafael ;

Pang, Yuanjie ;

Sinton, David ;

Sargent, Edward H. .

SCIENCE, 2018, 360 (6390) :783-787

[8] Cu-C(O) Interfaces Deliver Remarkable Selectivity and Stability for CO2 Reduction to C2+ Products at Industrial Current Density of 500 mA cm-2 [J].

Du, Ruian ;

Wu, Qiqi ;

Zhang, Shiyi ;

Wang, Peng ;

Li, Zhengjian ;

Qiu, Yongcai ;

Yan, Keyou ;

Waterhouse, Geoffrey I. N. ;

Wang, Pei ;

Li, Jia ;

Zhao, Yun ;

Zhao, Wei-Wei ;

Wang, Xue ;

Chen, Guangxu .

SMALL, 2023, 19 (28)

[9] In Situ Engineering of the Cu+/Cu0 Interface to Boost C2+ Selectivity in CO2 Electroreduction [J].

Du, Ruian ;

Li, Tan ;

Wu, Qiqi ;

Wang, Peng ;

Yang, Xianfeng ;

Fan, Yan ;

Qiu, Yongcai ;

Yan, Keyou ;

Wang, Pei ;

Zhao, Yun ;

Zhao, Wei-Wei ;

Chen, Guangxu .

ACS APPLIED MATERIALS & INTERFACES, 2022, 14 (32) :36527-36535

[10] Selective CO2 Electroreduction to Ethylene and Multicarbon Alcohols via Electrolyte-Driven Nanostructuring [J].

Gao, Dunfeng ;

Sinev, Ilya ;

Scholten, Fabian ;

Aran-Ais, Rosa M. ;

Divins, Nuria J. ;

Kvashnina, Kristina ;

Timoshenko, Janis ;

Roldan Cuenya, Beatriz .

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2019, 58 (47) :17047-17053

← 1 2 3 4 5 6 7 →