Stabilizing Copper by a Reconstruction-Resistant Atomic Cu-O-Si Interface for Electrochemical CO2 Reduction

被引:145
作者
Tan, Xin [1 ]
Sun, Kaian [1 ]
Zhuang, Zewen [1 ,2 ]
Hu, Botao [1 ,3 ]
Zhang, Yu [1 ]
Liu, Qinggang [4 ]
He, Chang [1 ]
Xu, Zhiyuan [1 ]
Chen, Chang [1 ]
Xiao, Hai [1 ]
Chen, Chen [1 ]
机构
[1] Tsinghua Univ, Engn Res Ctr Adv Rare Earth Mat, Dept Chem, Beijing 100084, Peoples R China
[2] Fuzhou Univ, Coll Mat Sci & Engn, Fuzhou 350108, Peoples R China
[3] China Acad Space Technol, Qian Xuesen Lab Space Technol, Beijing 100094, Peoples R China
[4] Chinese Acad Sci, Dalian Inst Chem Phys, Dalian 116023, Peoples R China
基金
中国国家自然科学基金;
关键词
CARBON-DIOXIDE; ELECTROREDUCTION; METHANE; HYDROCARBONS; EFFICIENCY; CATALYSTS;
D O I
10.1021/jacs.3c01638
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Copper (Cu), a promising catalyst for electrochemical CO2 reduction (CO2R) to multi-electron reduction products, suffers from an unavoidable and uncontrollable reconstruction process during the reaction, which not only may lead to catalyst deactivation but also brings great challenges to the exploration of the structure-performance relationship. Herein, we present an efficient strategy for stabilizing Cu with silica and synthesize reconstruction-resistant CuSiOx amorphous nanotube catalysts with abundant atomic Cu-O-Si interfacial sites. The strong interfacial interaction between Cu and silica makes the Cu-O-Si interfacial sites ultrastable in the CO2R reaction without any apparent reconstruction, thus exhibiting high CO2-to-CH4 selectivity (72.5%) and stability (FECH4 remains above 60% after 12 h of test). A remarkable CO2-to-CH4 conversion rate of 0.22 mu mol cm-2 s-1 was also achieved in a flow cell device. This work provides a very promising route for the design of highly active and stable Cu-based CO2R catalysts.
引用
收藏
页码:8656 / 8664
页数:9
相关论文
共 57 条
[1]   Advances and challenges in understanding the electrocatalytic conversion of carbon dioxide to fuels [J].
Birdja, Yuvraj Y. ;
Perez-Gallent, Elena ;
Figueiredo, Marta C. ;
Gottle, Adrien J. ;
Calle-Vallejo, Federico ;
Koper, Marc T. M. .
NATURE ENERGY, 2019, 4 (09) :732-745
[2]   Dynamic Reoxidation/Reduction-Driven Atomic Interdiffusion for Highly Selective CO2 Reduction toward Methane [J].
Chang, Chia-Jui ;
Lin, Sheng-Chih ;
Chen, Hsiao-Chien ;
Wang, Jiali ;
Zheng, Kai Jen ;
Zhu, Yanping ;
Chen, Hao Ming .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2020, 142 (28) :12119-12132
[3]   Lewis Acid Site-Promoted Single-Atomic Cu Catalyzes Electrochemical CO2 Methanation [J].
Chen, Shenghua ;
Wang, Bingqing ;
Zhu, Jiexin ;
Wang, Liqiang ;
Ou, Honghui ;
Zhang, Zedong ;
Liang, Xiao ;
Zheng, Lirong ;
Zhou, Liang ;
Su, Ya-Qiong ;
Wang, Dingsheng ;
Li, Yadong .
NANO LETTERS, 2021, 21 (17) :7325-7331
[4]   Highly Selective Carbon Dioxide Electroreduction on Structure-Evolved Copper Perovskite Oxide toward Methane Production [J].
Chen, Shenghua ;
Su, Yaqiong ;
Deng, Peilin ;
Qi, Ruijuan ;
Zhu, Jiexin ;
Chen, Jinxi ;
Wang, Zhitong ;
Zhou, Liang ;
Guo, Xingpeng ;
Xia, Bao Yu .
ACS CATALYSIS, 2020, 10 (08) :4640-4646
[5]   Transition metal doped graphene-like germanium carbide: Screening of high performance electrocatalysts for oxygen reduction, oxygen evolution, or hydrogen evolution [J].
Chen, Xin ;
Zhang, Hui ;
Zhang, Yizhen .
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS, 2021, 630
[6]   Tuning local carbon active sites saturability of graphitic carbon nitride to boost CO2 electroreduction towards CH4 [J].
Chen, Zhou ;
Gao, Min-Rui ;
Zhang, Ya-Qian ;
Duan, Nanqi ;
Fan, Tingting ;
Xiao, Jing ;
Zhang, Jiawei ;
Dong, Yunyun ;
Li, Jianhui ;
Yi, Xiaodong ;
Luo, Jing-Li .
NANO ENERGY, 2020, 73
[7]   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
[8]   The Crystal Plane is not the Key Factor for CO2-to-Methane Electrosynthesis on Reconstructed Cu2O Microparticles [J].
Deng, Bangwei ;
Huang, Ming ;
Li, Kanglu ;
Zhao, Xiaoli ;
Geng, Qin ;
Chen, Si ;
Xie, Hongtao ;
Dong, Xing'an ;
Wang, Hong ;
Dong, Fan .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2022, 61 (07)
[9]  
Duan X., CHEM ENG J, V2022
[10]   Rational catalyst and electrolyte design for CO2 electroreduction towards multicarbon products [J].
Gao, Dunfeng ;
Aran-Ais, Rosa M. ;
Jeon, Hyo Sang ;
Roldan Cuenya, Beatriz .
NATURE CATALYSIS, 2019, 2 (03) :198-210