Boosting CO2 Electroreduction to Multi-carbon Products via Oxygen-rich Vacancies and Ce4+-O2--Cu+ Structure in Cu/CeO2 for Stabilizing Cu+

被引:3
作者
Fang, Minghui [1 ]
Xia, Wei [1 ]
Han, Shitao [1 ]
Yao, Ting [1 ]
Wang, Min [1 ]
Zhou, Dawei [1 ]
Dong, Xue [1 ]
Yang, Jiahao [1 ]
Jia, Shuaiqiang [1 ]
He, Mingyuan [1 ]
Wu, Haihong [1 ,2 ]
Han, Buxing [1 ,2 ,3 ]
机构
[1] East China Normal Univ, Sch Chem & Mol Engn, Shanghai Key Lab Green Chem & Chem Proc, Shanghai 200062, Peoples R China
[2] Inst Ecochongming, Shanghai 202162, Peoples R China
[3] Chinese Acad Sci, CAS Key Lab Colloid Interface & Chem Thermodynam, Beijing Natl Lab Mol Sci,Ctr Carbon Neutral Chem, CAS Res Educ Ctr Excellence Mol Sci,Inst Chem, Beijing 100190, Peoples R China
基金
中国国家自然科学基金;
关键词
Copper-ceria; C2+ production; Electrocatalyst; Electrochemical CO2 reduction; Oxygen vacancy; COPPER-CERIA; CATALYSTS; REDUCTION; OXIDATION; METHANOL;
D O I
10.1002/cctc.202301266
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
Cu is a promising electrocatalyst for the CO2 reduction reaction (CO2RR) to produce high-value C2+ products. Due to the fierce competition of the hydrogen evolution reaction, the slow diffusion of CO2, and the high energy barrier of the C C coupling reaction, it is still challenging to achieve high activity and high selectivity to produce multi-carbon products on copper-based electrocatalysts. In this work, we synthesized Cu/ CeO2 catalysts with varying amounts of Cu doping, aiming at effectively converting CO2 into C2+ products through electroreduction. At a copper doping level of 9.77 wt%, the catalyst exhibited a current density of 16.8 mAcm 2 using a standard H- type cell, achieving a C2+ faradaic efficiency (FE) of 78.3%. Through additional experiments and material characterization, we confirmed that controlling the Cu loading on the surface of CeO2 is an effective way to regulate the ratio of Cu+ to Cu0 active sites and the number of oxygen vacancies. Furthermore, the strong electron interaction between Ce-4+ O-2 Cu+ structure can stabilize Cu+ species and enhance the overall stability of the catalyst. This strategy enhances the selectivity towards C2+ products and effectively suppresses the competing hydrogen evolution reaction.
引用
收藏
页数:8
相关论文
共 53 条
[1]   Dynamic Stability of Copper Single-Atom Catalysts under Working Conditions [J].
Bai, Xiaowan ;
Zhao, Xunhua ;
Zhang, Yehui ;
Ling, Chongyi ;
Zhou, Yipeng ;
Wang, Jinlan ;
Liu, Yuanyue .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2022, 144 (37) :17140-17148
[2]   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
[3]   MOF Encapsulating N-Heterocyclic Carbene-Ligated Copper Single-Atom Site Catalyst towards Efficient Methane Electrosynthesis [J].
Chen, Shenghua ;
Li, Wen-Hao ;
Jiang, Wenjun ;
Yang, Jiarui ;
Zhu, Jiexin ;
Wang, Liqiang ;
Ou, Honghui ;
Zhuang, Zechao ;
Chen, Mingzhao ;
Sun, Xiaohui ;
Wang, Dingsheng ;
Li, Yadong .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2022, 61 (04)
[4]   Promoting water dissociation for efficient solar driven CO2 electroreduction via improving hydroxyl adsorption [J].
Chen, Xin ;
Chen, Junxiang ;
Chen, Huayu ;
Zhang, Qiqi ;
Li, Jiaxuan ;
Cui, Jiwei ;
Sun, Yanhui ;
Wang, Defa ;
Ye, Jinhua ;
Liu, Lequan .
NATURE COMMUNICATIONS, 2023, 14 (01)
[5]   Interfacial Electrolyte Effects on Electrocatalytic CO2 Reduction [J].
Deng, Bangwei ;
Huang, Ming ;
Zhao, Xiaoli ;
Mou, Shiyong ;
Dong, Fan .
ACS CATALYSIS, 2022, 12 (01) :331-362
[6]   Improving CO2-to-C2+Product Electroreduction Efficiency via Atomic Lanthanide Dopant-Induced Tensile-Strained CuOx Catalysts [J].
Feng, Jiaqi ;
Wu, Limin ;
Liu, Shoujie ;
Xu, Liang ;
Song, Xinning ;
Zhang, Libing ;
Zhu, Qinggong ;
Kang, Xinchen ;
Sun, Xiaofu ;
Han, Buxing .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2023, 145 (17) :9857-9866
[7]   Highly active copper-ceria and copper-ceria-titania catalysts for methanol synthesis from CO2 [J].
Graciani, Jesus ;
Mudiyanselage, Kumudu ;
Xu, Fang ;
Baber, Ashleigh E. ;
Evans, Jaime ;
Senanayake, Sanjaya D. ;
Stacchiola, Dario J. ;
Liu, Ping ;
Hrbek, Jan ;
Fernandez Sanz, Javier ;
Rodriguez, Jose A. .
SCIENCE, 2014, 345 (6196) :546-550
[8]   Solvent-induced fabrication of Cu/MnOx nanosheets with abundant oxygen vacancies for efficient and long-lasting photothermal catalytic degradation of humid toluene vapor [J].
Jiang, Shanliang ;
Li, Changhao ;
Muhammad, Yaseen ;
Tang, Ying ;
Wang, Ruimeng ;
Li, Junjie ;
Li, Jing ;
Zhao, Zhongxing ;
Zhao, Zhenxia .
APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY, 2023, 328
[9]   Structural Reconstruction of Cu2O Superparticles toward Electrocatalytic CO2 Reduction with High C2+ Products Selectivity [J].
Jiang, Yawen ;
Wang, Xinyu ;
Duan, Delong ;
He, Chaohua ;
Ma, Jun ;
Zhang, Wenqing ;
Liu, Hengjie ;
Long, Ran ;
Li, Zibiao ;
Kong, Tingting ;
Loh, Xian Jun ;
Song, Li ;
Ye, Enyi ;
Xiong, Yujie .
ADVANCED SCIENCE, 2022, 9 (16)
[10]   Stabilizing Oxidation State of SnO2 for Highly Selective CO2 Electroreduction to Formate at Large Current Densities [J].
Jiang, Yunling ;
Shan, Jieqiong ;
Wang, Pengtang ;
Huang, Linsen ;
Zheng, Yao ;
Qiao, Shi-Zhang .
ACS CATALYSIS, 2023, 13 (05) :3101-3108