Fe, Cu dual-metal single atom catalyst on commercial carbon black for efficient oxygen reduction reaction

被引:71
作者
Yang, Hongzhou [1 ,2 ]
Huang, He [1 ]
Wang, Qing [2 ]
Shang, Lu [2 ]
Zhang, Tierui [2 ,3 ]
Wang, Shouguo [1 ,4 ]
机构
[1] Univ Sci & Technol Beijing, Beijing Adv Innovat Ctr Mat Genome Engn, Sch Mat Sci & Engn, Beijing 100083, Peoples R China
[2] Chinese Acad Sci, Optoelect Mat Tech Inst Phys & Chem, Key Lab Photochem Convers, Beijing 100190, Peoples R China
[3] Univ Chinese Acad Sci, Ctr Mat Sci & Optoelect Engn, Beijing 100049, Peoples R China
[4] Anhui Univ, Sch Mat Sci & Engn, Hefei 230601, Peoples R China
基金
中国国家自然科学基金; 北京市自然科学基金;
关键词
ACTIVE-SITES; N-C; ELECTROCATALYSTS; PERFORMANCE; COPPER; IRON; ZN; DESIGN;
D O I
10.1039/d2ta09922e
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
3d transition metal single atom catalysts (SACs) (e.g. M = Fe, Co, Cu) are considered as promising catalysts for oxygen reduction reaction (ORR), among which Fe SACs display comparable performance to commercial Pt/C. However, Fe SACs still demand significant improvements in activity and stability for further industrial deployment. Herein, a Fe, Cu dual metal SAC was synthesized using a facile ligand-mediated method. Fe and Cu atoms were atomically dispersed on commercial carbon black in the form of FeN4 and CuN4 sites. Owing to the interactions between the adjacent Fe and Cu atoms co-existing in a very tiny area, the as-synthesized Fe, Cu dual metal SAC exhibited excellent ORR performance with a high half-wave potential of 0.926 V and good stability in 0.1 M KOH, which are significantly higher than that of the Fe-SAC or Cu-SAC control samples. Density function theory calculations showed that the Cu single atom can act as an electron donator enriching the electron density of Fe sites, thus endowing the Fe sites with optimized adsorption/desorption energy for ORR intermediates and thereby facilitating the ORR activity of FeCu-SAC. Moreover, a study on three typical commercial carbon substrates indicated that carbon support with high surface areas and hierarchical pore structure was beneficial for ORR. The excellent ORR activity and durability of FeCu-SAC enabled the constructed Zn-air battery to have a high power density of 201.4 mW cm(-2) and high specific energy of 827.68 W h kg(-1).
引用
收藏
页码:6191 / 6197
页数:7
相关论文
共 65 条
[1]   Recent Advances in Dual-Atom Site Catalysts for Efficient Oxygen and Carbon Dioxide Electrocatalysis [J].
An, Qizheng ;
Jiang, Jingjing ;
Cheng, Weiren ;
Su, Hui ;
Jiang, Yong ;
Liu, Qinghua .
SMALL METHODS, 2022, 6 (07)
[2]   Doped MXene combinations as highly efficient bifunctional and multifunctional catalysts for water splitting and metal-air batteries [J].
Anand, Rohit ;
Ram, Babu ;
Umer, Muhammad ;
Zafari, Mohammad ;
Umer, Sohaib ;
Lee, Geunsik ;
Kim, Kwang S. .
JOURNAL OF MATERIALS CHEMISTRY A, 2022, 10 (42) :22500-22511
[3]   Dual Single-Atomic Ni-N4and Fe-N4Sites Constructing Janus Hollow Graphene for Selective Oxygen Electrocatalysis [J].
Chen, Jiangyue ;
Li, Hao ;
Fan, Chuang ;
Meng, Qingwei ;
Tang, Yawen ;
Qiu, Xiaoyu ;
Fu, Gengtao ;
Ma, Tianyi .
ADVANCED MATERIALS, 2020, 32 (30)
[4]   Enhanced oxygen reduction with single-atomic-site iron catalysts for a zinc-air battery and hydrogen-air fuel cell [J].
Chen, Yuanjun ;
Ji, Shufang ;
Zhao, Shu ;
Chen, Wenxing ;
Dong, Juncai ;
Cheong, Weng-Chon ;
Shen, Rongan ;
Wen, Xiaodong ;
Zheng, Lirong ;
Rykov, Alexandre I. ;
Cai, Shichang ;
Tang, Haolin ;
Zhuang, Zhongbin ;
Chen, Chen ;
Peng, Qing ;
Wang, Dingsheng ;
Li, Yadong .
NATURE COMMUNICATIONS, 2018, 9
[5]   Boosting oxygen reduction reaction with Fe and Se dual-atom sites supported by nitrogen-doped porous carbon [J].
Chen, Zhaoyang ;
Su, Xiaozhi ;
Ding, Jie ;
Yang, Na ;
Zuo, Wenbin ;
He, Qinye ;
Wei, Zhiming ;
Zhang, Qiao ;
Huang, Jian ;
Zhai, Yueming .
APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY, 2022, 308
[6]   Enhanced performance of atomically dispersed dual-site Fe-Mn electrocatalysts through cascade reaction mechanism [J].
Chen, Zhe ;
Liao, Xiaobin ;
Sun, Congli ;
Zhao, Kangning ;
Ye, Daixin ;
Li, Jiantao ;
Wu, Gang ;
Fang, Jianhui ;
Zhao, Hongbin ;
Zhang, Jiujun .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2021, 288
[7]   Metal-air batteries: from oxygen reduction electrochemistry to cathode catalysts [J].
Cheng, Fangyi ;
Chen, Jun .
CHEMICAL SOCIETY REVIEWS, 2012, 41 (06) :2172-2192
[8]   A copper single-atom catalyst towards efficient and durable oxygen reduction for fuel cells [J].
Cui, Liting ;
Cui, Lirui ;
Li, Zhengjian ;
Zhang, Jin ;
Wang, Haining ;
Lu, Shanfu ;
Xiang, Yan .
JOURNAL OF MATERIALS CHEMISTRY A, 2019, 7 (28) :16690-16695
[9]   Engineering Dual Single-Atom Sites on 2D Ultrathin N-doped Carbon Nanosheets Attaining Ultra-Low-Temperature Zinc-Air Battery [J].
Cui, Tingting ;
Wang, Yun-Peng ;
Ye, Tong ;
Wu, Jiao ;
Chen, Zhiqiang ;
Li, Jiong ;
Lei, Yongpeng ;
Wang, Dingsheng ;
Li, Yadong .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2022, 61 (12)
[10]   Cobalt-doped Mn3O4 nanocrystals embedded in graphene nanosheets as a high-performance bifunctional oxygen electrocatalyst for rechargeable Zn-Air batteries [J].
Dong, Mengyang ;
Liu, Xu ;
Jiang, Lixue ;
Zhu, Zhengju ;
Shu, Yajie ;
Chen, Shan ;
Dou, Yuhai ;
Liu, Porun ;
Yin, Huajie ;
Zhao, Huijun .
GREEN ENERGY & ENVIRONMENT, 2020, 5 (04) :499-505