Inhibiting Demetalation of Fe―N―C via Mn Sites for Efficient Oxygen Reduction Reaction in Zinc-Air Batteries

被引:79
作者
Hu, Chuan [1 ]
Xing, Gengyu [1 ]
Han, Wentao [1 ]
Hao, Yixin [1 ]
Zhang, Chenchen [2 ]
Zhang, Ying [2 ]
Kuo, Chun-Han [3 ]
Chen, Han-Yi [3 ]
Hu, Feng [1 ]
Li, Linlin [1 ]
Peng, Shengjie [1 ]
机构
[1] Nanjing Univ Aeronaut & Astronaut, Coll Mat Sci & Technol, Nanjing 210016, Peoples R China
[2] Jiangnan Univ, Sch Chem & Mat Engn, Minist Educ, Key Lab Synthet & Biol Colloids, Wuxi 214122, Jiangsu, Peoples R China
[3] Natl Tsing Hua Univ, Dept Mat Sci & Engn, Hsinchu 30013, Taiwan
基金
中国国家自然科学基金;
关键词
demetalation effect; dual atomic sites; Fe & horbar; N & horbar; C; oxygen reduction reaction; Zn-air batteries; DURABILITY; IMPROVE;
D O I
10.1002/adma.202405763
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Demetalation caused by the electrochemical dissolution of metallic Fe atoms is a major challenge for the practical application of Fe & horbar;N & horbar;C catalysts. Herein, an efficient single metallic Mn active site is constructed to improve the strength of the Fe & horbar;N bond, inhibiting the demetalation effect of Fe & horbar;N & horbar;C. Mn acts as an electron donor inducing more delocalized electrons to reduce the oxidation state of Fe by increasing the electron density, thereby enhancing the Fe & horbar;N bond and inhibiting the electrochemical dissolution of Fe. The oxygen reduction reaction pathway for the dissociation of Fe & horbar;Mn dual sites can overcome the high energy barriers to direct O & horbar;O bond dissociation and modulate the electronic states of Fe & horbar;N4 sites. The resulting FeMn & horbar;N & horbar;C exhibits excellent ORR activity with a high half-wave potential of 0.92 V in alkaline electrolytes. FeMn & horbar;N & horbar;C as a cathode catalyst for Zn-air batteries has a cycle stability of 700 h at 25 degrees C and a long cycle stability of more than 210 h under extremely cold conditions at -40 degrees C. These findings contribute to the development of efficient and stable metal-nitrogen-carbon catalysts for various energy devices. Mn acts as an electron donor to reduce the oxidation state of Fe by increasing the electron density at the Fe & horbar;N4 site, thereby strengthening the Fe & horbar;N bond and inhibiting the electrochemical dissolution of Fe. As a result, FeMn & horbar;N & horbar;C exhibits excellent discharge performance and stability in Zn-air batteries. image
引用
收藏
页数:12
相关论文
共 52 条
[11]   Breaking Sabatier's vertex via switching the oxygen adsorption configuration and reaction pathway on dual active sites for acidic oxygen reduction [J].
Guo, Pan ;
Liu, Bo ;
Tu, Fengdi ;
Dai, Yunkun ;
Zhang, Ziyu ;
Xia, Yunfei ;
Ma, Miao ;
Zhang, Yunlong ;
Zhao, Lei ;
Wang, Zhenbo .
ENERGY & ENVIRONMENTAL SCIENCE, 2024, 17 (09) :3077-3087
[12]   An Adjacent Atomic Platinum Site Enables Single-Atom Iron with High Oxygen Reduction Reaction Performance [J].
Han, Ali ;
Wang, Xijun ;
Tang, Kun ;
Zhang, Zedong ;
Ye, Chenliang ;
Kong, Kejian ;
Hu, Haibo ;
Zheng, Lirong ;
Jiang, Peng ;
Zhao, Changxin ;
Zhang, Qiang ;
Wang, Dingsheng ;
Li, Yadong .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2021, 60 (35) :19262-19271
[13]   Stereodivergent Construction of Csp3-Csp3 Bonds Bearing Vicinal Stereocenters by Synergistic Palladium and Phase-Transfer Catalysis [J].
Han, Jingqiang ;
Liu, Rixin ;
Lin, Zitong ;
Zi, Weiwei .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2023, 62 (02)
[14]   Atomically Dispersed Binary Co-Ni Sites in Nitrogen-Doped Hollow Carbon Nanocubes for Reversible Oxygen Reduction and Evolution [J].
Han, Xiaopeng ;
Ling, Xiaofei ;
Yu, Deshuang ;
Xie, Dengyu ;
Li, Linlin ;
Peng, Shengjie ;
Zhong, Cheng ;
Zhao, Naiqin ;
Deng, Yida ;
Hu, Wenbin .
ADVANCED MATERIALS, 2019, 31 (49)
[15]   Generation of Nanoparticle, Atomic-Cluster, and Single-Atom Cobalt Catalysts from Zeolitic Imidazole Frameworks by Spatial Isolation and Their Use in Zinc-Air Batteries [J].
Han, Xiaopeng ;
Ling, Xiaofei ;
Wang, Ying ;
Ma, Tianyi ;
Zhong, Cheng ;
Hu, Wenbin ;
Deng, Yida .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2019, 58 (16) :5359-5364
[16]   Hollow N-Doped Carbon Spheres with Isolated Cobalt Single Atomic Sites: Superior Electrocatalysts for Oxygen Reduction [J].
Han, Yunhu ;
Wang, Yang-Gang ;
Chen, Wenxing ;
Xu, Ruirui ;
Zheng, Lirong ;
Zhang, Jian ;
Luo, Jun ;
Shen, Rong-An ;
Zhu, Youqi ;
Cheong, Weng-Chon ;
Chen, Chen ;
Peng, Qing ;
Wang, Dingsheng ;
Li, Yadong .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2017, 139 (48) :17269-17272
[17]   Clusters Induced Electron Redistribution to Tune Oxygen Reduction Activity of Transition Metal Single-Atom for Metal-Air Batteries [J].
Huang, Hongjiao ;
Yu, Deshuang ;
Hu, Feng ;
Huang, Shao-Chu ;
Song, Junnan ;
Chen, Han-Yi ;
Li, Lin Lin ;
Peng, Shengjie .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2022, 61 (12)
[18]   Tailoring Oxygen Reduction Reaction Kinetics on Perovskite Oxides via Oxygen Vacancies for Low-Temperature and Knittable Zinc-Air Batteries [J].
Huang, Hongjiao ;
Huang, Aoming ;
Liu, Di ;
Han, Wentao ;
Kuo, Chun-Han ;
Chen, Han-Yi ;
Li, Linlin ;
Pan, Hui ;
Peng, Shengjie .
ADVANCED MATERIALS, 2023, 35 (36)
[19]  
Huang L, 2022, NAT COMMUN, V13, DOI 10.1038/s41467-022-34444-w
[20]   Axial Oxygen Ligands Regulating Electronic and Geometric Structure of Zn-N-C Sites to Boost Oxygen Reduction Reaction [J].
Jin, Qiuyan ;
Wang, Chenhui ;
Guo, Yingying ;
Xiao, Yuhang ;
Tan, Xiaohong ;
Chen, Jianpo ;
He, Weidong ;
Li, Yan ;
Cui, Hao ;
Wang, Chengxin .
ADVANCED SCIENCE, 2023, 10 (24)