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

被引:74
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
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页数:12
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