Anti-dissolving Fe2N6 site-based carbon fiber membranes for binder-free Zn–air batteries with a 200-day lifespan

Zian Xu; Jian Zhu; Jingze Shao; Yu Xia; Pengfei Liu; Guangshe Li; Rouxi Chen; Shaoqing Chen; Jiacheng Wang; Shi Chen; Fuqiang Huang; Hsing-Lin Wang

doi:10.1039/D4EE03148B

Anti-dissolving Fe₂N₆ site-based carbon fiber membranes for binder-free Zn–air batteries with a 200-day lifespan†

Zian Xu,‡^ac Jian Zhu,‡^a Jingze Shao,‡^d Yu Xia,^g Pengfei Liu,

^f Guangshe Li,^d Rouxi Chen,*^h Shaoqing Chen,^e Jiacheng Wang,ⁱ Shi Chen,

*^c Fuqiang Huang

*^b and Hsing-Lin Wang*^a

Author affiliations

* Corresponding authors

^a Department of Materials Science and Engineering, Southern University of Science and Technology, Shenzhen, P. R. China
E-mail: wangxl3@sustech.edu.cn

^b State Key Lab of Metal Matrix Composites, School of Materials Science and Engineering, Shanghai Jiao Tong University, Shanghai, P. R. China
E-mail: huangfq@mail.sic.ac.cn

^c Joint Key Laboratory of the Ministry of Education, Institute of Applied Physics and Materials Engineering, University of Macau, Macao, SAR, P. R. China
E-mail: shichen@um.edu.mo

^d State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry, Jilin University, Changchun, P. R. China

^e College of Energy, Soochow Institute for Energy and Materials Innovations, Jiangsu Provincial Key Laboratory for Advanced Carbon Materials and Wearable Energy Technologies, Soochow University, Suzhou, P. R. China

^f Institute of High Energy Physics, Chinese Academy of Sciences, Beijing 100049, P. R. China

^g Department of Materials and Environmental Chemistry, Stockholm University, Stockholm, Sweden

^h School of Innovation and Entrepreneurship, Southern University of Science and Technology, Shenzhen, P. R. China
E-mail: chenrx@sustech.edu.cn

ⁱ School of Materials Science and Engineering, Taizhou University, Taizhou, Zhejiang, P. R. China

Abstract

Durable and highly efficient electrocatalysts for the oxygen reduction reaction (ORR) are central to rechargeable Zn–air batteries (ZABs). The current best-performing ORR electrocatalysts are FeN₄-based powder materials among the non-noble metals, but they still suffer from peeling off and demetallation during long-term device operation. Herein, we constructed an anti-dissolving structure of dual-atomic Fe sites modified with carbon holes and pyridinic-N on carbon fiber membranes (Fe₂N₆-CMPCFs) as binder-free cathodes via two-step NH₃-assisted carbonization. Experimental and theoretical studies implied that the energy barrier of Fe dissolution is significantly higher in Fe₂N₆-CMPCFs (1.41 eV) compared to that of conventional non-defective FeN₄ (0.94 eV), which can significantly inhibit the demetallation of Fe sites during long-term electrocatalysis. Thus, the Fe₂N₆-CMPCFs-based cathode enabled ZABs to operate over 200 days (record-breaking 14 500 cycles) with a remarkable peak power density of 261.4 mW cm⁻². Furthermore, structure analysis uncovered the anti-dissolving origin of Fe sites in Fe₂N₆-CMPCFs, which can be attributed to the enhanced orbital interaction (Fe–N and Fe–Fe) and electrostatic force between the Fe and N atoms. This work provides a valuable route to design anti-dissolving atomic sites and binder-free cathodes for sustainable electronic devices.

Energy & Environmental Science

Anti-dissolving Fe₂N₆ site-based carbon fiber membranes for binder-free Zn–air batteries with a 200-day lifespan†

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