A pH-universal ORR catalyst with single-atom iron sites derived from a double-layer MOF for superior flexible quasi-solid-state rechargeable Zn–air batteries

Abstract

Developing a highly efficient, easy-to-fabricate and non-noble metal electrocatalyst is vital for the oxygen reduction reaction (ORR). Herein, we fabricate a single Fe site catalyst Fe1/d-CN by developing a double-layer MOF strategy. The Fe1/d-CN catalyst shows an excellent ORR activity in the pH-universal range, especially in alkaline electrolytes with a record-level half-wave potential of 0.950 V, exceeding those of almost all the reported non-noble electrocatalysts and the commercial Pt/C catalyst (0.863 V). Besides its exceptional ORR activity in alkaline electrolytes, it also exhibits comparable ORR activity to the commercial Pt/C catalyst in acidic and neutral electrolytes. We speculate that the sources of the excellent pH-universal ORR performance can be attributed to the regulation of the electronic structure of Fe centres and the excellent electron/proton transport capability that comes from the rich defects and hierarchical porous features of the Fe1/d-CN catalyst. More excitingly, the catalyst possesses remarkable durability, and exhibits a negligible decrease after 30k accelerated durability test (ADT) cycles in pH-universal media. The flexible quasi-solid-state alkaline rechargeable Zn–air batteries with the Fe1/d-CN catalyst as the cathode show superior performance such as a high OCV of 1.50 V and peak power density of 78.0 mW cm−2. Furthermore, the flexible quasi-solid-state neutral rechargeable Zn–air batteries also exhibited remarkable performance.

Graphical abstract: A pH-universal ORR catalyst with single-atom iron sites derived from a double-layer MOF for superior flexible quasi-solid-state rechargeable Zn–air batteries

Supplementary files

Article information

Article type
Paper
Submitted
26 May 2021
Accepted
15 Oct 2021
First published
15 Oct 2021

Energy Environ. Sci., 2021, Advance Article

A pH-universal ORR catalyst with single-atom iron sites derived from a double-layer MOF for superior flexible quasi-solid-state rechargeable Zn–air batteries

M. Zhao, H. Liu, H. Zhang, W. Chen, H. Sun, Z. Wang, B. Zhang, L. Song, Y. Yang, C. Ma, Y. Han and W. Huang, Energy Environ. Sci., 2021, Advance Article , DOI: 10.1039/D1EE01602D

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