Achieving pH-universal oxygen electrolysis via synergistic density and coordination tuning over biomass-derived Fe single-atom catalyst

Wei Guo, Meiling Pan, Qianjie Xie, Hua Fan, Laihao Luo, Qun Jing (), Yehua Shen (), Yan Yan (), Mingkai Liu () and Zheng Wang ()
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Wei Guo: Xi’an University of Technology
Meiling Pan: Xinjiang University
Qianjie Xie: Shaanxi Institute of Medical Device Quality Inspection
Hua Fan: Xi’an University of Technology
Laihao Luo: University of Science and Technology of China
Qun Jing: Xinjiang University
Yehua Shen: Xi’an University of Technology
Yan Yan: Anhui University of Technology
Mingkai Liu: Anhui University of Technology
Zheng Wang: Xi’an Rare Metal Materials Research Institute Co.

Nature Communications, 2025, vol. 16, issue 1, 1-13

Abstract: Abstract Renewable biomass serves as a cost-effective source of carbon matrix to carry single-atom catalysts (SACs). However, the natural abundant oxygen in these materials hinders the sufficient dispersion of element with high oxygen affinity such iron (Fe). The lowered-density and oxidized SACs greatly limits their catalytic applications. Here we develop a facile continuous activation (CA) approach for synthesizing robust biomass-derived Fe-SACs. Comparing to the traditional pyrolysis method, the CA approach significantly increases the Fe loading density from 1.13 atoms nm−2 to 4.70 atoms nm−2. Simultaneously, the CA approach induces a distinct coordination tuning from dominated Fe-O to Fe-N moieties. We observe a pH-universal oxygen reduction reaction (ORR) performance over the CA-derived Fe-SACs with a half-wave potential of 0.93 V and 0.78 V vs. RHE in alkaline and acidic electrolyte, respectively. Density functional theory calculations further reveal that the increased Fe-N coordination effectively reduces the energy barriers for the ORR, thus enhancing the catalytic activity. The Fe-SACs-based zinc-air batteries show a specific capacity of 792 mA·h·gZn−1 and ultra-long life span of over 650 h at 5 mA cm−2.

Date: 2025
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DOI: 10.1038/s41467-025-58297-1

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