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<p>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<sup>−2</sup> to 4.70 atoms nm<sup>−2</sup>. 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·g<sub>Zn</sub><sup>−1</sup> and ultra-long life span of over 650 h at 5 mA&#xa0;cm<sup>−2</sup>.</p>

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

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年3月25日

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  • Wei Guo,
  • Meiling Pan,
  • Qianjie Xie,
  • Hua Fan,
  • Laihao Luo,
  • Qun Jing,
  • Yehua Shen,
  • Yan Yan,
  • Mingkai Liu,
  • Zheng Wang

摘要

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.