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<p>Despite that enhancing site utilization (<i>U</i><sub>site</sub>) of single atoms (SAs) is crucial in electrocatalysis beyond increasing intrinsic activity and site density, numerous SAs are inaccessible during reaction due to the dense micropores and disordered stacking of carbon particles. Here, the enhancement for <i>U</i><sub>site</sub> of SAs is achieved through a surfactant-assis'ted freeze-casting (SAFC) strategy. The sodium dodecyl sulfate (SDS)-modified Fe-doped zeolitic imidazolate framework-8 (Fe/ZIF-8) particles assemble into single-layer two-dimensional (2D) superstructures along the ice-crystal. During pyrolysis, the dual-stress effect derived from SDS shell and tight alignment of particles induces Fe/ZIF-8 to transform into concave and mesopore-rich carbon. 2D FeNC with optimized structures at both macro- and micro-scales exhibits enhanced electron/mass transport capabilities, achieving near-100% <i>U</i><sub>site</sub> of SAs and a half-wave potential of 0.958 V for oxygen reduction in alkali. This SAFC strategy demonstrates its universality in improving the catalytic performance of various 2D MNCs across different electrocatalytic reactions.</p>

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Near-100% site utilization of single atoms for efficient electrocatalysis

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2026年1月20日

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  • Xiaoqian Wei,
  • Meng An,
  • Xiannong Tang,
  • Jiamin Wei,
  • Peng Yan,
  • Yiwei Qiu,
  • Dong Jiang,
  • Yusuke Asakura,
  • Xiaokai Song,
  • Tour Asahi,
  • Chengzhou Zhu,
  • Yusuke Yamauchi

摘要

Despite that enhancing site utilization (Usite) of single atoms (SAs) is crucial in electrocatalysis beyond increasing intrinsic activity and site density, numerous SAs are inaccessible during reaction due to the dense micropores and disordered stacking of carbon particles. Here, the enhancement for Usite of SAs is achieved through a surfactant-assis'ted freeze-casting (SAFC) strategy. The sodium dodecyl sulfate (SDS)-modified Fe-doped zeolitic imidazolate framework-8 (Fe/ZIF-8) particles assemble into single-layer two-dimensional (2D) superstructures along the ice-crystal. During pyrolysis, the dual-stress effect derived from SDS shell and tight alignment of particles induces Fe/ZIF-8 to transform into concave and mesopore-rich carbon. 2D FeNC with optimized structures at both macro- and micro-scales exhibits enhanced electron/mass transport capabilities, achieving near-100% Usite of SAs and a half-wave potential of 0.958 V for oxygen reduction in alkali. This SAFC strategy demonstrates its universality in improving the catalytic performance of various 2D MNCs across different electrocatalytic reactions.