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<p>Natural biomass-derived carbon material is one promising alternative to traditional graphene-based catalyst for oxygen electrocatalysis. However, their electrocatalytic performance were constrained by the limited modulating strategy. Herein, using N-doped commercial coconut shell-derived activated carbon (AC) as catalyst model, the controllably enhanced <i>sp</i><sup>2</sup>-C domains, through an flash Joule heating process, effectively improve the edge defect density and overall graphitization degree of AC catalyst, which tunes the electronic structure of N configurations and accelerates electron transfer, leading to excellent oxygen reduction reaction performance (half-wave potential of 0.884 V<sub>RHE</sub>, equivalent to commercial 20% Pt/C, with a higher kinetic current density of 5.88&#xa0;mA&#xa0;cm<sup>−2</sup>) and oxygen evolution reaction activity (overpotential of 295&#xa0;mV at 10&#xa0;mA cm<sup>2</sup>). In a Zn-air battery, the catalyst shows outstanding cycle stability (over 1200&#xa0;h) and a peak power density of 121 mW cm<sup>−2</sup>, surpassing commercial Pt/C and RuO<sub>2</sub> catalysts. Density functional theory simulation reveals that the enhanced catalytic activity arises from the axial regulation of local <i>sp</i><sup>2</sup>-C domains. This work establishes a robust strategy for <i>sp</i><sup>2</sup>-C domain modulation, offering broad applicability in natural biomass-based carbon catalysts for electrocatalysis.</p>

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Joule Heating-Driven sp2-C Domains Modulation in Biomass Carbon for High-Performance Bifunctional Oxygen Electrocatalysis

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年4月18日

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  • Jiawei He,
  • Yuying Zhao,
  • Yang Li,
  • Qixin Yuan,
  • Yuhan Wu,
  • Kui Wang,
  • Kang Sun,
  • Jingjie Wu,
  • Jianchun Jiang,
  • Baohua Zhang,
  • Liang Wang,
  • Mengmeng Fan

摘要

Natural biomass-derived carbon material is one promising alternative to traditional graphene-based catalyst for oxygen electrocatalysis. However, their electrocatalytic performance were constrained by the limited modulating strategy. Herein, using N-doped commercial coconut shell-derived activated carbon (AC) as catalyst model, the controllably enhanced sp2-C domains, through an flash Joule heating process, effectively improve the edge defect density and overall graphitization degree of AC catalyst, which tunes the electronic structure of N configurations and accelerates electron transfer, leading to excellent oxygen reduction reaction performance (half-wave potential of 0.884 VRHE, equivalent to commercial 20% Pt/C, with a higher kinetic current density of 5.88 mA cm−2) and oxygen evolution reaction activity (overpotential of 295 mV at 10 mA cm2). In a Zn-air battery, the catalyst shows outstanding cycle stability (over 1200 h) and a peak power density of 121 mW cm−2, surpassing commercial Pt/C and RuO2 catalysts. Density functional theory simulation reveals that the enhanced catalytic activity arises from the axial regulation of local sp2-C domains. This work establishes a robust strategy for sp2-C domain modulation, offering broad applicability in natural biomass-based carbon catalysts for electrocatalysis.