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<p>Electrocatalytic oxygen reduction is an attractive alternative for sustainable H<sub>2</sub>O<sub>2</sub> production. However, the electrocatalyst still suffers from low H<sub>2</sub>O<sub>2</sub> efficiency due to unsuitable intermediate binding, sluggish active hydrogen (*H) generation in neutral/alkaline solutions and high interfacial proton concentration in acid. Meanwhile, the modulation mechanism remains insufficiently understood. Here we report efficient pH-universal H<sub>2</sub>O<sub>2</sub> electrosynthesis at ampere-level current densities by modulating interfacial microenvironment via sulfonic acid (SO<sub>3</sub>H)-functionalization of carbon nanotubes (SCNT). Experimental and theoretical results show that SO<sub>3</sub>H-functionalization accelerates *H generation from water dissociation for neutral/alkaline H<sub>2</sub>O<sub>2</sub> electrosynthesis while creating more alkaline microenvironment in acid. Moreover, it not only optimizes *OOH binding energy and facilitates *OOH generation, but also reduces the energy barrier for *HOOH desorption (rate-determining step). It exhibits good H<sub>2</sub>O<sub>2</sub> electrosynthesis performance with Faradaic efficiencies of 81.7–97.2% and H<sub>2</sub>O<sub>2</sub> concentrations of 834–1537 mM (0.8 min) at pH 0.7–13 and 1.0–1.5 A cm<sup>−2</sup>. The estimated cost for H<sub>2</sub>O<sub>2</sub> electrosynthesis is 28.5% of industrial anthraquinone process. The on-site application of SCNT has been demonstrated by efficient pollutant degradation and sterilization.</p>

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Regulating active hydrogen supply and intermediate binding for pH-universal H2O2 electrosynthesis at ampere-level current density

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年11月28日

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  • Yueling Yu,
  • Xinfei Fan,
  • Bing Shan,
  • Genwang Zhu,
  • Yuanlu Xu,
  • Yanming Liu,
  • Xie Quan

摘要

Electrocatalytic oxygen reduction is an attractive alternative for sustainable H2O2 production. However, the electrocatalyst still suffers from low H2O2 efficiency due to unsuitable intermediate binding, sluggish active hydrogen (*H) generation in neutral/alkaline solutions and high interfacial proton concentration in acid. Meanwhile, the modulation mechanism remains insufficiently understood. Here we report efficient pH-universal H2O2 electrosynthesis at ampere-level current densities by modulating interfacial microenvironment via sulfonic acid (SO3H)-functionalization of carbon nanotubes (SCNT). Experimental and theoretical results show that SO3H-functionalization accelerates *H generation from water dissociation for neutral/alkaline H2O2 electrosynthesis while creating more alkaline microenvironment in acid. Moreover, it not only optimizes *OOH binding energy and facilitates *OOH generation, but also reduces the energy barrier for *HOOH desorption (rate-determining step). It exhibits good H2O2 electrosynthesis performance with Faradaic efficiencies of 81.7–97.2% and H2O2 concentrations of 834–1537 mM (0.8 min) at pH 0.7–13 and 1.0–1.5 A cm−2. The estimated cost for H2O2 electrosynthesis is 28.5% of industrial anthraquinone process. The on-site application of SCNT has been demonstrated by efficient pollutant degradation and sterilization.