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<p>Rational design of electrode–electrolyte interfaces is central to achieving an efficient oxygen reduction reaction (ORR) in proton-exchange membrane fuel cells. Here we demonstrate that 7-alkyltheophyllines are a group of bifunctional molecular additives capable of enhancing ORR activity on Pt(111) in the presence of strongly binding anions, for example, sulfonate in Nafion and phosphate, by enhancing intrinsic ORR kinetics and suppressing the specific adsorption of anions. Single-crystal voltammetric analysis and computational investigations reveal that the enhanced intrinsic ORR kinetics by adsorbed 7-alkyltheophyllines stems from facilitating the reduction of *O to *OH, which is a kinetically important step in the ORR on Pt surfaces. Mechanistic insights regarding the molecular additives gained on Pt(111) are shown to be valid on polycrystalline Pt. Finally, the practical relevance of this discovery is demonstrated by substantial performance enhancements in proton-exchange membrane fuel cells with Pt/C catalysts modified by 7-ethyltheophylline, highlighting the transferability of fundamental insights.</p><p></p>

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Bifunctional molecular additives enable efficient oxygen reduction reaction on platinum electrodes in the presence of strongly binding anions

  • 期刊论文

  • 发表日期：

    2026年7月2日

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  • Kaiyue Zhao,
  • Linke Fu,
  • Zelong Qiao,
  • Yuke Li,
  • Chaoran Huang,
  • Bingyuan Chen,
  • Zihan Jin,
  • Xiaoqing Cao,
  • Junrong Zheng,
  • Shaojun Guo,
  • Dapeng Cao,
  • Xiaoxia Chang,
  • Bingjun Xu

摘要

Rational design of electrode–electrolyte interfaces is central to achieving an efficient oxygen reduction reaction (ORR) in proton-exchange membrane fuel cells. Here we demonstrate that 7-alkyltheophyllines are a group of bifunctional molecular additives capable of enhancing ORR activity on Pt(111) in the presence of strongly binding anions, for example, sulfonate in Nafion and phosphate, by enhancing intrinsic ORR kinetics and suppressing the specific adsorption of anions. Single-crystal voltammetric analysis and computational investigations reveal that the enhanced intrinsic ORR kinetics by adsorbed 7-alkyltheophyllines stems from facilitating the reduction of *O to *OH, which is a kinetically important step in the ORR on Pt surfaces. Mechanistic insights regarding the molecular additives gained on Pt(111) are shown to be valid on polycrystalline Pt. Finally, the practical relevance of this discovery is demonstrated by substantial performance enhancements in proton-exchange membrane fuel cells with Pt/C catalysts modified by 7-ethyltheophylline, highlighting the transferability of fundamental insights.