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<p>Perchlorate (ClO<sub>4</sub><sup>−</sup>) contamination in water poses global health risks, yet its efficient reduction to harmless Cl<sup>−</sup> under mild conditions remains challenging. Here, we report a donor−acceptor catalytic system comprising defective MoS<sub>2</sub> on N-doped carbon (MoS<sub>2</sub>−NC) coupled with zerovalent iron (Fe<sup>0</sup>), which enables rapid ClO<sub>4</sub><sup>−</sup> reduction at near-neutral pH (rate constant, 2.36 h<sup>−1</sup>), yielding Cl<sup>−</sup> as the sole product. In the MoS<sub>2</sub>−NC/Fe<sup>0</sup> system, Fe<sup>0</sup> acts as the electron donor, while undercoordinated Mo atoms in defective MoS<sub>2</sub> serve as the active sites, and N-doped carbon mediates electron transfer and optimizes the electronic environment for ClO<sub>4</sub><sup>−</sup> reduction. The reduction proceeds via oxygen atom transfer, involving Cl−O bond cleavage, O binding to Mo sites, and hydrodeoxygenation of the Mo-bound O atoms. Our observations offer a practical strategy for ClO<sub>4</sub><sup>−</sup> reduction without harsh conditions or noble metals and underscore the promise of donor−acceptor-based, defect-engineered catalysts for reductive transformation of challenging oxyanions.</p>

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Donor−acceptor catalysis with defective MoS2 and Fe0 breaks barriers to perchlorate reduction under mild conditions

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2026年5月20日

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  • Hejie Qin,
  • Han Yang,
  • Zhenmin Zhang,
  • Yiran Feng,
  • Yuankui Sun,
  • Peng Fan,
  • Zhimin Ao,
  • T. David Waite,
  • Xiaohong Guan

摘要

Perchlorate (ClO4−) contamination in water poses global health risks, yet its efficient reduction to harmless Cl− under mild conditions remains challenging. Here, we report a donor−acceptor catalytic system comprising defective MoS2 on N-doped carbon (MoS2−NC) coupled with zerovalent iron (Fe0), which enables rapid ClO4− reduction at near-neutral pH (rate constant, 2.36 h−1), yielding Cl− as the sole product. In the MoS2−NC/Fe0 system, Fe0 acts as the electron donor, while undercoordinated Mo atoms in defective MoS2 serve as the active sites, and N-doped carbon mediates electron transfer and optimizes the electronic environment for ClO4− reduction. The reduction proceeds via oxygen atom transfer, involving Cl−O bond cleavage, O binding to Mo sites, and hydrodeoxygenation of the Mo-bound O atoms. Our observations offer a practical strategy for ClO4− reduction without harsh conditions or noble metals and underscore the promise of donor−acceptor-based, defect-engineered catalysts for reductive transformation of challenging oxyanions.