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<p>Compared to other reactive oxygen species, singlet oxygen (<sup>1</sup>O<sub>2</sub>) exhibits unique advantages, including high selectivity and strong oxidative capacity, for the targeted oxidation of pollutants. However, its production is often limited by the narrow spectral response and low intersystem crossing efficiency of conventional photocatalysts. In this study, we constructed a composite photocatalytic system based on metal–organic frameworks (MOFs) loaded with gold nanoparticles (Au NPs) to elucidate the enhancement mechanism by which singlet oxygen generation is enhanced through synergistic modulation of localized surface plasmon resonance (LSPR) and excitonic states. The introduction of Au NPs significantly enhanced the LSPR absorption of the material, effectively promoting the conversion of excitons from singlet-to-triplet states. This was achieved by lowering the energy barrier for singlet-to-triplet conversion (<i>Δ</i><sub>EST</sub> decreased from 0.172&#xa0;eV to 0.162&#xa0;eV), thereby accelerating the intersystem crossing process and improving <sup>1</sup>O₂ generation efficiency, consequently, the system enabled efficient removal of <i>p</i>-chlorophenol. This work proposes a novel “LSPR–exciton regulation–photothermal synergy” mechanism, offering new strategies for the rational design of high-activity photosensitizers and targeted pollutant oxidation.</p>

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Enhanced singlet oxygen generation over Au modified Zr-MOF photocatalyst for efficient photocatalytic degradation of organic pollutants

  • 期刊论文

  • 发表日期：

    2025年10月30日

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  • Xin Jiang,
  • Aiyu Yang,
  • Lei Tang,
  • Caixia Zhong,
  • Zhenxing Zeng

摘要

Compared to other reactive oxygen species, singlet oxygen (1O2) exhibits unique advantages, including high selectivity and strong oxidative capacity, for the targeted oxidation of pollutants. However, its production is often limited by the narrow spectral response and low intersystem crossing efficiency of conventional photocatalysts. In this study, we constructed a composite photocatalytic system based on metal–organic frameworks (MOFs) loaded with gold nanoparticles (Au NPs) to elucidate the enhancement mechanism by which singlet oxygen generation is enhanced through synergistic modulation of localized surface plasmon resonance (LSPR) and excitonic states. The introduction of Au NPs significantly enhanced the LSPR absorption of the material, effectively promoting the conversion of excitons from singlet-to-triplet states. This was achieved by lowering the energy barrier for singlet-to-triplet conversion (ΔEST decreased from 0.172 eV to 0.162 eV), thereby accelerating the intersystem crossing process and improving 1O₂ generation efficiency, consequently, the system enabled efficient removal of p-chlorophenol. This work proposes a novel “LSPR–exciton regulation–photothermal synergy” mechanism, offering new strategies for the rational design of high-activity photosensitizers and targeted pollutant oxidation.