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<p>The transformation of noble metal nanoparticles into atomically dispersed catalysts has been a long-standing goal to enhance metal utilization and regenerate the activity of agglomerated catalysts. Traditional methods, however, often require high temperatures, specific atmospheres, or complex chemical processes. We present a novel photoinduced strategy for atomic dispersion of noble metal nanoparticles under ambient conditions. Experimental and density functional theory calculations reveal that chlorine radicals (•Cl), together with •O<sub>2</sub><sup>-</sup>, promote Pd-Pd bond cleavage. The intermediate [PdCl<sub>4</sub>]<sup>2-</sup> species formed adsorbs onto TiO<sub>2</sub> via electrostatic interactions and, upon dechlorination, stabilizes into a single-atom Pd<sub>1</sub>-N<sub>2</sub>O<sub>1</sub> structure. This method is applicable to various noble metals (Pd, Pt, Rh) and different oxide supports (TiO<sub>2</sub> and WO<sub>3</sub>), and significantly enhances the catalytic activity of both commercial Pd/C and industrial waste Pd/C catalysts by 17.8-fold and 26-fold, respectively, in the hydrogenation of styrene. This approach offers a simple, green, and sustainable solution for advancing catalytic technologies.</p>

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Photoinduced radical-mediated atomic dispersion of noble metal nanoparticles

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2026年3月14日

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  • Xiang Chen,
  • Qingfei Zhao,
  • Jingyuan Zhang,
  • Kehan Zhou,
  • Xufang Qian,
  • Zhenfeng Bian

摘要

The transformation of noble metal nanoparticles into atomically dispersed catalysts has been a long-standing goal to enhance metal utilization and regenerate the activity of agglomerated catalysts. Traditional methods, however, often require high temperatures, specific atmospheres, or complex chemical processes. We present a novel photoinduced strategy for atomic dispersion of noble metal nanoparticles under ambient conditions. Experimental and density functional theory calculations reveal that chlorine radicals (•Cl), together with •O2-, promote Pd-Pd bond cleavage. The intermediate [PdCl4]2- species formed adsorbs onto TiO2 via electrostatic interactions and, upon dechlorination, stabilizes into a single-atom Pd1-N2O1 structure. This method is applicable to various noble metals (Pd, Pt, Rh) and different oxide supports (TiO2 and WO3), and significantly enhances the catalytic activity of both commercial Pd/C and industrial waste Pd/C catalysts by 17.8-fold and 26-fold, respectively, in the hydrogenation of styrene. This approach offers a simple, green, and sustainable solution for advancing catalytic technologies.