Photochemical tuning of dynamic defects for high-performance atomically dispersed catalysts.

Developing active and stable atomically dispersed catalysts is challenging because of weak non-specific interactions between catalytically active metal atoms and supports. Here we demonstrate a general method for synthesizing atomically dispersed catalysts via photochemical defect tuning for controlling oxygen-vacancy dynamics, which can induce specific metal-support interactions. The developed synthesis method offers metal-dynamically stabilized atomic catalysts, and it can be applied to reducible metal oxides, including TiO 2 , ZnO and CeO 2 , containing various catalytically active transition metals, including Pt, Ir and Cu. The optimized Pt-DSA/TiO 2 shows unprecedentedly high photocatalytic hydrogen evolution activity, producing 164 mmol g -1  h -1 with a turnover frequency of 1.27 s -1 . Furthermore, it generates 42.2 mmol g sub -1 of hydrogen via a non-recyclable-plastic-photoreforming process, achieving a total conversion of 98%; this offers a promising solution for mitigating plastic waste and simultaneously producing valuable energy sources.