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Pt-Cu Interaction Induced Construction of Single Pt Sites for Synchronous Electron Capture and Transfer in Photocatalysis

机译：Pt-Cu Interaction Induced Construction of Single Pt Sites for Synchronous Electron Capture and Transfer in Photocatalysis

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摘要

Single-atom photocatalysts have shown their fascinating strengths in enhancing charge transfer dynamics; however, rationally designing coordination sites by metal doping to stabilize isolated atoms is still challenging. Here, a one-unit-cell ZnIn2S4 (ZIS) nanosheet with abundant Cu dopants serving as the suitable support to achieve a single atom Pt catalyst (Pt-1/Cu-ZIS) is reported, and hence the metal single atom-metal dopant interaction at an atomic level is disclosed. Experimental results and density functional theory calculations highlight the unique stabilizing effect (Pt-Cu interaction) of single Pt atoms in Cu-doped ZIS, while apparent Pt clusters are observed in pristine ZIS. Specifically, Pt-Cu interaction provides an extra coordination site except three S sites on the surface, which induces a higher diffusion barrier and makes the single atom more stable on the surface. Apart from stabilizing Pt single atoms, Pt-Cu interaction also serves as the efficient channel to transfer electrons from Cu trap states to Pt active sites, thereby enhancing the charge separation and transfer efficiency. Remarkably, the Pt-1/Cu-ZIS exhibits a superb activity, giving a photocatalytic hydrogen evolution rate of 5.02 mmol g(-1) h(-1), nearly 49 times higher than that of pristine ZIS.

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