4.8 Article

Coordinatively unsaturated atomically dispersed Pt+2-N4 sites on hexagonal nanosheet structure of g-C3N4 for high-performance photocatalytic H2 production

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APPLIED CATALYSIS B-ENVIRONMENTAL
卷 337, 期 -, 页码 -

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ELSEVIER
DOI: 10.1016/j.apcatb.2023.122959

关键词

Single atom catalysis; Electronic metal -support interactions; Local coordination environment; Photocatalytic hydrogen production

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This paper reports the formation of coordinatively unsaturated atomically dispersed Pt+2 sites on hexagonal nanosheets of g-C3N4. The structure with a Pt loading of 0.38 wt% exhibited a superb photocatalytic hydrogen evolution rate of 2900 μmol g-1 h-1, which was 5.6 times higher than that of the reactive Pt1 sites on bulk. Advanced spectroscopic analysis and DFT calculations revealed the strong electronic metal-support interactions between Pt1 and HCN, which effectively reduced the adsorbed Pt+4 sites into Pt+2 and created favorable uniform Pt+2-N4 moieties at low Pt loading for water adsorption, dissociation, and H2 evolution.
Developing active and stable metal single-atom catalysts is technically challenging. The electronic interactions between the metal site and its supports play a key role in altering electronic properties for the creation of more reactive and stable centers. The local environment of a single-atom catalyst directly affects its stability and reactivity. Herein, we describe the formation of coordinatively unsaturated atomically dispersed Pt+2 sites (Pt+2N4) on hexagonal nanosheets of g-C3N4 (Pt1-HCN). This structure with Pt loading of 0.38 wt% exhibited a superb photocatalytic hydrogen evolution rate of 2900 & mu;mol g-1 h-1 which was 5.6 times higher than that of the reactive Pt1 sites (Pt+4-N5) on bulk (Pt1-BCN). The comprehensive advance spectroscopic analysis combined with DFT calculations revealed that the strong electronic metal-support interactions between Pt1 and HCN effectively reduced the adsorbed Pt+4 sites into Pt+2 and create favorable uniform Pt+2-N4 moieties at low Pt loading for water adsorption, dissociation, and H2 evolution.

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