School of Chemistry and Materials Science, University of Science and Technology of China, 230026, Hefei, China.
State Key Laboratory of Catalysis, Dalian National Laboratory for Clean Energy, iChEM (Collaborative Innovation Center of Chemistry for Energy Materials), Dalian Institute of Chemical Physics, Chinese Academy of Sciences, 116023, Dalian, China.
Angew Chem Int Ed Engl. 2023 May 15;62(21):e202302575. doi: 10.1002/anie.202302575. Epub 2023 Apr 17.
The interfacial barrier of charge transfer from semiconductors to cocatalysts means that the photogenerated charges cannot be fully utilized, especially for the challenging water oxidation reaction. Using cobalt cubane molecules (Co O ) as water oxidation cocatalysts, we rationally assembled partially oxidized graphene (pGO), acting as a charge-transfer mediator, on the hole-accumulating {-101} facets of lead chromate (PbCrO ) crystal. The assembled pGO enables preferable immobilization of Co O molecules on the {-101} facets of the PbCrO crystal, which is favorable for the photogenerated holes transferring from PbCrO to Co O molecules. The surface charge-transfer efficiency of PbCrO was boosted by selective assembly of pGO between PbCrO and Co O molecules. An apparent quantum efficiency for photocatalytic water oxidation on the Co O /pGO/PbCrO photocatalyst exceeded 10 % at 500 nm. This strategy of rationally assembling charge-transfer mediator provides a feasible method for acceleration of charge transfer and utilization in semiconductor photocatalysis.
界面电荷转移障碍意味着光生电荷不能被充分利用，特别是对于具有挑战性的水氧化反应。我们使用钴立方烷分子（Co O ）作为水氧化助催化剂，合理地将部分氧化石墨烯（pGO）组装在铅铬酸盐（PbCrO ）晶体的空穴积累 {-101} 晶面上，作为电荷转移介体。组装的 pGO 能够更好地将 Co O 分子固定在 PbCrO 晶体的 {-101} 晶面上，有利于光生空穴从 PbCrO 转移到 Co O 分子上。通过在 PbCrO 和 Co O 分子之间选择性组装 pGO，提高了 PbCrO 的表面电荷转移效率。在 Co O /pGO/PbCrO 光催化剂上，500nm 处光催化水氧化的表观量子效率超过 10%。这种合理组装电荷转移介体的策略为加速半导体光催化中的电荷转移和利用提供了一种可行的方法。
