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Criteria for Efficient Photocatalytic Water Splitting Revealed by Studying Carrier Dynamics in a Model Al‐doped SrTiO<sub>3</sub> Photocatalyst

Ronghua Li, Tsuyoshi Takata, Beibei Zhang, Chao Feng, Qianbao Wu, Chunhua Cui, Zemin Zhang, Kazunari Domen, Yanbo Li

2023Angewandte Chemie International Edition109 citationsDOI

Abstract

Abstract Overall water splitting (OWS) using semiconductor photocatalysts is a promising method for solar fuel production. Achieving a high quantum efficiency is one of the most important prerequisites for photocatalysts to realize high solar‐to‐fuel efficiency. In a recent study ( Nature 2020 , 58 , 411–414), a quantum efficiency of almost 100 % has been achieved in an aluminum‐doped strontium titanate (SrTiO 3 : Al) photocatalyst. Herein, using the SrTiO 3 : Al as a model photocatalyst, we reveal the criteria for efficient photocatalytic water splitting by investigating the carrier dynamics through a comprehensive photoluminescence study. It is found that the Al doping suppresses the generation of Ti 3+ recombination centers in SrTiO 3 , the surface band bending facilitates charge separation, and the in situ photo‐deposited Rh/Cr 2 O 3 and CoOOH co‐catalysts render efficient charge extraction. By suppressing photocarrier recombination and establishing a facile charge separation and extraction mechanism, high quantum efficiency can be achieved even on photocatalysts with a very short (sub‐ns) intrinsic photocarrier lifetime, challenging the belief that a long carrier lifetime is a fundamental requirement. Our findings could provide guidance on the design of OWS photocatalysts toward more efficient solar‐to‐fuel conversion.

Topics & Concepts

PhotocatalysisMaterials scienceDopingQuantum efficiencyCharge carrierPhotoluminescenceSemiconductorOptoelectronicsWater splittingStrontium titanatePhotocatalytic water splittingBand bendingNanotechnologyChemical engineeringCatalysisChemistryThin filmEngineeringBiochemistryAdvanced Photocatalysis TechniquesElectronic and Structural Properties of OxidesPerovskite Materials and Applications