摘要
Perovskite BaTaO_(2) N(BTON) is one of the most promising photocatalysts for solar water splitting due to its wide visible-light absorption and suitable conduction/valence bands,but it still confronts the challenge of high defect density causing decreased charge separation as well as photocatalytic activity.In this work,we develop a simple zinc doping strategy to greatly suppress its defect density and promote its water reduction performance.It is found that the defect formation on the nitrided Ba(Zn_(1/3-x)Ta_(2/3))O_(3-y)N_z(denoted as BZTON hereafter) will be greatly inhibited when the Zn-doped Ba(Zn_(1/3)Ta_(2/3))O_(3)(BZTO) oxide is used as the nitridation precursor.The structural characterizations and discussion demonstrate that the effective inhibition of Ta^(5+)into Ta^(4+)defects in BZTON mainly results from the easy reduction of zinc ions into metal and further the evaporation of zinc metal under the thermal ammonia flow.Interestingly,this simply doping methodology can be easily extended into the synthesis of SrTaO_(2) N(STON) with extremely low defect density,demonstrating its generality.Benefiting from the successful control to the defect density,the as-obtained BZTON photocatalyst exhibits remarkably promoted charge separation as well as water reduction activity to produce hydrogen with respect to the pristine BTON.Our work may provide an alternative avenue to prepare oxynitride semiconductors with reduced defect density for promoted solar energy conversion.
基金
supported by the National Natural Science Foundation of China (21633009, 21925206)
the National Key R&D Program of China (2020YFA0406102)
the Dalian National Laboratory for Clean Energy (DNL) Cooperation Fund,Chinese Academy of Sciences (DNL 201913)
the International Partnership Program of Chinese Academy of Sciences (121421KYSB20190025)
the DICP foundation of innovative research (DICP I201927)。
