Atomic sites co-catalyst (ASC) on photocatalytic materials possesses an attractive prospect to promote charge carrier separation and tune surface reaction kinetics,yet the synthesis of earth-abundant ASC under low tem...Atomic sites co-catalyst (ASC) on photocatalytic materials possesses an attractive prospect to promote charge carrier separation and tune surface reaction kinetics,yet the synthesis of earth-abundant ASC under low temperature remains a great challenge.Here,a novel in-situ NH_(4)^(+)-etched strategy to anchor atomic Mo sites on ZnIn_(2)S_(4)hierarchical nanotubes (HNTs) with abundant mesopores under mild conditions for promoting charge carrier separation and enhancing light multi-reflections is developed for efficient photocatalytic H_(2) evolution.Density functional theory calculations and linear sweep voltammetry demonstrate that the well-defined Mo-S_(2)O_(1) sites with distinctive coordination configuration and electronic property contribute to the enhanced separation of photo-generated charge carriers and reduced Gibbs free energy for H_(2) evolution.Consequently,the well-defined MoSA-ZIS HNTs present an excellent photocatalytic activity with a rate of 29.9μmol h^(-1)(5.98 mmol g^(-1)h^(-1)),which is 7.3 times higher than that of ZnIn_(2)S_(4)nanosheets (NSs),to be among the best ZnIn_(2)S_(4)-based photocatalysts.The present strategy breaks the high-temperature limitation of conventional top-down thermal dissociation/emitting approach for anchoring non-noble metal atomic sites on catalyst support.展开更多
基金the Beijing Natural Science Foundation(JQ18005)the National Science Fund for Distinguished Young Scholars(52025133)+3 种基金the Tencent Foundation through the XPLORER PRIZEthe National Natural Science Foundation of China(22002003)China Postdoctoral Science Foundation(2019TQ0001,2020M670020)the Fund of the State Key Laboratory of Solidification Processing in Northwestern Polytechnic University(NWPU)(SKLSP202004)。
文摘Atomic sites co-catalyst (ASC) on photocatalytic materials possesses an attractive prospect to promote charge carrier separation and tune surface reaction kinetics,yet the synthesis of earth-abundant ASC under low temperature remains a great challenge.Here,a novel in-situ NH_(4)^(+)-etched strategy to anchor atomic Mo sites on ZnIn_(2)S_(4)hierarchical nanotubes (HNTs) with abundant mesopores under mild conditions for promoting charge carrier separation and enhancing light multi-reflections is developed for efficient photocatalytic H_(2) evolution.Density functional theory calculations and linear sweep voltammetry demonstrate that the well-defined Mo-S_(2)O_(1) sites with distinctive coordination configuration and electronic property contribute to the enhanced separation of photo-generated charge carriers and reduced Gibbs free energy for H_(2) evolution.Consequently,the well-defined MoSA-ZIS HNTs present an excellent photocatalytic activity with a rate of 29.9μmol h^(-1)(5.98 mmol g^(-1)h^(-1)),which is 7.3 times higher than that of ZnIn_(2)S_(4)nanosheets (NSs),to be among the best ZnIn_(2)S_(4)-based photocatalysts.The present strategy breaks the high-temperature limitation of conventional top-down thermal dissociation/emitting approach for anchoring non-noble metal atomic sites on catalyst support.
