In the realm of photoenergy conversion,the scarcity of efficient light-driven semiconductors poses a significant obstacle to the advancement of photocatalysis,highlighting the critical need for researchers to explore ...In the realm of photoenergy conversion,the scarcity of efficient light-driven semiconductors poses a significant obstacle to the advancement of photocatalysis,highlighting the critical need for researchers to explore novel semiconductor materials.Herein,we present the inaugural synthesis of a novel semiconductor,CdNCN,under mild conditions,while shedding light on its formation mechanism.By effectively harnessing the[NCN]^(2⁻)moiety in the thiourea process,we successfully achieve the one-pot synthesis of CdNCN-CdS heterostructure photocatalysts.Notably,the optimal CdNCN-CdS sample demonstrates a hydrogen evolution rate of 14.7 mmol g^(-1)h^(-1)under visible light irradiation,establishing itself as the most efficient catalyst among all reported CdS-based composites without any cocatalysts.This outstanding hydrogen evolution performance of CdNCN-CdS primarily arises from two key factors:i)the establishment of an atomic-level N-Cd-S heterostructure at the interface between CdNCN and CdS,which facilitating highly efficient electron transfer;ii)the directed transfer of electrons to the(110)crystal plane of CdNCN,promoting optimal hydrogen adsorption and active participation in the hydrogen evolution reaction.This study provides a new method for synthesizing CdNCN materials and offers insights into the design and preparation of innovative atomic-level composite semiconductor photocatalysts.展开更多
基金financially supported by the National Natural Science Foundation of China(Nos.22078118,22274059 and 42277219)the Natural Science Foundation of Guangdong Province,China(Nos.2023A1515010740 and 2023A1515030131).
文摘In the realm of photoenergy conversion,the scarcity of efficient light-driven semiconductors poses a significant obstacle to the advancement of photocatalysis,highlighting the critical need for researchers to explore novel semiconductor materials.Herein,we present the inaugural synthesis of a novel semiconductor,CdNCN,under mild conditions,while shedding light on its formation mechanism.By effectively harnessing the[NCN]^(2⁻)moiety in the thiourea process,we successfully achieve the one-pot synthesis of CdNCN-CdS heterostructure photocatalysts.Notably,the optimal CdNCN-CdS sample demonstrates a hydrogen evolution rate of 14.7 mmol g^(-1)h^(-1)under visible light irradiation,establishing itself as the most efficient catalyst among all reported CdS-based composites without any cocatalysts.This outstanding hydrogen evolution performance of CdNCN-CdS primarily arises from two key factors:i)the establishment of an atomic-level N-Cd-S heterostructure at the interface between CdNCN and CdS,which facilitating highly efficient electron transfer;ii)the directed transfer of electrons to the(110)crystal plane of CdNCN,promoting optimal hydrogen adsorption and active participation in the hydrogen evolution reaction.This study provides a new method for synthesizing CdNCN materials and offers insights into the design and preparation of innovative atomic-level composite semiconductor photocatalysts.
