Ammonia(NH_(3))is one of the most important building blocks of the chemical industry and a promising sustainable energy carrier.Conventional production of NH_(3)via the Haber-Bosch process requires high temperature an...Ammonia(NH_(3))is one of the most important building blocks of the chemical industry and a promising sustainable energy carrier.Conventional production of NH_(3)via the Haber-Bosch process requires high temperature and high pressure,which is energy demanding and suffers safety issues.Photocatalytic nitrogen reduction reaction(NRR)is a green and sustainable route for NH_(3) production,and has been expected to be an alternative for NH_(3)production under mild conditions.However,solar-driven N_(2)activated has appeared as the bottleneck for photocatalytic NRR.In this work,we propose that single Ru atom supported by BeO monolayer is a promising photocatalytic single atom catalyst(SAC)for efficient N_(2)activation with visible illumination.The high efficiency originates from the enhanced absorption in the visible range,as well as the back-donation mechanism when N_(2)were adsorbed on the SAC.Our results show that N_(2)can be efficiently activated by the Ru/BeO SAC and be reduced to NH_(3) with extremely low limiting potential of-0.41 V.The NRR process also exhibits dominate selectivity respect to hydrogen evolution.展开更多
基金the financial support from the National Natural Science Foundation of China(NSFC,Nos.21773309,21776315)the Fundamental Research Funds for the Central Universities(Nos.19CX05001A,20CX05010A)+1 种基金Hubei University of Arts and Science(Nos.2020kypytd002,2020kypytd003)Xiangyang Science and Technology Research and Development(No.2020YL09)。
文摘Ammonia(NH_(3))is one of the most important building blocks of the chemical industry and a promising sustainable energy carrier.Conventional production of NH_(3)via the Haber-Bosch process requires high temperature and high pressure,which is energy demanding and suffers safety issues.Photocatalytic nitrogen reduction reaction(NRR)is a green and sustainable route for NH_(3) production,and has been expected to be an alternative for NH_(3)production under mild conditions.However,solar-driven N_(2)activated has appeared as the bottleneck for photocatalytic NRR.In this work,we propose that single Ru atom supported by BeO monolayer is a promising photocatalytic single atom catalyst(SAC)for efficient N_(2)activation with visible illumination.The high efficiency originates from the enhanced absorption in the visible range,as well as the back-donation mechanism when N_(2)were adsorbed on the SAC.Our results show that N_(2)can be efficiently activated by the Ru/BeO SAC and be reduced to NH_(3) with extremely low limiting potential of-0.41 V.The NRR process also exhibits dominate selectivity respect to hydrogen evolution.
