Electrochemical nitrogen reduction reaction(eNRR)is one of the most important chemical reactions for the production of ammonia under ambient environment.However,the lack of in-depth understanding of the structure-acti...Electrochemical nitrogen reduction reaction(eNRR)is one of the most important chemical reactions for the production of ammonia under ambient environment.However,the lack of in-depth understanding of the structure-activity relationship impedes the development of high-performance catalysts for ammonia production.Herein,the density functional theory(DFT)calculations are performed to reveal the structure–activity relationship for the single-atom catalysts(SACs)supported on g-C_(3)N_(4),which is modified by molecular groups(i.e.,H,O,and OH).The computational results demonstrate that the W-based SACs are beneficial to produce ammonia with a low limiting potential(UL).Particularly,the W-OH@g-C_(3)N_(4) catalyst exhibits an ultralow UL of−0.22 V for eNRR.And the competitive eNRR selectivity can be identified by the dominant*N2 adsorption free energy than that of*H.Our findings provide a theoretical basis for the synthesis of efficient catalysts to produce ammonia.展开更多
基金supported by the National Natural Science Foundation of China(Nos.91934302,51762005,and 21878078)Key Projects of Guangxi Natural Science Foundation(No.2020GXNSFDA297015)+1 种基金the China Postdoctoral Science Foundation(No.2020M683617XB)the Opening Project of Guangxi Key Laboratory of Petrochemical Resource Processing and Process Intensification Technology(No.2020K006)。
文摘Electrochemical nitrogen reduction reaction(eNRR)is one of the most important chemical reactions for the production of ammonia under ambient environment.However,the lack of in-depth understanding of the structure-activity relationship impedes the development of high-performance catalysts for ammonia production.Herein,the density functional theory(DFT)calculations are performed to reveal the structure–activity relationship for the single-atom catalysts(SACs)supported on g-C_(3)N_(4),which is modified by molecular groups(i.e.,H,O,and OH).The computational results demonstrate that the W-based SACs are beneficial to produce ammonia with a low limiting potential(UL).Particularly,the W-OH@g-C_(3)N_(4) catalyst exhibits an ultralow UL of−0.22 V for eNRR.And the competitive eNRR selectivity can be identified by the dominant*N2 adsorption free energy than that of*H.Our findings provide a theoretical basis for the synthesis of efficient catalysts to produce ammonia.
