Nitric oxide reduction to ammonia by electrocatalysis is the potential application in the elimination of smog and energy conversion. In this work, the feasibility of the application of two-dimensional metal borides(MB...Nitric oxide reduction to ammonia by electrocatalysis is the potential application in the elimination of smog and energy conversion. In this work, the feasibility of the application of two-dimensional metal borides(MBenes) in nitric oxide electroreduction reaction(NOER) was investigated through density functional theory calculations. Including the geometry and electronic structure of five kinds of MBenes, the adsorption of NO on the surface of these substrates, the selective adsorption of hydrogen protons during the hydrogenation process, and the overpotential in the electrocatalytic ammonia synthesis process. As a result, Mn B exhibited the most favorable catalytic performance according to the associative pathways,which is thermodynamically performed spontaneously, and WB has a minimum overpotential of 0.37 V vs. RHE in the process of ammonia production according to the dissociative pathway. Overall, our work is the first to explore the electrocatalytic NO through the dissociative mechanism to synthesize ammonia in-depth and proves that MBenes are efficient NO electrocatalytic ammonia synthesis catalysts. These research results provide a new direction for the development of electrocatalytic ammonia synthesis experimentally and theoretically.展开更多
The electrochemical NO reduction(NOER)is one of the most promising routes for ammonia synthesis and for simultaneously removing the air pollutant,NO.However,the current electro-catalysts are mainly metal based,and the...The electrochemical NO reduction(NOER)is one of the most promising routes for ammonia synthesis and for simultaneously removing the air pollutant,NO.However,the current electro-catalysts are mainly metal based,and the search for new and cost-efficient NOER catalysts is in the pipeline.Polyoxometalates,a class of metal–oxide clusters,exhibiting unique electrochemical redox behavior,have been widely applied to many electrocatalytic processes.展开更多
基金funded by the Natural Science Foundation of China (No.21603109)the Henan Joint Fund of the National Natural Science Foundation of China (No.U1404216)+1 种基金the Special Fund of Tianshui Normal University,China (No.CXJ2020-08)the Scientific Research Program Funded by Shaanxi Provincial Education Department (No.20JK0676)。
文摘Nitric oxide reduction to ammonia by electrocatalysis is the potential application in the elimination of smog and energy conversion. In this work, the feasibility of the application of two-dimensional metal borides(MBenes) in nitric oxide electroreduction reaction(NOER) was investigated through density functional theory calculations. Including the geometry and electronic structure of five kinds of MBenes, the adsorption of NO on the surface of these substrates, the selective adsorption of hydrogen protons during the hydrogenation process, and the overpotential in the electrocatalytic ammonia synthesis process. As a result, Mn B exhibited the most favorable catalytic performance according to the associative pathways,which is thermodynamically performed spontaneously, and WB has a minimum overpotential of 0.37 V vs. RHE in the process of ammonia production according to the dissociative pathway. Overall, our work is the first to explore the electrocatalytic NO through the dissociative mechanism to synthesize ammonia in-depth and proves that MBenes are efficient NO electrocatalytic ammonia synthesis catalysts. These research results provide a new direction for the development of electrocatalytic ammonia synthesis experimentally and theoretically.
基金financially supported by the National Natural Science Foundation of China(grant no.21771033,21671036,and 21901035)the Fundamental Research Funds for the Central Universities(grant no.2412018BJ001,2412018ZD007,and 2412018QD005)+5 种基金the China Postdoctoral Science Foundation funded project(grant no.2018M631849)the Foundation of Jilin Educational Committee(grant no.JJKH20190268KJ)the Scientific Development Project of Jilin Province(grant no.20190201206JC)the Shenzhen Nobel Prize Scientists Laboratory Project(grant no.C17783101)Start-up Fund From SUSTech(grant no.Y01216127 and Y01216227)The computational work was carried out at the LvLiang Cloud Computing Center of China,and the calculations were performed on TianHe-2.
文摘The electrochemical NO reduction(NOER)is one of the most promising routes for ammonia synthesis and for simultaneously removing the air pollutant,NO.However,the current electro-catalysts are mainly metal based,and the search for new and cost-efficient NOER catalysts is in the pipeline.Polyoxometalates,a class of metal–oxide clusters,exhibiting unique electrochemical redox behavior,have been widely applied to many electrocatalytic processes.
