Developing transition metal-nitrogen-carbon materials(M-N-C)as electrocatalysts for the oxygen evolution reaction(OER)is significant for low-cost energy conversion systems.Further d-orbital adjustment of M center in M...Developing transition metal-nitrogen-carbon materials(M-N-C)as electrocatalysts for the oxygen evolution reaction(OER)is significant for low-cost energy conversion systems.Further d-orbital adjustment of M center in M-N-C is beneficial to the improvement of OER performance.Herein,we synthesize a single-Mn-atom catalyst based on carbon skeleton(Mn_(1)-N_(2)S_(2)C_(x))with isolated Mn-N_(2)S_(2)sites,which exhibits high alkaline OER activity(η10=280 mV),low Tafel slope(44 mV·dec^(−1)),and excellent stability.Theoretical calculations reveal the pivotal function of isolated Mn-N_(2)S_(2)sites in promoting OER,including the adsorption kinetics of intermediates and activation mechanism of active sites.The doping of S causes the increase in both charge density and work function of active Mn center,and ortho-Mn_(1)-N_(2)S_(2)C_(x)expresses the fastest OER kinetics due to the asymmetric plane.展开更多
基金supported by the National Natural Science Foundation of China(No.22075099)the Natural Science Foundation of Jilin Province(No.20220101051JC)the Education Department of Jilin Province(No.JJKH20220967KJ)。
文摘Developing transition metal-nitrogen-carbon materials(M-N-C)as electrocatalysts for the oxygen evolution reaction(OER)is significant for low-cost energy conversion systems.Further d-orbital adjustment of M center in M-N-C is beneficial to the improvement of OER performance.Herein,we synthesize a single-Mn-atom catalyst based on carbon skeleton(Mn_(1)-N_(2)S_(2)C_(x))with isolated Mn-N_(2)S_(2)sites,which exhibits high alkaline OER activity(η10=280 mV),low Tafel slope(44 mV·dec^(−1)),and excellent stability.Theoretical calculations reveal the pivotal function of isolated Mn-N_(2)S_(2)sites in promoting OER,including the adsorption kinetics of intermediates and activation mechanism of active sites.The doping of S causes the increase in both charge density and work function of active Mn center,and ortho-Mn_(1)-N_(2)S_(2)C_(x)expresses the fastest OER kinetics due to the asymmetric plane.
