Designing catalysts with capable dual-active sites to drive catalytic hydrogen generation is necessary for the future hydrogen economy.Herein,the interfacial active sites consisting of Co and Co-C on Co-Co_(2)C@carbon...Designing catalysts with capable dual-active sites to drive catalytic hydrogen generation is necessary for the future hydrogen economy.Herein,the interfacial active sites consisting of Co and Co-C on Co-Co_(2)C@carbon heterostructure are designed through annealing and highpressure carbonization.The operating temperature during the high-pressure carbonization under a CO-reducing environment is responsible for the construction and regulation of Co-Co_(2)C@C heterostructure.The optimal catalyst has a high turnover frequency(TOF) of33.1 min^(-1) and low activation energy(E_a) of27.3 kJ-mol^(-1) during the hydrolysis of NH_(3)BH_(3).The catalytic stability of Co-Co_(2)C@C has no dramatic deterioration even after 5 cyclic usages.The interfacial active sites and the carbon on the catalyst surface enhance hydrogen generation kinetics and catalytic stability.The construction of interfacial active sites in Co-Co_(2)C@C prompts the dissociation of reactants(NH_(3)BH_(3) and H_(2)O molecules),leading to an enhanced catalytic hydrogen generation from NH_(3)BH_(3) hydrolysis(Co activates NH_(3)BH_(3) and Co-C activates H_(2)O).The construction of hetero-structural catalysts provides theoretical direction for the rational design of advanced transition metal carbide materials in the field of energy catalysis and conversion.展开更多
基金financially supported by the National Natural Science Foundation of China (Nos.52071135, 51871090 and U1804135)the Fundamental Research Funds for the Universities of Henan Province (Nos.NSFRF220201 and NSFRF200402)。
文摘Designing catalysts with capable dual-active sites to drive catalytic hydrogen generation is necessary for the future hydrogen economy.Herein,the interfacial active sites consisting of Co and Co-C on Co-Co_(2)C@carbon heterostructure are designed through annealing and highpressure carbonization.The operating temperature during the high-pressure carbonization under a CO-reducing environment is responsible for the construction and regulation of Co-Co_(2)C@C heterostructure.The optimal catalyst has a high turnover frequency(TOF) of33.1 min^(-1) and low activation energy(E_a) of27.3 kJ-mol^(-1) during the hydrolysis of NH_(3)BH_(3).The catalytic stability of Co-Co_(2)C@C has no dramatic deterioration even after 5 cyclic usages.The interfacial active sites and the carbon on the catalyst surface enhance hydrogen generation kinetics and catalytic stability.The construction of interfacial active sites in Co-Co_(2)C@C prompts the dissociation of reactants(NH_(3)BH_(3) and H_(2)O molecules),leading to an enhanced catalytic hydrogen generation from NH_(3)BH_(3) hydrolysis(Co activates NH_(3)BH_(3) and Co-C activates H_(2)O).The construction of hetero-structural catalysts provides theoretical direction for the rational design of advanced transition metal carbide materials in the field of energy catalysis and conversion.