期刊
RARE METALS
卷 42, 期 6, 页码 1935-1945出版社
NONFERROUS METALS SOC CHINA
DOI: 10.1007/s12598-022-02224-6
关键词
Interfacial active sites; Bimolecular activation; Heterostructure; Hydrogen generation; Catalytic mechanism
Design catalysts with interfacial active sites consisting of Co and Co-C on Co-Co2C@carbon heterostructure, which are designed through annealing and high-pressure carbonization, for efficient catalytic hydrogen generation. The operating temperature during the high-pressure carbonization is responsible for the construction and regulation of the Co-Co2C@C heterostructure. The optimal catalyst exhibits high turnover frequency and low activation energy during the hydrolysis of NH3BH3.
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-Co2C@carbon heterostructure are designed through annealing and high-pressure carbonization. The operating temperature during the high-pressure carbonization under a CO-reducing environment is responsible for the construction and regulation of Co-Co2C@C heterostructure. The optimal catalyst has a high turnover frequency (TOF) of 33.1 min(-1) and low activation energy (E-a) of 27.3 kJ center dot mol(-1) during the hydrolysis of NH3BH3. The catalytic stability of Co-Co2C@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-Co2C@C prompts the dissociation of reactants (NH3BH3 and H2O molecules), leading to an enhanced catalytic hydrogen generation from NH3BH3 hydrolysis (Co activates NH3BH3 and Co-C activates H2O). 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.
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