Ammonia borane(NHsBH3,AB)is an ideal raw material of hydrogen production with higher hydrogen storage capacity.In this paper,the catalytic processes of AB dehydrogenation were described from different ways,including t...Ammonia borane(NHsBH3,AB)is an ideal raw material of hydrogen production with higher hydrogen storage capacity.In this paper,the catalytic processes of AB dehydrogenation were described from different ways,including thermal dehydrogenation,hydrolysis,methanolysis,photocatalysis and photopiezoelectric synergy catalysis with experimental research and theoretical calculations.Catalyst models include bulk materials,two-dimensional materials,nanocluster particles and single/diatomic structures.Among them,the proportion of H2 released is different,and the reaction conditions are also different,which are suitable for different application scenarios.Through this review,we could have a preliminary comprehensive understanding of AB dehydrogenation reaction.展开更多
In this paper,Fe_(36)Co_(44)nanocluster structure is used to catalyze the hydrolysis reaction of ammonia borane to produce H_(2).Firstly,we complete the construction of Fe_(36)Co_(44)cluster structure and calculate th...In this paper,Fe_(36)Co_(44)nanocluster structure is used to catalyze the hydrolysis reaction of ammonia borane to produce H_(2).Firstly,we complete the construction of Fe_(36)Co_(44)cluster structure and calculate the electronic properties of the cluster.By comparing the adsorption process of Ammonia Borane (AB) in active sites of the cluster,which have different Effective Coordination Number (ECN),the qualitative relationship between ECN and the catalytic activation of AB is clarified,and the optimal catalytic active site is obtained.Then,from the perspective of different reaction paths,we study the hydrolysis reaction of AB in multiple paths,and obtain 5 different reaction paths and energy profiles.The calculation results show that in the case of N–H bond priority break (path 5),the reaction has the minimum rate-determining step (RDS) barrier (about 1.02 e V) and the entire reaction is exothermic (about 0.40 e V).So,path 5 is an optimal catalytic reaction path.This study will have an important guiding significance for the study of the AB hydrolysis reaction mechanism.展开更多
基金funded by the Natural Science Basic Research Program of Shaanxi(Nos.2022JQ-108 and 2022JQ-096)the National Natural Science Foundation of China(No.22104079).
文摘Ammonia borane(NHsBH3,AB)is an ideal raw material of hydrogen production with higher hydrogen storage capacity.In this paper,the catalytic processes of AB dehydrogenation were described from different ways,including thermal dehydrogenation,hydrolysis,methanolysis,photocatalysis and photopiezoelectric synergy catalysis with experimental research and theoretical calculations.Catalyst models include bulk materials,two-dimensional materials,nanocluster particles and single/diatomic structures.Among them,the proportion of H2 released is different,and the reaction conditions are also different,which are suitable for different application scenarios.Through this review,we could have a preliminary comprehensive understanding of AB dehydrogenation reaction.
基金funded by the Scientific Research Program Funded by Shaanxi Provincial Education Department (No. 20JK0676)the National Supercomputing Center in Zhengzhoupartially supported by the postgraduate research opportunities program of HZWTECH (No. HZWTECH-PROP)。
文摘In this paper,Fe_(36)Co_(44)nanocluster structure is used to catalyze the hydrolysis reaction of ammonia borane to produce H_(2).Firstly,we complete the construction of Fe_(36)Co_(44)cluster structure and calculate the electronic properties of the cluster.By comparing the adsorption process of Ammonia Borane (AB) in active sites of the cluster,which have different Effective Coordination Number (ECN),the qualitative relationship between ECN and the catalytic activation of AB is clarified,and the optimal catalytic active site is obtained.Then,from the perspective of different reaction paths,we study the hydrolysis reaction of AB in multiple paths,and obtain 5 different reaction paths and energy profiles.The calculation results show that in the case of N–H bond priority break (path 5),the reaction has the minimum rate-determining step (RDS) barrier (about 1.02 e V) and the entire reaction is exothermic (about 0.40 e V).So,path 5 is an optimal catalytic reaction path.This study will have an important guiding significance for the study of the AB hydrolysis reaction mechanism.
