As a promising route to hydrogen production,hydrolysis of ammonia borane(AB)aqueous solution requires efficient and stable catalysts.In this paper,a carbon-coated zeolite is prepared by high temperature calcination us...As a promising route to hydrogen production,hydrolysis of ammonia borane(AB)aqueous solution requires efficient and stable catalysts.In this paper,a carbon-coated zeolite is prepared by high temperature calcination using glucose as carbon source.Ultrafine Ru nanoparticles are anchored on the composite support with core-shell structure using a simple in situ reduction method.The prepared catalyst expressed outstanding catalytic activity in the hydrolytic dehydrogenation of AB.The effects of support prepared by different synthesis parameters on the performance of catalyst are investigated.The Ru/S-1@C(RSC-2)catalyst exhibited the highest catalytic activity for hydrolytic dehydrogenation of AB with a turnover frequency of 892 min^(-1)at room temperature.This performance is superior to that of many catalysts previously reported.The excellent catalytic activity is attributed to the carbon layer on catalyst surface effectively limiting the aggregation of Ru nanoparticles in the hydrolysis reaction.The zeolite also plays a role in preactivation of water.This pre-activation accelerates the ratelimiting step of water dissociation in the reaction.The kinetic studies for determining the activation energy(E_(a)=36.8 kJ·mol^(-1))were based on reaction temperature.The effects of catalyst concentration,AB concentration and NaOH concentration on hydrolysis rate of AB were further investigated.The high-performance catalysts and the preparation method in this study have wide application prospects in the field of clean energy.展开更多
基金financially supported by the National Natural Science Foundation of China(Nos.22279118,31901272,U1204203 and 21401168)the Key Projects of Shanxi Coal-based Low Carbon Joint Fund(No.U1710221)。
文摘As a promising route to hydrogen production,hydrolysis of ammonia borane(AB)aqueous solution requires efficient and stable catalysts.In this paper,a carbon-coated zeolite is prepared by high temperature calcination using glucose as carbon source.Ultrafine Ru nanoparticles are anchored on the composite support with core-shell structure using a simple in situ reduction method.The prepared catalyst expressed outstanding catalytic activity in the hydrolytic dehydrogenation of AB.The effects of support prepared by different synthesis parameters on the performance of catalyst are investigated.The Ru/S-1@C(RSC-2)catalyst exhibited the highest catalytic activity for hydrolytic dehydrogenation of AB with a turnover frequency of 892 min^(-1)at room temperature.This performance is superior to that of many catalysts previously reported.The excellent catalytic activity is attributed to the carbon layer on catalyst surface effectively limiting the aggregation of Ru nanoparticles in the hydrolysis reaction.The zeolite also plays a role in preactivation of water.This pre-activation accelerates the ratelimiting step of water dissociation in the reaction.The kinetic studies for determining the activation energy(E_(a)=36.8 kJ·mol^(-1))were based on reaction temperature.The effects of catalyst concentration,AB concentration and NaOH concentration on hydrolysis rate of AB were further investigated.The high-performance catalysts and the preparation method in this study have wide application prospects in the field of clean energy.
