膨润土负载钌催化剂制备及其催化氨硼烷水解产氢研究

doi:10.19964/j.issn.1006-4990.2020-0421

Abstract

Abstract:

Ruthenium/bentonite（Ru/Ben） catalysts were prepared via an impregnation-reduction method using NaBH₄ as the reducing agent.The effects of ruthenium content,amount of reducing agent of sodium borohydride,reduction temperature and reaction conditions on the hydrolysis of ammonia borane（NH₃BH₃） catalyzed by Ru/Ben were investigated.The results showed that under the conditions of Ru loading of 0.3%（mass fraction）,the molar ratio of Ru to NaBH₄ was 1∶2.5,and the reduction temperature was 303 K,the size of Ru microcrystalline in Ru/Ben was 3.8 nm,and the conversion frequency（TOF） of Ru/Ben catalyzed hydrolysis of NH₃BH₃ was 145 mol/（mol·min）.When the stirring speed reached 450 r/min,external diffusion could be neglected,resulting in the highest reaction rate towards hydrogen generation.The rate of hydrogen production was directly proportional to the concentration of Ru/Ben.The interfacial reaction of catalyst was the decisive step in the hydrolysis of NH₃BH₃ to generate hydrogen.The order of Ru/Ben catalyzed hydrolysis of NH₃BH₃ to generate hydrogen was 0.7.The higher the reaction temperature,the higher the mass transfer rate of ammonia borane to the catalyst surface,the easier desorption of hydrogen and sodium metaborate from the catalyst surface,and the higher the hydrogen generation rate.The kinetic calculation showed that the hydrogen production rate of NH₃BH₃ hydrolysis catalyzed by Ru/Ben was independent of the concentration of aminoborane,and the activation energy was 15 kJ/mol.

Key words: Ru, bentonite, ammonia borane, hydrogen generation

CLC Number:

O643.36

Chen Lingxia,Wang Qi,Sun Haijie,Chen Zhihao,Liu Ranran. Study on preparation of bentonite supported Ru catalysts and their performance for hydrogen generation from catalytic hydrolysis of ammonia borane[J]. Inorganic Chemicals Industry, 2021, 53(6): 199-204.

Figures/Tables 7

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References 31

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催化剂	表观活化能/ （kJ·mol^-1）	催化剂	表观活化能/ （kJ·mol^-1）
Ru/g-C₃N₄^[23]	37	Ru/MIL-96^[27]	48
Ru/C^[24]	35	Ru/MIL-101^[28]	51
Ru/Graphene^[14]	12	Ru/micro HAP^[18]	58
Ru/Carbon^[15]	76	Ru/TiO₂^[29]	87
Ru/γ-Al₂O₃^[16]	67	Ru/Ce（OH）CO₃^[30]	60
Ru/Al₂O₃^[17]	48	Ru/HAP^[31]	44
Ru/MIL-41^[25]	42	Ru/Ben（本研究）	15
Ru/MIL-53^[26]	29

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Study on preparation of bentonite supported Ru catalysts and their performance for hydrogen generation from catalytic hydrolysis of ammonia borane

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