二氧化硅负载钌催化剂催化氨硼烷水解产氢研究
收稿日期: 2019-11-24
网络出版日期: 2020-05-21
基金资助
国家级大学生创新创业训练计划项目(201912949002);河南省科技攻关项目(192102210139);河南省高等学校青年骨干教师培养计划(2019GGJS252);河南省高等学校重点科研项目(18A150018);郑州师范学院环境催化科研创新团队(702010);郑州师范学院大学生创新实验计划项目(DCZ2018022)
Research on Ru/SiO2 catalysts for hydrogen generation from catalytic hydrolysis of ammonia borane
Received date: 2019-11-24
Online published: 2020-05-21
采用浸渍-还原法制备了Ru/SiO2催化剂,并考察了钌负载量、还原剂硼氢化钠的用量、还原温度以及反应条件对催化剂Ru/SiO2催化BH3NH3水解产氢的影响。结果表明,在钌的负载量为0.1%(质量分数)、还原剂硼氢化钠与钌的物质的量比为2.2∶1、还原温度为303 K时制备的催化剂,催化BH3NH3水解产氢速率最快[转化频率TOF为140.8 L H2/(mol Ru·min)]。搅拌转速为450 r/min时,氨硼烷向催化剂表面传质最快,产氢速率最大。氨硼烷水解反应由催化剂界面反应控制,产氢速率与催化剂用量成正比。随着反应温度的升高,Ru活化的氨硼烷分子能量增加,反应速率逐渐增加。反应动力学计算表明Ru/SiO2催化剂催化BH3NH3水解产氢反应对氨硼烷浓度为零级反应,活化能为45 kJ/mol。
孙海杰 , 刘欣改 , 陈志浩 , 陈凌霞 , 李聪聪 , 梅洋洋 . 二氧化硅负载钌催化剂催化氨硼烷水解产氢研究[J]. 无机盐工业, 2020 , 52(5) : 81 -85 . DOI: 10.11962/1006-4990.2019-0398
Ru/SiO2 catalysts were synthesized via an impregnation-reduction method.The effect of Ru loading amount,amount of NaBH4 as the reducing agent,reduction temperature as well as the reaction conditions was investigated on the hydrogen generation from hydrolysis of BH3NH3 over Ru/SiO2 catalyst.Results showed that when Ru/SiO2 was prepared under the condi-tions as follows: Ru loading amount was 0.1%(mass fraction),n(NaBH4)∶n(Ru)=2.2∶1 and reduction temperature was 303 K,the highest catalytic activity towards hydrogen generation from hydrolysis of BH3NH3 was observed and the turnover frequency (TOF) reached up to 140.8 L/(mol·min),the volume-to-molar ratio of H2 to Ru .When stirring speed reached 450 r/min,the highest BH3NH3 adsorption rate was observed,leading to the highest reaction rate of hydrogen generation.Further,hydrolysis of BH3NH3 was controlled by the surface reaction of catalyst,and the catalytic activity towards hydrogen production increased with enhancing the amount of used catalyst.With increasing the reaction temperature,the activation energy of BH3NH3 was enhanced over Ru,resulting in the improvement of reaction rate.According to the kinetic study,H2 production from the hydro-lysis of BH3NH3 over Ru/SiO2 was a zero order reaction against the concentration of BH3NH3,and the Eawas 45 kJ/mol.
Key words: Ru; SiO2; BH3NH3; H2 generation
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