| 原位生成非晶纳米钴高效催化氨硼烷的醇解制氢 |
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| 引用本文： | 陈浩,俞哲健,徐丹丹,李洋,王明明,夏良敏,罗书平.原位生成非晶纳米钴高效催化氨硼烷的醇解制氢[J].无机化学学报,2019,35(1):141-148. |
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| 作者姓名： | 陈浩 俞哲健 徐丹丹 李洋 王明明 夏良敏 罗书平 |
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| 作者单位： | 浙江工业大学绿色化学合成技术国家重点实验室培育基地 |
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| 基金项目： | 国家自然科学基金（No.21376222）和浙江省自然科学基金（No.LY18B060011）资助项目。 |
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| 摘 要： | 用金属钴配合物和过渡金属(Cu,Ni,Co等)原位生成的非晶纳米粒子作为均相、多相催化剂,研究氨硼烷的醇解放氢反应,结果发现原位生成的非晶钴纳米粒子展现出优异的产氢性能。通过10次的催化循环测试,钴纳米粒子放氢催化转换数(TON)可达6 000,最高催化产氢速率(TOF)达515 mol_(H_2)·mol_(metal)~(-1)·h~(-1)。该催化剂制备方便,且产氢稳定性好。此外,对钴纳米粒子催化氨硼烷放氢实验做动力学研究,计算其催化活化能为20.00 kJ·mol~(-1),低于大多数已经报道的其他纳米催化剂催化氨硼烷放氢反应的活化能。通过硼谱的跟踪检测,发现钴纳米催化氨硼烷的醇解反应产物是硼酸三甲酯,并对此催化反应机理进行了初步的解释和讨论。
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| 关 键 词： | 原位合成 氨硼烷 醇解 制氢 |
| 收稿时间： | 2018/8/14 0:00:00 |
| 修稿时间： | 2018/11/14 0:00:00 |
In-Situ Formed Amorphous Co Nanoparticles for Efficiently Catalytic Hydrogen Production from the Methanolysis of Ammonia Borane |
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| CHEN Hao,YU Zhe-Jian,XU Dan-Dan,LI Yang,WANG Ming-Ming,XIA Liang-Min and LUO Shu-Ping.In-Situ Formed Amorphous Co Nanoparticles for Efficiently Catalytic Hydrogen Production from the Methanolysis of Ammonia Borane[J].Chinese Journal of Inorganic Chemistry,2019,35(1):141-148. |
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| Authors: | CHEN Hao YU Zhe-Jian XU Dan-Dan LI Yang WANG Ming-Ming XIA Liang-Min and LUO Shu-Ping |
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| Institution: | State Key Laboratory Breeding Base of Green Chemistry-Synthesis Technology, Zhejiang University of Technology, Hangzhou 310014, China,State Key Laboratory Breeding Base of Green Chemistry-Synthesis Technology, Zhejiang University of Technology, Hangzhou 310014, China,State Key Laboratory Breeding Base of Green Chemistry-Synthesis Technology, Zhejiang University of Technology, Hangzhou 310014, China,State Key Laboratory Breeding Base of Green Chemistry-Synthesis Technology, Zhejiang University of Technology, Hangzhou 310014, China,State Key Laboratory Breeding Base of Green Chemistry-Synthesis Technology, Zhejiang University of Technology, Hangzhou 310014, China,State Key Laboratory Breeding Base of Green Chemistry-Synthesis Technology, Zhejiang University of Technology, Hangzhou 310014, China and State Key Laboratory Breeding Base of Green Chemistry-Synthesis Technology, Zhejiang University of Technology, Hangzhou 310014, China |
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| Abstract: | Amorphous Co nanoparticles formed in-situ displayed high catalytic activity for hydrogen generation from the methanolysis reaction of ammonia borane, among many homogeneous catalysts and heterogeneous catalysts of cobalt. Its turnover number (TON) was up to 6 000 for ten cycles and its turnover frequency (TOF) was up to 515 molH2·molmetal-1·h-1. Moreover, the easily preparation and the great recycling performance made it have good application in future. After the kinetics studies, its catalytic activation energy (Ea) for the methanolysis reaction was measured as 20.00 kJ·mol-1, which was lower than most of the reported values for other nano-sized catalysts. Through the 11B NMR, trimethylborate was the only product. Furthermore, the catalytic reaction mechanism was preliminarily explained and discussed. |
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| Keywords: | in-situ synthesis ammonia borane methanolysis hydrogen generation |
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