摘要
开发一种在温和条件下具有高活性、高选择性的催化剂是实现氨硼烷水解制氢应用的关键。以构建具有P掺杂材料为出发点,以两种不同比例的金属盐作为模板剂,以过渡非贵金属Co为中心金属,合成出制作方法简便、性能优异的催化剂。通过乙酸钴和氨水制备出Co_(3)O_(4)前躯体,将Co_(3)O_(4)前躯体与NaH_(2)PO_(2),NaCl,LiCl混合,在N_(2)气氛下焙烧,然后进行水洗将两种盐模板剂去除,得到纳米片催化剂CO_(2)P-NaLi。试验结果表明,当n(NaCl)∶n(LiCl)=1∶0.15时制备的催化剂CO_(2)P-NaLi_(0.15)催化活性最高,其在298 K、光照条件下催化氨硼烷水解反应的初始转化率(TOF)为31.2 min^(-1),且该催化剂上氨硼烷分解的活化能(E_(a))为60.8 kJ/mol。循环5次后,催化剂依然保持良好活性,表明其拥有良好的稳定性。
The development of a kind of catalyst with high activity and high selectivity under mild conditions is the key to realize the application of hydrolysis of ammonia borane(AB)for hydrogen production.Starting from the construction of P-doped materials,the catalyst with two different proportions of metal salts as the salt template and the transition non-precious metal CO^(2+)as the center metal was prepared.The Co_(3)O_(4)precursor was prepared by cobalt acetate and ammonia water,and the Co_(3)O_(4)precursor was mixed with NaH_(2)PO_(4),NaCl and LiCl,and calcined in N_(2)atmosphere to synthesize CO_(2)P-NaLi catalyst.After washing,the two salt templates were removed to obtain the final CO_(2)P-NaLi catalyst,which was a highly efficient catalyst that could react under mild conditions.The results showed that the catalytic activity of CO_(2)P-NaLi_(0.15)catalyst was the highest when n(NaCl)∶n(LiCl)=1∶0.15,its initial conversion rate(TOF)was 31.2 min^(-1) at 298 K under light irradiation,and the activation energy(E_(a))for the decomposition of ammonia borane on the catalyst was 60.8 kJ mol.After 5 cycles,the catalytic still keep good activity,which indicated that it had good stability.
作者
孙佳丽
郑君宁
花俊峰
邱小魁
许立信
叶明富
万超
Sun Jiali;Zheng Junning;Hua Junfeng;Qiu Xiaokui;Xu Lixin;Ye Mingfu;Wan Chao(GBXF Silicones Co.,Ltd.,Ma’anshan,Anhui 243000;School of Chemistry and Chemical Engineering,Anhui University of Technology;Zhejiang Environment Technology Co.,Ltd.;Key Laboratory of Advanced Energy Materials Chemistry(Ministry of Education),Nankai University;Key Laboratory of Green Energy and Environment Catalysis(Ningde Normal University),Fujian Province University;College of Chemical Engineering and Biological Engineering,Zhejiang University;Jiangsu Key Laboratory of Advanced Catalytic Materials and Technology,Changzhou University)
出处
《石油炼制与化工》
CAS
CSCD
北大核心
2024年第2期186-192,共7页
Petroleum Processing and Petrochemicals
基金
国家自然科学基金青年基金项目(22108238)
中国博士后面上项目(2019M662060)
特别资助站中项目(2020T130580)
浙江省化工高效制造技术重点实验室开放项目(ZJKL-ACEMT-1802)。
关键词
磷化钴
氨硼烷
储氢材料
盐模板剂法
cobalt phosphide
ammonia borane
hydrogen storage material
salt template method
