双模板剂合成CO_(2)P纳米片及其催化氨硼烷水解性能的研究  

SYNTHESIS OF Co_(2)P NANOPLATES WITH DUAL-TEMPLATE METHOD AND THEIR CATALYTIC ACTIVITY FOR HYDROLYSIS OF AMMONIA BORANE

作　　者：孙佳丽 郑君宁 花俊峰 邱小魁 许立信 叶明富[2,4,5] 万超[2,4,6,7] 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)

机构地区：[1]安徽硅宝有机硅新材料有限公司,安徽马鞍山243000 [2]安徽工业大学化学与化工学院 [3]浙江省环境科技有限公司 [4]南开大学先进能源材料化学教育部重点实验室 [5]宁德师范学院绿色能源与环境催化福建高校重点实验室 [6]浙江大学化学工程与生物工程学院 [7]常州大学江苏省绿色催化材料与技术重点实验室

出　　处：《石油炼制与化工》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)。

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.

关 键 词：磷化钴 氨硼烷 储氢材料 盐模板剂法 

分 类 号：TQ116.2[化学工程—无机化工] TB383.1[一般工业技术—材料科学与工程] TQ426