异质结Al-PMOFs/CdZnS的制备及光催化苯甲胺氧化
Preparation of heterojunction Al-PMOFs/CdZnS and photocatalytic oxidation of benzylamine
席辉 1尹雪 1康燕 2杨静 1徐雪青 1杨志旺1
作者信息
- 1. 西北师范大学 化学化工学院,生态功能高分子材料教育部重点实验室,甘肃省生态环境高分子材料重点实验室,甘肃 兰州 730070
- 2. 西藏藏医药大学 藏药系,西藏 拉萨 850000
- 折叠
摘要
以 5,10,15,20-(4-羧基苯基)卟啉(TCPP)和AlCl3·6H2O为原料,采用水热法合成了具有立方柱状结构的卟啉基金属有机框架化合物(Al-PMOFs),然后通过共沉淀法将CdZnS纳米颗粒沉积在Al-PMOFs棱柱上,得到了界面接触良好的异质结Al-PMOFs/CdZnS.利用SEM、XPS、FTIR及UV-Vis对产物进行了表征.将其应用于可见光催化苯甲胺氧化偶联反应中,并探讨了光催化反应机理.结果表明,Al-PMOFs/CdZnS 具有较好的光催化反应活性和稳定性.室温下,以N,N-二甲基甲酰胺为溶剂,经可见光照射 7 h后,苯甲胺发生氧化偶联反应生成了N-苄基-1-苯基甲亚胺(BPMI),苯甲胺的转化率可达97%,BPMI的选择性达99%.Al-PMOFs/CdZnS光催化性能的提高主要归因于Al-PMOFs与CdZnS之间形成了直接Z-scheme异质结,促进了Al-PMOFs和CdZnS界面电荷的传输,抑制了Al-PMOFs/CdZnS表面光生载流子的复合.
Abstract
Porphyrin-based metal organic framework compound(Al-PMOFs)with cubic columnar crystal structure was synthesized from hydrothermal reaction of 5,10,15,20-(4-carboxyphenyl)porphyrin(TCPP)and AlCl3·6H2O.Then,heterojunction Al-PMOFs/CdZnS with good interfacial contact was obtained by depositing CdZnS nanoparticles on the surface of Al-PMOFs cubic columns via chemical coprecipitation,characterized by SEM,XPS,FTIR and UV-Vis adsorption spectroscopy,and analyzed on its photocatalytic activity for the photooxidative coupling reaction of benzylamine.The results showed that Al-PMOFs/CdZnS exhibited excellent photocatalytic activity and stability.The mechanism of photocatalytic reaction was discussed.Benzylamine was oxidized to form n-benzyl-1-phenylmethylimine(BPMI)when N,N-dimethylformamide(DMF)was used as solvent at room temperature,under irradiation of visible light for 7 h.The conversion rate of benzylamine reached 97%,and the selectivity of BPMI reached 99%.The improvement in photoactivity of Al-PMOFs/CdZnS was mainly attributed to the formation of Z-scheme heterojunction between Al-PMOFs and CdZnS,which could promote charge transfer at the interface of Al-PMOFs and CdZnS,and inhibit the recombination of Al-PMOFs/CdZnS surface photocarriers.
关键词
Al-PMOFs/CdZnS/可见光催化/苯甲胺氧化偶联/异质结/催化技术Key words
Al-PMOFs/CdZnS/visible-light photocatalysis/oxidative coupling reaction of benzylamine/heterojunction/catalysis technology引用本文复制引用
基金项目
国家自然科学基金项目(52063026)
国家自然科学基金项目(21563026)
出版年
2024
NETL
NSTL
维普
万方数据