首页|异质结Al-PMOFs/CdZnS的制备及光催化苯甲胺氧化

异质结Al-PMOFs/CdZnS的制备及光催化苯甲胺氧化

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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.
Preparation of heterojunction Al-PMOFs/CdZnS and photocatalytic oxidation of benzylamine
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.

Al-PMOFsCdZnSvisible-light photocatalysisoxidative coupling reaction of benzylamineheterojunctioncatalysis technology

席辉、尹雪、康燕、杨静、徐雪青、杨志旺

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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

西藏藏医药大学 藏药系,西藏 拉萨 850000

Al-PMOFs CdZnS 可见光催化 苯甲胺氧化偶联 异质结 催化技术

国家自然科学基金项目国家自然科学基金项目

5206302621563026

2024

精细化工
大连化工研究院设计院 中国化工学会精细化工专业委员会 辽宁省化工研究院

精细化工

CSTPCD北大核心
影响因子:0.557
ISSN:1003-5214
年,卷(期):2024.41(2)
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