Meso- and Microporous Metal–Organic Frameworks for Efficient Photo-Oxidation of Benzylamine

IF 3.7 2区化学 Q2 CHEMISTRY, APPLIED

Applied Organometallic Chemistry Pub Date : 2024-08-11 DOI:10.1002/aoc.7670

Lifei Liu, Xiaoqing Yang, Pengfei Li, Luyuan Zhang, Yali Luo, Meng Yan, Yang Deng, Xia An, Jianling Zhang, Xu Wu

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Abstract

The construction of metal–organic frameworks (MOFs) with desirable structures for high-performance photocatalysis is attractive but remains challenging. Here, a hierarchically meso- and microporous scCu-MOF-74 was synthesized in supercritical CO₂ (scCO₂)/methanol solution. Compared with the conventional microporous Cu-MOF-74, the meso- and microporous scCu-MOF-74 has more exposed and accessible Lewis acid sites derived from the missing-linker defects. The unique structure endows scCu-MOF-74 with superior molecular accessibility, enhanced separation, and transfer efficiency of photogenerated charges. High catalytic activity and reusability can be achieved in photo-oxidative coupling of amines, reaching a maximum N-benzylbenzaldimine yield rate of 4.80 mmol g⁻¹ h⁻¹ under mild conditions, that is, air atmosphere and room temperature. This study provides a new idea for improving the intrinsic photocatalytic activities of MOFs.

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用于高效光氧化苄胺的中孔和微孔金属有机框架

为实现高性能光催化而构建具有理想结构的金属有机框架（MOFs）非常有吸引力，但仍然具有挑战性。本文在超临界二氧化碳（scCO2）/甲醇溶液中合成了分层介孔和微孔scCu-MOF-74。与传统的微孔Cu-MOF-74相比，介孔和微孔scCu-MOF-74具有更多暴露和可访问的路易斯酸位点，这些位点来自于缺失的连接体缺陷。这种独特的结构赋予了 scCu-MOF-74 优异的分子可及性，提高了光生电荷的分离和转移效率。这种催化剂在胺的光氧化偶联反应中具有很高的催化活性和可重复使用性，在温和的条件下，即空气环境和室温下，N-苄基苯甲醛二胺的最大产率可达 4.80 mmol g-1 h-1。这项研究为提高 MOFs 的内在光催化活性提供了新思路。

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来源期刊

Applied Organometallic Chemistry 化学-无机化学与核化学

CiteScore

7.80

自引率

10.30%

发文量

408

审稿时长

2.2 months

期刊介绍： All new compounds should be satisfactorily identified and proof of their structure given according to generally accepted standards. Structural reports, such as papers exclusively dealing with synthesis and characterization, analytical techniques, or X-ray diffraction studies of metal-organic or organometallic compounds will not be considered. The editors reserve the right to refuse without peer review any manuscript that does not comply with the aims and scope of the journal. Applied Organometallic Chemistry publishes Full Papers, Reviews, Mini Reviews and Communications of scientific research in all areas of organometallic and metal-organic chemistry involving main group metals, transition metals, lanthanides and actinides. All contributions should contain an explicit application of novel compounds, for instance in materials science, nano science, catalysis, chemical vapour deposition, metal-mediated organic synthesis, polymers, bio-organometallics, metallo-therapy, metallo-diagnostics and medicine. Reviews of books covering aspects of the fields of focus are also published.