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用于通过环加成反应进行光催化CO转化的钛金属有机框架

Titanium metal-organic frameworks for photocatalytic CO conversion through a cycloaddition reaction.

作者信息

Kegere James, Alneyadi Shaikha S, Paz Alejandro Perez, Siddig Lamia A, Alblooshi Afra, Alnaqbi Mohamed A, Alzamly Ahmed, Greish Yaser E

机构信息

Department of Chemistry, College of Science UAE.

Zayed Centre for Health Sciences, United Arab Emirates University Al Ain 15551 UAE

出版信息

Nanoscale Adv. 2024 Aug 16;6(19):4804-13. doi: 10.1039/d4na00535j.

Abstract

The elevated levels of CO in the atmosphere have been a major concern for environmental scientists. Capturing CO gas and its subsequent conversion to useful organic compounds is one of the avenues that have been extensively studied in the last decade. The photocatalytic cycloaddition of CO is a promising approach for effective CO capture and the production of value-added chemicals such as cyclic carbonates. MOF-901, a titanium-based metal-organic framework with hexagonal layers and imine linkages, was successfully oxidized in this study to MOF-997, incorporating amide linkages using Oxone. Both MOFs displayed remarkable photocatalytic activity in CO cycloaddition under mild conditions, including moderate temperatures and visible light exposure. Particularly noteworthy is MOF-997, exhibiting superior performance with donor-acceptor active sites, achieving a 99.9% yield in catalyzing CO conversion from styrene epoxide to styrene carbonate under solvent conditions.

摘要

大气中一氧化碳(CO)水平的升高一直是环境科学家主要关注的问题。捕获CO气体并将其随后转化为有用的有机化合物是过去十年中得到广泛研究的途径之一。CO的光催化环加成是有效捕获CO以及生产环状碳酸酯等增值化学品的一种有前景的方法。MOF-901是一种具有六边形层和亚胺键的钛基金属有机框架,在本研究中通过使用过氧单硫酸盐成功氧化为包含酰胺键的MOF-997。在温和条件下,包括适度温度和可见光照射下,两种金属有机框架在CO环加成反应中均表现出显著的光催化活性。特别值得注意的是MOF-997,它具有供体-受体活性位点,表现出卓越的性能,在溶剂条件下催化从苯乙烯环氧化物到苯乙烯碳酸酯的CO转化反应中,产率达到99.9%。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/4222/11421550/c31cab219610/d4na00535j-f1.jpg

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