Supercharging green chemistry: Unleashing 1, 4-NADH regeneration and unprecedented C(sp3)-F bond activation via NiS-NiO/S-g-C3N4 nanocomposite photocatalyst under solar light

IF 16.4 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY
Sanjana Kumari, Atul P. Singh, Rajesh K. Yadav, Satyam Singh, Rehana Shahin, Indra Kumari, Aditya Nath Yadav, Abhishek K. Yadav, Kavita Sharma, Dilip K. Dwivedi, Hany W. Darwish, Jeong Ryeol Choi
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引用次数: 0

Abstract

Fluorinated and enzymatic chemicals are widely used in society due to their chemical, physical, and biological qualities. Nevertheless, despite their vital importance, present approaches to adding fluorine to molecules and regenerating enzyme cofactors have serious flaws. For instance, numerous approaches are photocatalytic and employ stoichiometric counterparts of heavy metals. Prevailing photocatalytic approaches, on the other hand, show very poor activity, and selectivity has not been attained by heterogeneous photocatalysis, despite the several benefits such a method would provide. Here, we show how heterogeneous photocatalysis may be used to selectively create C(sp3)-F bonds and 1,4-NADH regeneration cofactor. Employing NiS-NiO/S-g-C3N4 nanocomposite photocatalyst as a photocatalyst, NAD+ and Selectfluor as an acceptor and mild fluorine donor, effective 1,4-NADH regeneration, and decarboxylative fluorination of carboxylic acids can be attained in very short reaction times. Furthermore, NiS-NiO/S-g-C3N4 nanocomposite photocatalyst exhibits outstanding levels of robustness and photo-catching capacity. These aspects, attached to the mild environment of the reaction scheme, exhibit a breakthrough toward the sustainable cofactor of 1,4-NADH regeneration and synthesis of fluorinated compounds.

超级绿色化学:在太阳光下通过 NiS-NiO/S-g-C3N4 纳米复合光催化剂实现 1,4-NADH 再生和前所未有的 C(sp3)-F 键活化
氟化化学品和酶制剂因其化学、物理和生物特性而被社会广泛使用。然而,尽管它们至关重要,但目前向分子中添加氟和再生酶辅助因子的方法存在严重缺陷。例如,许多方法都是光催化法,采用的是重金属的化学计量对应物。另一方面,目前流行的光催化方法显示出非常差的活性,而且异相光催化还没有达到选择性,尽管这种方法会带来一些好处。在这里,我们展示了如何利用异相光催化技术选择性地生成 C(sp3)-F 键和 1,4-NADH 再生辅因子。利用 NiS-NiO/S-g-C3N4 纳米复合光催化剂作为光催化剂,NAD+ 和 Selectfluor 作为受体和温和的氟供体,可以在很短的反应时间内实现有效的 1,4-NADH 再生和羧酸的脱羧氟化反应。此外,NiS-NiO/S-g-C3N4 纳米复合光催化剂还具有出色的稳健性和光捕捉能力。这些方面与反应方案的温和环境相辅相成,为 1,4-NADH 的可持续再生辅因子和含氟化合物的合成带来了突破性进展。
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来源期刊
Accounts of Chemical Research
Accounts of Chemical Research 化学-化学综合
CiteScore
31.40
自引率
1.10%
发文量
312
审稿时长
2 months
期刊介绍: Accounts of Chemical Research presents short, concise and critical articles offering easy-to-read overviews of basic research and applications in all areas of chemistry and biochemistry. These short reviews focus on research from the author’s own laboratory and are designed to teach the reader about a research project. In addition, Accounts of Chemical Research publishes commentaries that give an informed opinion on a current research problem. Special Issues online are devoted to a single topic of unusual activity and significance. Accounts of Chemical Research replaces the traditional article abstract with an article "Conspectus." These entries synopsize the research affording the reader a closer look at the content and significance of an article. Through this provision of a more detailed description of the article contents, the Conspectus enhances the article's discoverability by search engines and the exposure for the research.
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