光催化C(sp3) -C (sp3)交叉偶联羧酸和烷基卤化物的镍配合物和氮化碳

IF 15.7 1区 综合性期刊 Q1 MULTIDISCIPLINARY SCIENCES
Miguel M. de Vries Ibáñez, Luis A. Cipriano, Valeria Lagostina, Andrea Olivati, Mario Chiesa, Annamaria Petrozza, Giovanni Di Liberto, Gianvito Vilé
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引用次数: 0

摘要

开发构建C(sp3) -C (sp3)键的强大催化方法对于合成多种药物分子至关重要。然而,从化学的角度来看,由于区域选择性、官能团耐受性和复杂的催化剂设计等问题,这种类型的反应提出了重大的挑战。目前的金属光氧化还原方法并没有提供一个可行的解决方案,因为它们依赖于昂贵、有毒和稀有的铱基光催化剂,严重限制了它们的广泛应用。在这项研究中,我们介绍了氮化碳纳米片作为传统光催化剂的高效和可持续的替代品。当与镍结合时,氮化碳纳米片有利于烷基卤化物和羧酸的交叉偶联。我们的研究结果展示了广泛的衬底范围,并突出了光催化剂的可回收性。密度泛函理论计算为催化系统在促进光脱羧和随后的C-C键形成中的作用提供了分子见解。这项工作拓展了光氧化还原化学的潜力,并为有效的工业相关光化学转化过程提供了一种新方法。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

Photocatalytic C(sp3)–C(sp3) cross-coupling of carboxylic acids and alkyl halides using a nickel complex and carbon nitride

Photocatalytic C(sp3)–C(sp3) cross-coupling of carboxylic acids and alkyl halides using a nickel complex and carbon nitride

Developing robust catalytic methods for constructing C(sp3)–C(sp3) bonds is critically important for synthesizing a diverse array of drug molecules. However, this type of reaction poses significant challenges from a chemical standpoint due to issues with regioselectivity, functional group tolerance and complex catalyst design. Current metallaphotoredox approaches do not provide a viable solution because they rely on expensive, toxic, and rare iridium-based photocatalysts, severely limiting their widespread application. In this study, we introduce carbon nitride nanosheets as an efficient and sustainable alternative to traditional photocatalysts. When combined with nickel, carbon nitride nanosheets facilitates the cross-coupling of alkyl halides and carboxylic acids. Our results demonstrate a broad substrate scope and highlight the recyclability of the photocatalyst. Density functional theory calculations provide molecular insights into the role of the catalytic system in facilitating photodecarboxylation and subsequent C–C bond formation. This work expands the potential of photoredox chemistry, and offers a novel method for efficient, industrially relevant light-to-chemical conversion processes.

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来源期刊
Nature Communications
Nature Communications Biological Science Disciplines-
CiteScore
24.90
自引率
2.40%
发文量
6928
审稿时长
3.7 months
期刊介绍: Nature Communications, an open-access journal, publishes high-quality research spanning all areas of the natural sciences. Papers featured in the journal showcase significant advances relevant to specialists in each respective field. With a 2-year impact factor of 16.6 (2022) and a median time of 8 days from submission to the first editorial decision, Nature Communications is committed to rapid dissemination of research findings. As a multidisciplinary journal, it welcomes contributions from biological, health, physical, chemical, Earth, social, mathematical, applied, and engineering sciences, aiming to highlight important breakthroughs within each domain.
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