Dual Ce@g-C3N4-Photoredox/Chlorine Catalysis: Cross-Dehydrogenative Coupling of N-Heteroarenes and Alkanes/Ethers with H2 Evolution

IF 4.9 1区 化学 Q1 CHEMISTRY, ORGANIC Organic Letters Pub Date : 2024-11-11 DOI:10.1021/acs.orglett.4c03538
Hong-Tao Ji, Yu-Qi Tang, Yao-Hui Wang, Jia-Sheng Wang, Yao-Dan Xu, Yan-Yan Zeng, Ting Li, Shao-Feng Gong, Wei-Min He
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Abstract

With Ce@g-C3N4 as a heterogeneous semiconductor photocatalyst, nBu4NCl as both a redox catalyst and a hydrogen atom transfer catalyst, the first example of semiheterogeneous photocatalytic cross-dehydrogenative coupling of N-heteroarenes and alkanes/ethers with H2 evolution was developed. Both a diverse array of high-value alkylated N-heteroarenes and clean H2 can be efficiently coproduced under sacrificial reagent- and chemical oxidant/reductant-free conditions. Combining both the reversible Ce4+/Ce3+ redox pair and the reversible Cl̅/Cl ̇ redox pair can considerably improve the photocatalytic efficiency.

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Ce@g-C3N4 光氧/氯双重催化:N-Heteroarenes 和烷烃/醚的交叉脱氢偶联与 H2 进化
以 Ce@g-C3N4 作为异相半导体光催化剂,以 nBu4NCl 作为氧化还原催化剂和氢原子转移催化剂,首次开发了半异相光催化交叉脱氢偶联 N-heteroarenes 和烷烃/醚与 H2 进化的实例。在无牺牲试剂和无化学氧化剂/还原剂的条件下,可以高效地共同生成各种高价值的烷基化 N-heteroarenes 和清洁的 H2。将可逆的 Ce4+/Ce3+ 氧化还原对和可逆的 Cl̅/Cl ̅ 氧化还原对结合起来,可以大大提高光催化效率。
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来源期刊
Organic Letters
Organic Letters 化学-有机化学
CiteScore
9.30
自引率
11.50%
发文量
1607
审稿时长
1.5 months
期刊介绍: Organic Letters invites original reports of fundamental research in all branches of the theory and practice of organic, physical organic, organometallic,medicinal, and bioorganic chemistry. Organic Letters provides rapid disclosure of the key elements of significant studies that are of interest to a large portion of the organic community. In selecting manuscripts for publication, the Editors place emphasis on the originality, quality and wide interest of the work. Authors should provide enough background information to place the new disclosure in context and to justify the rapid publication format. Back-to-back Letters will be considered. Full details should be reserved for an Article, which should appear in due course.
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