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首页> 外文期刊>Catalysis science & technology >Visible-light photocatalytic selective oxidation of C(sp(3))-H bonds by anion-cation dual-metal-site nanoscale localized carbon nitride
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Visible-light photocatalytic selective oxidation of C(sp(3))-H bonds by anion-cation dual-metal-site nanoscale localized carbon nitride

机译：可见光的光催化选择性氧化C (sp (3)) - h anion-cation债券dual-metal-site纳米本地化碳氮化

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摘要

Selective oxidation of C(sp(3))-H bonds to carbonyl groups by abstracting H with a photoinduced highly active oxygen radical is an effective method used to give high value products. Here, we report a heterogeneous photocatalytic alkanes C-H bonds oxidation method under the irradiation of visible light (lambda = 425 nm) at ambient temperature using an anion-cation dual-metal-site modulated carbon nitride. The optimized cation (C) of Fe3+ or Ni2+, with an anion (A) of phosphotungstate (PW123-) constitutes the nanoscale dual-metal-site (DMS). With a Fe-PW12 dual-metal-site as a model (FePW), we demonstrate a A-C DMS nanoscale localized carbon nitride (A-C/g-C3N4) exhibiting a highly enhanced photocatalytic activity with a high product yield (86% conversion), selectivity (up to 99%), and a wide functional group tolerance (52 examples). The carbon nitride performs the roles of both the visible light response, and improves the selectivity for the oxidation of C(sp(3))-H bonds to carbonyl groups, along with the function of A-C DMS in promoting product yield. Mechanistic studies indicate that this reaction follows a radical pathway catalyzed by a photogenerated electron and hole on A-C/g-C3N4 that is mediated by the (BuO)-Bu-t and (BuOO)-Bu-t radicals. Notably, a 10 g scale reaction was successfully achieved for alkane photocatalytic oxidation to the corresponding product with a good yield (80% conversion), and high selectivity (95%) under natural sunlight at ambient temperature. In addition, this A-C/g-C3N4 photocatalyst is highly robust and can be reused at least six times and the activity is maintained.
机译：选择性氧化的C - h键(sp (3))羰基化合物通过抽象的H光诱导的高度活性氧自由基是一种有效的方法用于提供高价值产品。光催化氧化烷烃碳氢键的方法可见光的照射下(λ=425海里)在环境温度下使用anion-cation dual-metal-site调制碳氮化。Ni2 +,磷钨酸的阴离子(A)(PW123)构成了纳米级dual-metal-site (DMS)。dual-metal-site模型(FePW),我们将演示得了DMS纳米本地化碳氮化(a - c / g-C3N4)表现出一个高度增强光催化活性高的产品产量转换(86%),选择性(99%),和一个宽官能团容忍(52例)。碳氮化执行的角色可见光响应,提高了选择性氧化的C - h键(sp (3))羰基化合物的功能得了DMS在促进产品产量。研究表明,这个反应之前激进的通路photogenerated催化电子和洞a - c / g-C3N4介导(BuO)里和(BuOO)里的激进分子。值得注意的是,10 g规模反应是成功实现对烷烃光催化氧化相应的产品与良好的收益率(80%转换)和高选择性(95%)自然光照环境温度。此外,a - c / g-C3N4光催化剂是高度健壮和可重用和至少6倍该活动。

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