Photoredox‐Catalyzed Simultaneous Olefin Hydrogenation and Alcohol Oxidation over Crystalline Porous Polymeric Carbon Nitride
Photoredox‐Catalyzed Simultaneous Olefin Hydrogenation and Alcohol Oxidation over Crystalline Porous Polymeric Carbon Nitride
复制标题
光氧化还原——结晶多孔聚合物氮化碳催化同步烯烃加氢和醇氧化
DOI：
10.1002/cssc.202101041
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发表时间：
2021
期刊：
影响因子：
8.4
通讯作者：
Chenliang Su
中科院分区：
文献类型：
--
作者：
Chuntian Qiu;Yangyang Sun;Yangsen Xu;Bing Zhang;Xu Zhang;Lei Yu;Chenliang Su
光催化水分解技术（PWST）的蓬勃发展为高附加值氢化和氧化精细化学品的可持续合成开辟了新途径，其中设计用于原位和协同利用光生氧化还原中心的高效半导体是关键。在此，构建了具有晶体主链的多孔聚合碳氮化物（PPCN），用于可见光诱导光激发电子光催化制氢，然后原位用于烯烃加氢。同时，各种醇通过光激发空穴选择性地转化为有价值的醛或酮。 PPCN的孔隙率为其提供了大的表面积和光生载流子从本体到表面的短传输路径，并且晶体结构有利于光生电荷的转移和分离，从而提高了整体光催化性能。该协同光催化体系实现了高反应活性和选择性、良好的官能度耐受性和广泛的反应范围。研究结果有助于开发高效半导体光催化剂和基于 PWST 的协同氧化还原反应系统，用于高附加值精细化学品生产。
Booming of photocatalytic water splitting technology (PWST) opens a new avenue for the sustainable synthesis of high‐value‐added hydrogenated and oxidized fine chemicals, in which the design of efficient semiconductors for the in‐situ and synergistic utilization of photogenerated redox centers are key roles. Herein, a porous polymeric carbon nitride (PPCN) with a crystalline backbone was constructed for visible light‐induced photocatalytic hydrogen generation by photoexcited electrons, followed by in‐situ utilization for olefin hydrogenation. Simultaneously, various alcohols were selectively transformed to valuable aldehydes or ketones by photoexcited holes. The porosity of PPCN provided it with a large surface area and a short transfer path for photogenerated carriers from the bulk to the surface, and the crystalline structure facilitated photogenerated charge transfer and separation, thus enhancing the overall photocatalytic performance. High reactivity and selectivity, good functionality tolerance, and broad reaction scope were achieved by this concerted photocatalysis system. The results contribute to the development of highly efficient semiconductor photocatalysts and synergistic redox reaction systems based on PWST for high‐value‐added fine chemical production.