4.8 Article

Photoredox-Catalyzed Simultaneous Olefin Hydrogenation and Alcohol Oxidation over Crystalline Porous Polymeric Carbon Nitride

Journal

CHEMSUSCHEM
Volume 14, Issue 16, Pages 3344-3350

Publisher

WILEY-V C H VERLAG GMBH
DOI: 10.1002/cssc.202101041

Keywords

alcohol oxidation; hydrogenation; polymeric carbon nitride; photocatalysis; water splitting

Funding

  1. National Natural Science Foundation of China [21902105, 21972094]
  2. Guangdong Basic and Applied Basic Research Foundation [2020A1515010471]
  3. Foundation for Distinguished Young Talents in Higher Education of Guangdong [2018KQNCX221]
  4. Shenzhen Innovation Program [RCJC20200714114434086, JCYJ20190808142001745, JCYJ20200812160737002, KQTD2016053112042971]
  5. Guangdong Special Support Program
  6. Jiangsu Provincial Six Talent Peaks Project [XCL-090]
  7. Priority Academic Program Development of Jiangsu Higher Education Institutions (PAPD)
  8. Pengcheng Scholar Program

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The study introduces a porous polymeric carbon nitride with a crystalline backbone for visible light-induced photocatalytic hydrogen generation and alcohol transformation. The material's large surface area, short transfer path, and crystalline structure enhance photocatalytic performance, achieving high reactivity and selectivity in redox reactions.
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.

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