Loofah-like carbon nitride sponge towards the highly-efficient photocatalytic transfer hydrogenation of nitrophenols with water as the hydrogen source

Fanglei Yao, Liming Dai, Jiabao Bi, Wenkang Xue, Jingyao Deng, Chenchen Fang, Litong Zhang, Hongan Zhao, Wenyao Zhang, Pan Xiong, Yongsheng Fu, Jingwen Sun, Junwu Zhu

Research output: Contribution to journalArticlepeer-review

11 Scopus citations

Abstract

The vigorous development of photocatalytic water splitting technology has laid the foundation for the photocatalytic transfer hydrogenation of organic substrates to produce the high value-added chemicals using water as hydrogen source. Nevertheless, the high dissociation energy of the O–H bond impedes its academic progress and the practical applications. Herein, we synthesize a 3D hierarchical porous loofah-like carbon nitride sponge (LCN) with ultrathin thickness via the supramolecular pre-organization coupling with the oxidation etching process, in which the heterogeneous oxygen atoms and the nitrogen vacancies are in-situ engineered. On top of the adorable photocatalytic H2 evolution (4812 μmol h−1 g−1), LCN associated with Pt cocatalyst reveals a conversion rate of 96.5 % towards the hydrogenation of 4-nitrophenol, substantially superior to the reference experiment (8.3 %). Further based on the isotope-labeling tests and the density functional theory calculations, the photo-generated H0 from water is clarified to be the direct reducing agent, tactfully skipping the hydrogen extraction step in the traditional path. This work provides a green and sustainable methodology to transfer the solar energy to the valuable fine chemicals, as well as highlights the importance of the 3D hierarchical porous structure to the catalytic activity.

Original languageEnglish
Article number136430
JournalChemical Engineering Journal
Volume444
DOIs
StatePublished - 15 Sep 2022
Externally publishedYes

Keywords

  • Carbon nitride
  • Hydrogen evolution
  • Nitrogen vacancy
  • Oxygen doping
  • Photocatalytic transfer hydrogenation

ASJC Scopus subject areas

  • General Chemistry
  • Environmental Chemistry
  • General Chemical Engineering
  • Industrial and Manufacturing Engineering

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