4.8 Article

Photocatalytic Selective Oxidation of HMF Coupled with H2 Evolution on Flexible Ultrathin g-C3N4 Nanosheets with Enhanced N-H Interaction

Journal

ACS CATALYSIS
Volume 12, Issue 3, Pages 1919-1929

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acscatal.1c05357

Keywords

strong interaction; hydrogen evolution; selective oxidation of HMF; flexible surface; ultrathin g-C3N4 nanosheets

Funding

  1. National Key Research and Development Program of China [2020YFA0710301]
  2. National Natural Science Foundation of China [21972078, 51972195, 21573135, 51602179]
  3. Shandong Provincial Natural Science Foundation [ZR2019MEM004]
  4. Shandong University Multidisciplinary Research and Innovation Team of Young Scholars [2020QNQT11]
  5. Qilu Young Scholar Program of Shandong University

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The flexible ultrathin graphitic carbon nitride (UCNT) is found to be an active and stable photocatalyst for the solar-driven selective oxidation of 5-hydroxymethylfurfural (HMF) into 2,5-diformylfuran (DFF) coupled with H-2 evolution. The UCNT exhibits high activity and selectivity, as well as good cycling stability.
Solar-driven catalytic oxidation of 5-hydroxymethylfurfural (HMF) into 2,5-diformylfuran (DFF) coupled with H-2 evolution has been considered a promising approach. The exploration of an active and stable photocatalyst still remains challenging work. Herein, we found that the flexible ultrathin graphitic carbon nitride (UCNT) could be an ideal candidate. The UCNT exhibits photocatalytic performance in selective oxidation of HMF into DFF coupled with H-2 evolution with activities of 95.0 and 92.0 mu mol g(-1) h(-1) under visible light irradiation. Importantly, the UCNT also demonstrates high DFF selectivity (95%) and good cycling stability. The activity may be ascribed to the strong specific interaction between HMF and UCNT. Solid-state nuclear magnetic resonance (NMR) and density functional theory (DFT) results reveal that the twisted structure of HMF molecules could form a strong interaction between HMF and UCNT, reducing the dehydrogenation energy barrier for HMF oxidation. In addition, mechanistic studies reveal that center dot C6H4O3 is the key radical intermediate during the HMF oxidation process by a in situ electron spin resonance (ESR) trapping test. Our work clarifies the interaction of complex biomass molecules on the flexible catalyst surface and provides views on the further development of heterogeneous catalytic biomass conversion.

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