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Issue 36, 2017
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Brønsted base site engineering of graphitic carbon nitride for enhanced photocatalytic activity

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Abstract

Graphitic carbon nitride (g-C3N4) is a promising two-dimensional polymeric photocatalyst in the field of solar energy conversion. In the past few years many modifications of g-C3N4 have been studied extensively; however, the difficulty in obtaining detailed structural information both on its intrinsic covalent interactions and surrounding bonding environments largely restricts the rational design and development of inherent structure-controlled g-C3N4 based photocatalysts and fundamental understanding of their mechanistic operations. Herein, we demonstrate a high-pressure hydrogenation treatment method for g-C3N4 and introduce 1D 13C and 15N and 2D 15N Radio Frequency-driven Dipolar Recoupling (RFDR) solid-state nuclear magnetic resonance spectroscopy for identifying the structural information and surrounding hydrogen-bonding environment of treated g-C3N4 samples. The surface Brønsted base sites of g-C3N4 samples can be tuned systematically through changing the treatment conditions. We find that the terminal isolated –NH2 and the hydrogenated nitrogen species in treated g-C3N4 samples seem to be the origin of their improved activities for photocatalytic hydrogen evolution and favor the enhancement of light harvesting and carrier transport. The as-prepared HCN400-4-2 sample treated at a pressure of 4 MPa and a temperature of 400 °C for 2 h in a hydrogen atmosphere displays the highest H2 evolution reaction (HER) activity, which is over 26 times higher than that of pristine g-C3N4.

Graphical abstract: Brønsted base site engineering of graphitic carbon nitride for enhanced photocatalytic activity

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Publication details

The article was received on 27 Jul 2017, accepted on 14 Aug 2017 and first published on 14 Aug 2017


Article type: Paper
DOI: 10.1039/C7TA06602C
Citation: J. Mater. Chem. A, 2017,5, 19227-19236
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    Brønsted base site engineering of graphitic carbon nitride for enhanced photocatalytic activity

    X. L. Wang, W. Q. Fang, W. Liu, Y. Jia, D. Jing, Y. Wang, L. Yang, X. Gong, Y. Yao, H. G. Yang and X. Yao, J. Mater. Chem. A, 2017, 5, 19227
    DOI: 10.1039/C7TA06602C

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