Journal
JOURNAL OF MATERIALS CHEMISTRY C
Volume 8, Issue 27, Pages 9366-9372Publisher
ROYAL SOC CHEMISTRY
DOI: 10.1039/d0tc01479f
Keywords
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Funding
- NSFC [51762011, 51801041]
- Guangxi Natural Science Foundation [2016GXNSFAA380040, 2017GXNSFAA198353, 2017JJB150085]
- Fujian NSF [2015J01068]
- Excellent Graduate Thesis Cultivation Project of GUET [17YJPYSS34]
- Guangxi Scholarship Fund of GED
- Guangxi Collaborative Innovation Centre of Structure and Property for New Energy and Materials
- Bagui Scholars Program of Guangxi
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Defect engineering of graphitic carbon nitride (CN) has been proved to enable the alignment of energy levels for enhanced photocatalytic H(2)evolution (PHE). As the majority of defects in imperfect structured CN, native defects are critical but their role in PHE still lacks in-depth understanding. In this work, nitrogen vacancy, hydroxyl or nitrogen vacancy and hydroxyl co-modified CN was prepared by thermodynamic atmosphere control of the polymerization. It was found that the hydrogen production rate of nitrogen vacancy and hydroxyl co-modified CN is about 2253.6 mu mol h(-1)g(-1), about 3.0 times the PHE rate of either nitrogen vacancy or hydroxyl modified CN. Further transient photocurrent, electrochemical impedance spectroscopy and transient PL characterization confirmed the enhanced photogenerated electron-hole separation by the synergetic effects of the two defects in co-modified CN. In combination with density functional theory calculations, we revealed that co-modification of nitrogen vacancy and hydroxyl introduced gap states in the vicinity of the VBM and CBM of the host material, respectively, while deep trap states can be formed for CN modified by a single-type defect of nitrogen vacancy or hydroxyl.
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