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Oxygen Self-doped g-C3N4 with Tunable Electronic Band Structure for Unprecedentedly Enhanced Photocatalytic Performance

Accepted version
Peer-reviewed

Type

Article

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Authors

Wei, Fangyan 
Liu, Yang 
Zhao, Heng 
Ren, Xiaoning 
Liu, Jing 

Abstract

As a fascinating conjugated polymer, graphitic carbon nitride (g-C3N4) has attracted much attention for solving the worldwide energy shortage and environmental pollution. In this work, for the first time we report oxygen self-doping of solvothermally synthesized g-C3N4 nanospheres with tunable electronic band structure via ambient air exposure for unprecedentedly enhanced photocatalytic perfromance. Various measurements, such as XPS, Mott–Schottky plots, and density functional theory (DFT) calculations reveal that such oxygen doping can tune the intrinsic electronic state and band structure of g-C3N4 via the formation of C-O-C bond. Our results show that the oxygen doping content can be controlled by the copolymerization of the precursors. As a consequence, the oxygen doped g-C3N4 shows excellent photocatalytic performance, with an RhB photodegradation rate of 0.249 min-1 and a hydrogen evolution rate of 3174 μmol h-1 g-1, >35 times and ~4 times higher than that of conventional thermally made pure g-C3N4 (0.007 min-1 and 846 μmol h-1 g-1, respectively) under visible light. Our work introduces a new route for the rational design and fabrication of doping modified g-C3N4 photocatalyst for efficient degradation of organic pollutants and H2 production.

Description

Keywords

40 Engineering, 34 Chemical Sciences, 4018 Nanotechnology, 3406 Physical Chemistry, 7 Affordable and Clean Energy

Journal Title

Nanoscale

Conference Name

Journal ISSN

2040-3364
2040-3372

Volume Title

10

Publisher

Royal Society of Chemistry
Sponsorship
Royal Academy of Engineering (RAEng) (10216/105)
Y. Li acknowledges Hubei Provincial Department of Education for the “Chutian Scholar” program. B. L. Su acknowledges the Chinese Central Government for an “Expert of the State” position in the Program of the “Thousand Talents” and a Life Membership at the Clare Hall, Cambridge and the financial support of the Department of Chemistry, University of Cambridge. T. Hasan acknowledges support from the Royal Academyof Engineering (Graphlex). This work is supported by the National Key R&D Program of China (2016YFA0202602), Program for Changjiang Scholars and Innovative Research Team in University (IRT-15R52), National Natural Science Foundation of China (U1663225, 21671155) and the Fundamental Research Funds for the Central Universities (WUT: 2016III029).