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C/N Vacancy Co‐Enhanced Visible‐Light‐Driven Hydrogen Evolution of g‐C 3 N 4 Nanosheets Through Controlled He + Ion Irradiation
Author(s) -
Wang Xuening,
Wu Liang,
Wang Zhaowu,
Wu Hengyi,
Zhou Xuemei,
Ma Hongyu,
Zhong Huizhou,
Xing Zhuo,
Cai Guangxu,
Jiang Changzhong,
Ren Feng
Publication year - 2019
Publication title -
solar rrl
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 2.544
H-Index - 37
ISSN - 2367-198X
DOI - 10.1002/solr.201800298
Subject(s) - photocurrent , water splitting , materials science , photocatalysis , irradiation , visible spectrum , vacancy defect , graphitic carbon nitride , ion , absorption (acoustics) , charge carrier , hydrogen , semiconductor , fluence , density functional theory , analytical chemistry (journal) , nanotechnology , optoelectronics , crystallography , chemistry , computational chemistry , physics , catalysis , organic chemistry , nuclear physics , biochemistry , chromatography , composite material
Graphitic carbon nitride (g‐C 3 N 4 ) is reported to be a promising metal‐free semiconductor for photocatalytic water splitting. However, the performance of g‐C 3 N 4 is substantially limited by its insufficient visible‐light absorption and low photogenerated charge carrier separation efficiency. In this work, an innovative method (ion irradiation) to efficiently introduce both defined C‐ and N‐vacancies ( V C and V N ) simultaneously into g‐C 3 N 4 nanosheets are explored. Unlike traditional chemical methods, by controlling He + ion fluence, tunable vacancy concentrations are able to be obtained in g‐C 3 N 4 . Defect‐engineered g‐C 3 N 4 shows highly improved performance under optimized conditions, the defective g‐C 3 N 4 exhibits a significantly higher (2.7‐fold) hydrogen evolution rate of 1271 µmol g −1 h −1 than that of the g‐C 3 N 4 nanosheets under visible light ( λ > 420 nm) illumination. Meanwhile, the defective g‐C 3 N 4 exhibits a significantly enhanced (threefold) photocurrent density as photoanodes for photoelectrochemical (PEC) water splitting. Further characterizations show that the enhanced visible light absorption and an extended charge carrier lifetime, can be ascribed to the presence of C‐ and N‐ vacancies. These experimental results are in line with density functional theory (DFT) calculations. Therefore, the present work shows that defect‐engineering on g‐C 3 N 4 using ion irradiation technique, is an effective, controllable, and defined approach to improve the photocatalytic and PEC water splitting performance of g‐C 3 N 4 .