期刊
APPLIED CATALYSIS B-ENVIRONMENTAL
卷 241, 期 -, 页码 141-148出版社
ELSEVIER SCIENCE BV
DOI: 10.1016/j.apcatb.2018.09.023
关键词
Photocatalysis; g-C3N4; CO2 atmosphere; Hydrogen; Evolution reaction; Triazole
资金
- Ministry of Education, Culture, Sports, Science and Technology (MEXT) of Japanese Government [25220806]
- National Natural Science Foundation of China [21707052]
- China Postdoctoral Science Foundation [2016M601718]
- Key Research and Development Program of Jiangsu Province [BE2017623]
- Fundamental Research Funds for the Central Universities [JUSRP51714B]
Gaseous atmosphere during graphitic carbon nitride (g-C3N4) preparation can have a significant influence on modifying the morphological texture, polymeric structure, charge carrier behavior, and consequently the photocatalytic performance. Herein, we developed a new one-step method to fabricate g-C3N4 through direct pyrolysis of 3-amino-1,2,4-triazole in CO2 atmosphere (C3N4-T-CO2) with no additive. Surprisingly, the H-2 production activity of C3N4-T-CO2 photocatalyst under visible light irradiation was 2.4 and 1.7 times as high as that of g-C3N4 obtained under air and N-2 atmosphere with the same heating process, respectively. Detailed characterizations indicated that the CO2 calcination atmosphere induced less nitrogen vacancies with no charge transport ability, more NHx groups, and faster rate of the electron transport between heptazine rings for C3N4-TCO2 among three samples. It is also suggested that the larger number of NHx in C3N4-T-CO2 could enhance the interlayer electron transport through the hydrogen-bonding interaction between C3N4 layers. Time-resolved photoluminescence, single-particle fluorescence, and femtosecond time-resolved transient absorption measurements were performed to elucidate the efficient charge transfer and trapping processes in C3N4-T-CO2. For the first time, such unprecedented effect of CO2 calcination atmosphere was observed for g-C3N4. This work not only presents a promising strategy in designing highly effective g-C3N4 photocatalyst for solar energy conversion, but also makes an insight into the charge transfer process in g-C3N4 photocatalyst.
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