Enhancement of photocatalytic hydrogen evolution activity of g-C3N4 induced by structural distortion via post-fluorination treatment

Zeng, Lei1,2; Ding, Xue1; Sun, Zongzhao1; Hua, Weiming2; Song, Wulin3,4; Liu, Shuangyi1,5; Huang, Limin1

2018-07-05

10.1016/j.apcatb.2018.01.040

APPLIED CATALYSIS B-ENVIRONMENTAL   影响因子和分区

0926-3373

1873-3883

Graphic carbon nitride (g-C3N4) has recently attracted a great deal of attention for its application in solar energy conversion. The photocatalytic activities, however, suffer from fast electron-hole recombination and insufficient solar absorption of g-C3N4. Here, a modified g-C3N4 (CNF) photocatalyst, which was prepared by a simple hydrothermal treatment with dilute hydrofluoric acid (0.1 M HF), has achieved a 2.4-fold enhanced photo catalytic activity for hydrogen production under visible light irradiation compared to pristine g-C3N4. It is demonstrated that a structural distortion is introduced in the CNF sheets without the formation of C-F bonds after the hydrothermal treatment, which can effectively separate photogenerated electron-hole pairs. Interestingly, the g-C3N4 treated by oil bath reflux reaction with dilute hydrofluoric acid (CNFO) under the same reaction condition (concentration, temperature and duration) has no sign of structural distortion, and shows a decline in the photocatalytic H-2 evolution activity. This may be attributed to the enhanced localization mobility of pi electrons induced by the formation of C-F bonds after the oil bath treatment. These findings provide a better understanding on the effect of different fluorination treatments on the surface states and photocatalytic activities of g-C3N4-based materials. Additionally, this work presents a promising strategy to improve the photocatalytic H-2 evolution activity of g-C3N4 or related polymer semiconductors via microstructure engineering.

g-C3N4 Fluorination Structural distortion Photocatalytic H-2 evolution

SCI ; EI

英语

第一 ; 通讯

National Natural Science Foundation of China[21703097]

Chemistry ; Engineering

Chemistry, Physical ; Engineering, Environmental ; Engineering, Chemical

WOS:000428491000029

ELSEVIER SCIENCE BV

20181004883986

Energy conversion ; Fluorination ; Hydrofluoric acid ; Hydrogen production ; Photocatalysis ; Photocatalysts ; Solar energy

Gas Fuels:522 ; Energy Conversion Issues:525.5 ; Solar Energy and Phenomena:657.1 ; Chemical Reactions:802.2 ; Chemical Agents and Basic Industrial Chemicals:803 ; Inorganic Compounds:804.2

CHEMISTRY

Web of Science

1.Southern Univ Sci & Technol China, Dept Chem, Shenzhen 518055, Peoples R China
2.Fudan Univ, Dept Chem, Shanghai, Peoples R China
3.Huazhong Univ Sci & Technol, State Key Lab Mat Proc & Die & Mould Technol, Wuhan, Hubei, Peoples R China
4.Huazhong Univ Sci & Technol, Anal & Testing Ctr, Wuhan, Hubei, Peoples R China
5.Chinese Acad Sci, Chongqing Inst Green & Intelligent Technol, Chongqing 400714, Peoples R China

Zeng, Lei,Ding, Xue,Sun, Zongzhao,et al. Enhancement of photocatalytic hydrogen evolution activity of g-C3N4 induced by structural distortion via post-fluorination treatment[J]. APPLIED CATALYSIS B-ENVIRONMENTAL,2018,227:276-284.

Zeng, Lei.,Ding, Xue.,Sun, Zongzhao.,Hua, Weiming.,Song, Wulin.,...&Huang, Limin.(2018).Enhancement of photocatalytic hydrogen evolution activity of g-C3N4 induced by structural distortion via post-fluorination treatment.APPLIED CATALYSIS B-ENVIRONMENTAL,227,276-284.

Zeng, Lei,et al."Enhancement of photocatalytic hydrogen evolution activity of g-C3N4 induced by structural distortion via post-fluorination treatment".APPLIED CATALYSIS B-ENVIRONMENTAL 227(2018):276-284.