One-step preparation of halogenated aminobenzonitrile modified g-C3N4 via copolymerization and in situ halogen doping for highly enhanced visible light hydrogen evolution |
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| Affiliation: | 1. Department of Chemistry for Materials, Graduate School of Engineering, Mie University, Tsu Mie 514-8507, Japan;2. Global Environment Center for Education & Research, Mie University, Tsu Mie 5148507, Japan;1. Institute of Green Chemistry and Chemical Technology, School of Chemistry and Chemical Engineering, Jiangsu University, Zhenjiang 212013, China;2. School of Materials and Engineering, Jiangsu University of Science and Technology, Zhenjiang 212003, China;1. Key Laboratory for Green Chemical Technology of the Ministry of Education, School of Chemical Engineering and Technology, Tianjin University, Tianjin 300072, China;2. Collaborative Innovative Center of Chemical Science and Engineering (Tianjin), Tianjin 300072, China;1. Key Laboratory of Enhanced Heat Transfer and Energy Conservation, The Ministry of Education, School of Chemistry and Chemical Engineering, South China University of Technology, Guangzhou, 510640, China;2. Guangdong Engineering Technology Research Center of Efficient Heat Storage and Application, South China University of Technology, Guangzhou, 510640, China;3. Key Lab Fuel Cell Technology Guangdong Province, School of Chemistry and Chemical Engineering, South China University of Technology, Guangzhou, 510640, China;1. International Research Center for Renewable Energy (IRCRE), State Key Laboratory of Multiphase Flow in Power Engineering (MFPE), Xi’an Jiaotong University (XJTU), 28 West Xianning Road, Xi’an 710049, China;2. Institute of Energy Research, Jiangxi Academy of Sciences, No. 7777 Changdong Avenue, Nanchang 330096, China;3. State Key Laboratory for Physical Chemistry of Solid Surfaces, Collaborative Innovation Center of Chemistry for Energy Materials, National & Local Joint Engineering Research Center for Preparation Technology of Nanomaterials and National Engineering Laboratory for Green Chemical Productions of Alcohols–Ethers–Esters, College of Chemistry and Chemical Engineering, Xiamen University, 422 Siming South Road, Xiamen 361005, China |
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| Abstract: | A series of halogenated aminobenzonitrile modified graphitic carbon nitride (g-C3N4) was prepared by a one-step calcination of dicyandiamide and 2-amino-5-halogen-benzonitriles (X-ABN, X = F, Cl, Br or I, 1.67 wt% of dicyandiamide) together, and named as X-ABN-CN. The resulting X-ABN-CN photocatalysts were characterized by X-ray diffraction, transmission electron microscopy, Fourier transform infrared spectroscopy, X-ray photoelectron spectroscopy, ultraviolet–visible diffuse reflection spectroscopy, and photoluminescence spectroscopy. The characterization results indicated that X-ABN-CN have been successfully prepared, and the π-conjugated system and electronic structure of X-ABN-CN could be improved via copolymerization, Ullmann reaction and in situ halogen doping. Under visible light irradiation (λ > 400 nm), the photocatalytic activity of X-ABN-CN were much higher than that of pure g-C3N4 and increase with the increase of halogen atomic number. The hydrogen evolution rate of I-ABN-CN (131.4 μmol h−1) was 7.4 times that of g-C3N4 (17.7 μmol h−1). Furthermore, the corresponding mesoporous X-ABN-CN (X-ABN-MCN, X = F, Cl, Br or I) were prepared by using SiO2 nanoparticles as template. As expected, I-ABN-MCN showed the highest photocatalytic activity in all mesoporous samples, which is about 8.8 times that of g-C3N4. The results manifest that the copolymerization, Ullmann reaction, in situ halogen doping and mesoporous structure could be integrated together to modify g-C3N4 by a simple one-step calcination process. |
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| Keywords: | Halogenated aminobenzonitrile Copolymerization In situ doping Photocatalytic hydrogen evolution |
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