Enhanced photocatalytic H2 evolution and phenol degradation over sulfur doped meso/macroporous g-C3N4 spheres with continuous channels |
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Affiliation: | 1. MIIT Key Laboratory of Critical Materials Technology for New Energy Conversion and Storage, School of Chemistry and Chemical Engineering, Harbin Institute of Technology, Harbin 150001, China;2. Key Laboratory of Aerospace Thermophysics, Ministry of Industry and Information Technology, School of Energy Science and Engineering, Harbin Institute of Technology, Harbin 150001, China;1. College of Chemistry, Chemical Engineering and Environmental Engineering, Liaoning Shihua University, Fushun 113001, China;2. College of Chemistry, Chemical Engineering and Material Science, Shandong Normal University, Jinan 250014, China;3. State Key Laboratory of Urban Water Resource and Environment, MIIT Key Laboratory of Critical Materials Technology for New Energy Conversion and Storage, School of Chemistry and Chemical Engineering, Harbin Institute of Technology, Harbin 150080, China;1. State Key Laboratory of Materials-Oriented Chemical Engineering, College of Materials Science and Engineering, Nanjing Tech University, Nanjing 210009, PR China;2. Jiangsu Collaborative Innovation Center for Advanced Inorganic Function Composites, Nanjing Tech University, Nanjing 210009, PR China;3. Jiangsu National Synergetic Innovation Center for Advanced Materials (SICAM), Nanjing Tech University, Nanjing 210009, PR China;1. School of Petrochemical Engineering, Changzhou University, Changzhou 213164, PR China;2. School of Materials Science & Engineering, Jiangsu Collaborative Innovation Center of Photovolatic Science and Engineering, Changzhou University, Changzhou 213164, PR China;1. MIIT Key Laboratory of Critical Materials Technology for New Energy Conversion and Storage, School of Chemistry and Chemical Engineering, Harbin Institute of Technology, Harbin, 150001, China;2. Key Laboratory of Bio-based Material Science & Technology (Northeast Forestry University), Ministry of Education, Harbin, 150040, China;1. School of Chemistry and Chemical Engineering, Jiangsu University, Zhenjiang 212013, China;2. Institute for Energy Research, Jiangsu University, Zhenjiang 212013, China;1. School of Materials Science and Engineering, Tianjin University, Tianjin 300350, China;2. School of Materials Science and Engineering, Lanzhou Jiaotong University, Lanzhou 730070, China;3. School of Mechanical Engineering, Dongguan University of Technology, Dongguan 523808, China;4. College of Chemistry Engineering and Materials Science, Quanzhou Normal University, Quanzhou 362000, Fujian, China |
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Abstract: | S-doped meso/macroporous g-C3N4 spheres (SMCN) were successfully synthesized via an in situ novel method utilizing millimeter-scale porous silica spheres as template and thiourea as precursor and S source. Such SMCN possessed millimeter-scale spherical morphology with continuous channels at 20–80 nm in the interior of the spheres, and exhibited increased H2 generation rate (15 times) and phenol degradation rate (5 times) under visible light irradiation compared with that over pristine g-C3N4, mainly due to the enlarged surface area, enhanced mass transfer and improved efficiency of charges separation all stemming from the synergetic effects of the S doping and pore creating. Notably, density functional theory (DFT) calculations were employed to further understand the mechanism of the photocatalytic enhancement with regard to the optical absorption property at atomic level. Combined with the finite difference time domain (FDTD) simulations aiming at evaluating the effect of the nanoscale pore architecture on the optical absorption ability, it was revealed that not only the S doping but also the meso/macroporous structure resulted in the enhancement of the optical absorption, which was considered to be an essential role for the enhanced photocatalytic performances over SMCN. |
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Keywords: | S-doping Continuous channels FDTD simulation DFT Optical absorption |
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