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ISSN 1000-6818CN 11-1892/O6CODEN WHXUEU
Acta Phys Chim Sin >> 2017,Vol.33>> Issue(3)>> 611-619     doi: 10.3866/PKU.WHXB201611102         中文摘要
Influence of Solvothermal Post-Treatment on Photochemical Nitrogen Conversion to Ammonia with g-C3N4 Catalyst
BAI Jin, CHEN Xin, XI Zhao-Yi, WANG Xiang, LI Qiang, HU Shao-Zheng
College of Chemistry, Chemical Engineering, and Environmental Engineering, Liaoning Shihua University, Fushun 113001, Liaoning Province, P. R. China
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In this work, graphitic carbon nitride (g-C3N4) with large surface area and many nitrogen vacancies was synthesized by introducing ionic liquid[Bmim]Br as a solvent into the solvothermal post-treatment. X-ray diffraction (XRD), N2 adsorption, scanning electron microscopy (SEM), UV-Vis spectroscopy, X-ray photoelectron spectroscopy (XPS), electron paramagnetic resonance (EPR), temperature-programmed desorption of N2 (N2-TPD), and photoluminescence (PL) spectroscopy were used to characterize the prepared catalysts. The morphology of the as-prepared g-C3N4 was markedly changed from an orderless layered structure to nanoparticles with a uniform size distribution of around 30-40 nm after the introduction of[Bmim]Br, leading an increase in surface area from 8.6 to 37.9 m2·g-1. N2-TPD, photoluminescence spectra, and density functional theory (DFT) simulations indicated that the nitrogen vacancies not only trapped the photogenerated electrons to enhance their separation rate, but also served as active sites for the adsorption and activation of N2 molecules. The increased surface area of the as-prepared g-C3N4 meant that more nitrogen vacancies were exposed on the surface, leading to a markedly promoted nitrogen photofixation ability. The possible reaction mechanism is proposed.



Keywords: Graphitic carbon nitride   Ionic liquid   [Bmim]Br   Nitrogen photofixation  
Received: 2016-09-23 Accepted: 2016-11-10 Publication Date (Web): 2016-11-10
Corresponding Authors: HU Shao-Zheng Email: hushaozhenglnpu@163.com

Fund: The project was supported by the National Natural Science Foundation of China (41571464);Education Department of Liaoning Province,China (L2014145);and Natural Science Foundation of Liaoning Province,China (201602467)

Cite this article: BAI Jin, CHEN Xin, XI Zhao-Yi, WANG Xiang, LI Qiang, HU Shao-Zheng. Influence of Solvothermal Post-Treatment on Photochemical Nitrogen Conversion to Ammonia with g-C3N4 Catalyst[J]. Acta Phys. -Chim. Sin., 2017,33 (3): 611-619.    doi: 10.3866/PKU.WHXB201611102

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57. ZHU Guang-Lai, WU Guo-Zhong, CUI Zhi-Feng, XU Xin-Sheng.Transient Absorption Spectroscopy of the Effects of the Ionic Liquid [bmim][BF4] on the Photochemical Reactions of Benzil[J]. Acta Phys. -Chim. Sin., 2011,27(04): 971-976
58. ZHANG Qi-Bo, HUA Yi-Xin.Effect of Alkylimidazolium Ionic Liquids on the Corrosion Inhibition of Copper in Sulfuric Acid Solution[J]. Acta Phys. -Chim. Sin., 2011,27(03): 655-663
59. CUI Wen-Yu, AN Mao-Zhong, YANG Pei-Xia, ZHANG Jin-Qiu.Cathodic and Thermal Stabilities of the P(VdF-HFP)-Based Ionic Liquid Composite Polymer Electrolyte[J]. Acta Phys. -Chim. Sin., 2011,27(01): 78-84
60. ZHANG Qi-Bo, HUA Yi-Xin.Effect of the Ionic Liquid Additive-[BMIM]HSO4 on the Kinetics of Oxygen Evolution during Zinc Electrowinning[J]. Acta Phys. -Chim. Sin., 2011,27(01): 149-155
61. ZHANG Li-Qun, LI Hao-Ran.Progress of Investigations on Structures and Interactions of Ionic Liquids by Infrared Spectroscopy and Raman Spectroscopy[J]. Acta Phys. -Chim. Sin., 2010,26(11): 2877-2889
62. PAN Shan-Fei, HU Gui-Xiang, LV Yang, ZOU Jian-Wei, YU Qing-Sen.QSPRModel Analysis on the Solubility of Organic Compounds in Ionic Liquids[J]. Acta Phys. -Chim. Sin., 2010,26(09): 2494-2502
63. CAO Hai, JIANG Jian, ZHU Xue-Feng, DUAN Peng-Fei, LIU Ming-Hua.Interfacial Assembly of Diethyl Ester Glutamic Acid Terminated Bolaamphiphile at the Air/Water Interface: Chiral Interaction and Morphology[J]. Acta Phys. -Chim. Sin., 2010,26(07): 1842-1846
64. LIU Qing-Shan, YANG Miao, TAN Zhi-Cheng, WELZ-BIERMANN Urs.Estimation and Prediction of the Physicochemical Properties of Imidazolium-Based Ionic Liquids[J]. Acta Phys. -Chim. Sin., 2010,26(06): 1463-1467
65. LIANG Rui, YANG Mei-Rong, ZHOU Qing-Xiang.Thermal Stability, Equilibrium Vapor Pressure and Standard Enthalpy of Vaporization of 1-Butyl-3-methylimidazolium Tetrafluoroborate[J]. Acta Phys. -Chim. Sin., 2010,26(06): 1468-1472
66. ZHAO Di, HUANG Qing, JIN Xian-Bo, WEI Xian-Jun, CHEN George Z..Capacitance at the Electrode/Ionic Liquid Interface[J]. Acta Phys. -Chim. Sin., 2010,26(05): 1239-1248
67. LI Xue-Liang, CHEN Jie-Jie, LUO Mei, CHEN Xiang-Ying, LI Pei-Pei.Quantum Chemical Calculation of Hydroxyalkyl Ammonium Functionalized Ionic Liquids for Absorbing SO2[J]. Acta Phys. -Chim. Sin., 2010,26(05): 1364-1372
68. CUI Wen-Yu, AN Mao-Zhong, YANG Pei-Xia.Preparation of an Ionic Liquid Gel Polymer Electrolyte and Its Compatibility with a LiFePO4 Cathode[J]. Acta Phys. -Chim. Sin., 2010,26(05): 1233-1238
69. WANG Wei, LV Rong, YU An-Chi.Low Frequency Spectrumof Ionic Liquid [bmim][PF6] Studied by Femtosecond Optically Heterodyne-Detected Optical Kerr Effect Spectroscopy and Low Frequency Raman Spectroscopy[J]. Acta Phys. -Chim. Sin., 2010,26(04): 964-970
70. YUAN Li-Yong, PENG Jing, LI Jiu-Qiang, ZHAI Mao-Lin.Radiation-Induced Changes of Phase Behavior and Fluorescence Properties of the Ionic Liquids [C4mim][PF6] and [C4mim][NTf2][J]. Acta Phys. -Chim. Sin., 2010,26(04): 981-987
71. YUAN Xiao, LOU Shu-Jie, KOU Yuan.Ionic Liquid and Water: Making Nanoparticle Catalysis More Efficient and Greener[J]. Acta Phys. -Chim. Sin., 2010,26(04): 908-914
72. WANG Wei-Bin, YIN Jian-Zhong, SUN Li-Hua, FENG En-Min.Molecular Dynamics Simulation of Thermodynamic Properties for CO2/Ionic Liquid Systems[J]. Acta Phys. -Chim. Sin., 2009,25(11): 2291-2295
73. WU Yang, ZHANG Tian-Tian, YU Ning.Interaction between 1-Ethyl-3-Methyl-Imidazolium Cation and Asparagine Anion[J]. Acta Phys. -Chim. Sin., 2009,25(08): 1689-1696
74. ZHAI Cui-Ping, LIU Xue-Jun, ZHAO Yang, WANG Jian-Ji.NMR Study on the Aggregation of [C4mim][BF4] in D2O and CDCl3[J]. Acta Phys. -Chim. Sin., 2009,25(06): 1185-1189
75. YAN Chao-Qun, WAN Hui, GUAN Guo-Feng.Prediction of Melting Points for 1,3-Disubstituent Imidazolium Ionic Liquids[J]. Acta Phys. -Chim. Sin., 2008,24(12): 2198-2202
76. WANG Xiao-Lu; WAN Hui; GUAN Guo-Feng.Structure and Interaction of Ion-Pairs of [EPy]Cl and [EPy]Br in Gas and Liquid Phases[J]. Acta Phys. -Chim. Sin., 2008,24(11): 2077-2082
77. YANG Pei-Xia; AN Mao-Zhong; SU Cai-Na; WANG Fu-Ping.Electrodeposition Behaviors of Pure Cobalt in Ionic Liquid[J]. Acta Phys. -Chim. Sin., 2008,24(11): 2032-2036
78. ZHENG Yong-Jun; ELI Wumanjiang.Phase Behavior of Tween80/BmimPF6/Alcohol/Toluene Systems[J]. Acta Phys. -Chim. Sin., 2008,24(11): 2143-2148
79. ZHANG Xu-Zhi; JIAO Kui.Single-Walled Carbon Nanotubes and RoomTemperature Ionic Liquid Composite Film Modified Electrode[J]. Acta Phys. -Chim. Sin., 2008,24(08): 1439-1444
80. GAO Li-Xia; WANG Li-Na; QI Tao; LI Yu-Ping; CHU Jing-Long; QU Jing-Kui.Electrodeposition of Aluminium from AlCl3/Et3NHCl Ionic Liquids[J]. Acta Phys. -Chim. Sin., 2008,24(06): 939-944
81. LI Wei; RONG Hua; WU Xin-Min; CHEN Zhong-Yuan.Microwave Synthesis, Characterization and Theoretical Study of para-Toluenesulfonic Acid Threonine Salt and Its Ester Derivatives[J]. Acta Phys. -Chim. Sin., 2008,24(05): 868-872
82. SUN Guo-Hua; LI Kai-Xi; FAN Hui; GU Jian-Yu; LI Qiang; LIU Yue.Eelectrochemical Performance of Capacitors Using [BMIm]BF4/Fc as Electrolyte[J]. Acta Phys. -Chim. Sin., 2008,24(01): 103-108
83. MA Chun-An; WANG Xiao-Juan; LI Guo-Hua; LI Mei-Chao; CHEN Song.Electroreduction Characteristics of Nitromethane in Ionic Liquid BMImBF4[J]. Acta Phys. -Chim. Sin., 2007,23(11): 1719-1722
84. ARSLAN Hakan; DEMIRCAN Aydin.Structure and Vibrational Spectra of Tert-butyl N-(2-bromocyclohex-2-enyl)-N-(2-furylmethyl)carbamate[J]. Acta Phys. -Chim. Sin., 2007,23(11): 1683-1690
85. LEI Sheng; ZHANG Jing; HUANG Jian-Bin.Promotion of the Surface Activity and Aggregation Ability of Sodium Dodecylsulfate in Aqueous Solution by Ionic Liquid 1-butyl-3-methyl-imidazolium Tetrafluoroborate[J]. Acta Phys. -Chim. Sin., 2007,23(11): 1657-1661
86. WANG Jin-Bo; MING Fang-Yong; JIANG Wei-Dong; FAN Guang-Yin; LIU De-Rong; CHEN Hua; LI Xian-Jun.Asymmetric Hydrogenation of Acetophenone and Its Derivatives Catalyzed by Ruthenium Nanoparticles in Ionic Liquid Media[J]. Acta Phys. -Chim. Sin., 2007,23(09): 1381-1386
87. SUN Wei; GAO Rui-Fang; WANG Dan-Dan; JIAO Kui.Direct Electrochemistry of Hemoglobin at Room Temperature Ionic Liquid [BMIM]PF6 Modified Carbon Paste Electrode[J]. Acta Phys. -Chim. Sin., 2007,23(08): 1247-1251
88. YAN Zhi-Ying; WU Li-Yan; SUN Gui-Xiang; ZHANG Ning; ZHENG Wen-Jun.Structural Characterization of Nanocrystalline TiO2 fromIonic Liquid-Water Solvent Mixture and Its Photocatalytic Activity[J]. Acta Phys. -Chim. Sin., 2007,23(07): 1032-1036
89. LI Shu; LIU Lei; CAO Zhen; WANG Ji-Qiang; YAN Tian-Ying.Molecular Dynamics Simulation on a Eutectic Systemof LiTFSI/Urea[J]. Acta Phys. -Chim. Sin., 2007,23(07): 983-986
90. MA Chun-An; CHEN Song; CHU You-Qun; MAO Xin-Biao.Electrochemical Reduction of Nitrobenzene in Ionic Liquid BMimBF4-H2O[J]. Acta Phys. -Chim. Sin., 2007,23(04): 575-580
91. LIN Qi;FU Hai-Yan;YUAN Mao-Lin;CHEN Hua;LI Xian-Jun.Carbonylation of Aryl Halide Catalyzed by Active-carbon Supported Ionic Liquid-phase Palladium Catalyst[J]. Acta Phys. -Chim. Sin., 2006,22(10): 1272-1276
92. LI Xue-Hui;JIANG Yan-Bin;ZHANG Lei;LI Rong.Synthesis and Characterization of N-ester Appended Pyridine Task-specific Ionic Liquids[J]. Acta Phys. -Chim. Sin., 2006,22(06): 747-751
93. Ding Yun-Sheng;Wang Seng-Shan;Zha Min;Wang Zhi-Gang.Adsorption and Aggregative Structures of an Organic Cation [C18mim] of the Ionic Liquid in the Interlayer of Montmorillonite[J]. Acta Phys. -Chim. Sin., 2006,22(05): 548-551
94. LI Xue-Hui;ZHANG Lei;WANG Le-Fu;TANG Ying-Biao.Characterization of N-carboxyl Appended Pyridine Task-Specific Ionic Liquids[J]. Acta Phys. -Chim. Sin., 2006,22(04): 430-435
95. LIN Qi;FU Hai-Yan;XUE Fang;YUAN Mao-Lin;CHEN Hua;LI Xian-Jun.Hydroformylation of Long-chain Olefins Catalyzed by Rhodium-Phosphine Complexes in New Ionic Liquids[J]. Acta Phys. -Chim. Sin., 2006,22(04): 465-469
96. ZHAI Cui-Ping;WANG Jian-Ji;XUAN Xiao-Peng;WANG Han-Qing.NMR Study on the Interactions of Ionic Liquid with Acetone[J]. Acta Phys. -Chim. Sin., 2006,22(04): 456-459
97. GENG Wei-guo; LI Xue-hui; WANG Le-fu; DUAN Hong-li; PAN Wei-ping.Acidic Characterization of Polycarboxyl Imidazolium Ionic Liquids[J]. Acta Phys. -Chim. Sin., 2006,22(02): 230-233
98. TONG Jing; ZHANG Qing-guo; HONG Mei; YANG Jia-zhen.Thermodynamic Properties of Ionic Liquid BMIAlCl4[J]. Acta Phys. -Chim. Sin., 2006,22(01): 71-75
99. WU Xiao-ping; LIU Zhi-ping; WANG Wen-chuan.Molecular Dynamics Simulation of Gas Solubility in Room Temperature Ionic Liquids[J]. Acta Phys. -Chim. Sin., 2005,21(10): 1138-1142
100. WU Xiao-ping; LIU Zhi-ping.Computer Simulation Study of the Mixtures of Room Temperature Ionic Liquid [bmim][BF4] and Water[J]. Acta Phys. -Chim. Sin., 2005,21(09): 1036-1041
101. CAO Jie-ming; WANG Jun; FANG Bao-qing; ZHENG Ming-bo; LU Hong-xia; CHANG Xin; WANG Hai-yan.Synthesis and Characterization of ZnO Nanomaterials with Different Morphologies in Ionic Liquids[J]. Acta Phys. -Chim. Sin., 2005,21(06): 668-672
102. PAN Xu; DAI Song-yuan; WANG Kong-jia; SHI Cheng-wu; GUO Li.Development and Application of Electrolyte based on Ionic Liquid in Dye-sensitized Solar Cells[J]. Acta Phys. -Chim. Sin., 2005,21(06): 697-702
103. WANG Yong; LI Hao-Ran; WU Tao; WANG Cong-Min; HAN Shi-Jun.Reaction Mechanism Study for the Synthesis of Alkylimidazolium-based Halide Ionic Liquids[J]. Acta Phys. -Chim. Sin., 2005,21(05): 517-522
104. WANG Xiao-Hua; TAO Guo-Hong; WU Xiao-Mu; KOU Yuan.Investigation of the Acidity of Ionic Liquids by IR Spectroscopy[J]. Acta Phys. -Chim. Sin., 2005,21(05): 528-533
105. PU Min; CHEN Biao-Hua; LI Hui-Ying; LIU Kun-Hui.DFT Studies on Reaction Mechanism of the Double Bond Isomerization of Butene Catalyzed by 1-ethyl-3-methyl-imidazolium of the Ionic Liquid (II)[J]. Acta Phys. -Chim. Sin., 2005,21(04): 383-387
106. Li Xue-Hui; Zhang Lei; Li Qiong; Geng Wei-Guo; Ye Yu-Jia; Wang Le-Fu.TGA-FTIR Study of 1-n-butyl-3-methylimidazolium Bromide Ionic Liquid[J]. Acta Phys. -Chim. Sin., 2004,20(12): 1465-1468
107. Zhang Zhi-Heng; Guan Wei; Yang Jia-Zhen; Tan Zhi-Cheng; Sun Li-Xian.The Standard Molar Enthalpy of Formation of Room Temperature Ionic Liquid EMIES[J]. Acta Phys. -Chim. Sin., 2004,20(12): 1469-1471
108. Piao Ling-Yu;Han Yang;Kou Yuan.The Reuse of Acidic Ionic Liquids as Catalysts in Diphenyl Oxide Alkylation with Dodecene[J]. Acta Phys. -Chim. Sin., 2004,20(09): 1083-1088
109. Pu Min;Liu Kun-Hui;Li Hui-Ying;Chen Biao-Hua.DFT Studies on Reaction Mechanism of the Double Bond Isomerization of Butene Catalyzed by 1-ethyl-3-methyl-lmidazolium of the Ionic Liquid[J]. Acta Phys. -Chim. Sin., 2004,20(08): 826-830
110. Zhang Sheng-Mao;Zhang Chun-Li;Zhang Jing-Wei;Zhang Zhi-Jun;Dang Hong-Xin;Wu Zhi-Shen;Liu Wei-Min.Preparation of Silver Nanoparticles in Room Temperature Ionic Liquids[J]. Acta Phys. -Chim. Sin., 2004,20(05): 554-556
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