多孔化改性对g-C_3N_4/CdS复合光催化剂制备及光催化活性的影响
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摘要
以三聚氰胺盐酸盐为前驱体,用高温缩聚方法制备多孔化改性的类石墨相氮化碳(pg-C_3N_4)材料;用水热法制备CdS纳米中空微球,用沉积法将pg-C_3N_4与CdS有效复合,制备pg-C_3N_4/CdS复合光催化剂;用X射线衍射(XRD)、透射电子显微镜(TEM)、Fourier变换红外光谱(FTIR)、紫外可见光谱(UV-Vis)、荧光光谱及电化学阻抗谱对样品进行表征;用可见光催化降解染料罗丹明B(RhB)对其光催化活性进行评价,并给出pg-C_3N_4/CdS光催化降解RhB的机理.结果表明:石墨相氮化碳(g-C_3N_4)的多孔化改性有利于其与CdS间形成紧密界面,进而促进pg-C_3N_4/CdS光生电子-空穴的分离和传递,有效提高了其光催化活性和稳定性.
A porous modified graphite-like phase carbon nitride(pg-C_3N_4)material was prepared by a high temperature condensation polymerization method using melamine hydrochloride as a precursor.The CdS nano-hollow microspheres were prepared by a hydrothermal method,and the pg-C_3N_4 and CdS were effectively combined by deposition method to prepare pg-C_3N_4/CdS composite photocatalyst.The samples were characterized by X-ray diffraction(XRD),transmission electron microscopy(TEM),Fourier transform infrared spectroscopy(FTIR),ultraviolet-visible spectroscopy(UV-Vis),fluorescence spectrum and electrochemical impedance spectroscopy.The photocatalytic activity was evaluated by the photocatalytic degradation of dye Rhodamine B(RhB)under the visible light,and the mechanism of photocatalytic degradation of RhB was given.The results show that the porous modification of graphite-like phase carbon nitride(g-C_3N_4)is beneficial to the formation of intimate interface between pg-C_3N_4 with CdS,and then it promotes the separation and transmission of photogenerated electron-hole of pg-C_3N_4/CdS,and effectively improves its photocatalytic activity and stability.
A porous modified graphite-like phase carbon nitride(pg-C_3N_4)material was prepared by a high temperature condensation polymerization method using melamine hydrochloride as a precursor.The CdS nano-hollow microspheres were prepared by a hydrothermal method,and the pg-C_3N_4 and CdS were effectively combined by deposition method to prepare pg-C_3N_4/CdS composite photocatalyst.The samples were characterized by X-ray diffraction(XRD),transmission electron microscopy(TEM),Fourier transform infrared spectroscopy(FTIR),ultraviolet-visible spectroscopy(UV-Vis),fluorescence spectrum and electrochemical impedance spectroscopy.The photocatalytic activity was evaluated by the photocatalytic degradation of dye Rhodamine B(RhB)under the visible light,and the mechanism of photocatalytic degradation of RhB was given.The results show that the porous modification of graphite-like phase carbon nitride(g-C_3N_4)is beneficial to the formation of intimate interface between pg-C_3N_4 with CdS,and then it promotes the separation and transmission of photogenerated electron-hole of pg-C_3N_4/CdS,and effectively improves its photocatalytic activity and stability.
引文
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[2]LAKHI K S,PARK D H,AL-BAHILY K,et al.Mesoporous Carbon Nitrides:Synthesis,Functionalization,and Applications[J].Chem Soc Rev,2017,46(1):72-101.
[3]KOFUJI Y,ISOBE Y,SHIRAISHI Y,et al.Carbon Nitride-Aromatic Diimide-Graphene Nanohybrids:MetalFree Photocatalysts for Solar-to-Hydrogen Peroxide Energy Conversion with 0.2%Efficiency[J].J Am Chem Soc,2016,138(31):10019-10025.
[4]SUN Lu,YANG Meijia,HUANG Jianfeng,et al.Freestanding Graphitic Carbon Nitride Photonic Crystalsfor Enhanced Potocatalysis[J].Adv Funct Mater,2016,26(27):4943-4950.
[5]TAY Q L,KANHERE P,NG C F,et al.Defect Engineered g-C3N4for Efficient Visible Light Photocatalytic Hydrogen Production[J].Chem Mater,2015,27(14):4930-4933.
[6]ZHAO Zaiwang,SUN Yanjuan,DONG Fan.Graphitic Carbon Nitride Based Nanocomposites:A Review[J].Nanoscale,2015,7(1):15-37.
[7]TIAN Liang,LI Junyi,LIANG Feng,et al.Molten Salt Synthesis of Tetragonal Carbon Nitride Hollow Tubes and Their Application for Removal of Pollutants from Wastewater[J].Appl Catal B,2018,225:307-313.
[8]SUYANA P,GANGULY P,NAIR B N,et al.Co3O4-C3N4 p-n Nano-heterojunctions for the Simultaneous Degradation of a Mixture of Pollutants under Solar Irradiation[J].Environ Sci:Nano,2017,4(1):212-221.
[9]SHEVLIN S A,GUO Zhengxiao.Anionic Dopants for Improved Optical Absorption and Enhanced Photocatalytic Hydrogen Production in Graphitic Carbon Nitride[J].Chem Mater,2016,28(20):7250-7256.
[10]MUNOZ-BATISTA M J,FONTELLES-CARCELLER O,FERRER M,et al.Disinfection Capability of Ag/g-C3N4 Composite Photocatalysts under UV and Visible Light Illumination[J].Appl Catal B,2016,183:86-95.
[11]ZHAO Dan,YANG Chunfeng.Recent Advances in the TiO2/CdS Nanocomposite Used for Photocatalytic Hydrogen Production and Quantum-Dot-Sensitized Solar Cells[J].Renewable Sustainable Energy Rev,2016,54:1048-1059.
[12]ZHAO Qi,ZHANG Bo,YAO Weifeng,et al.Synthesis and Photocatalytic Activity of Hollow CdS Microspheres[J].Catal Sci&Technol,2016,6(24):8474-8481.
[13]LI Qin,GUO Beidou,YU Jiaguo,et al.Highly Efficient Visible-Light-Driven Photocatalytic Hydrogen Production of CdS-Cluster-Decorated Graphene Nanosheets[J].J Am Chem Soc,2011,133(28):10878-10884.
[14]LU Meiliang,PEI Zengxia,WENG Sunxian,et al.Constructing Atomic Layer g-C3N4-CdS Nanoheterojunctions with Efficiently Enhanced Visible Light Photocatalytic Activity[J].Phys Chem Chem Phys,2014,16(39):21280-21288.
[15]LIU Yong,YAN Kai,ZHANG Jingdong.Graphitic Carbon Nitride Sensitized with CdS Quantum Dots for Visible-Light-Driven Photoelectrochemical Aptasensing of Tetracycline[J].Acs Appl Mater Interfaces,2015,8(42):28255-28264.
[16]赵瑞,李明,李雪飞.纳米片层结构石墨相氮化碳的光催化活性及循环利用[J].吉林大学学报(理学版),2017,55(4):1001-1004.(ZHAO Rui,LI Ming,LI Xuefei.Photocatalytic Activity and Cyclic Utilization of Nano Lamellar Structure of Graphite Carbon Nitride[J].Journal of Jilin University(Science Edition),2017,55(4):1001-1004.)
[17]LIU Ying,YU Yuxiang,ZHANG Weide.Carbon Quantum Dots-Doped CdS Microspheres with Enhanced Photocatalytic Performance[J].J Alloy Compd,2013,569(9):102-110.
[18]FU Jie,CHANG Binbin,TIAN Yanlong,et al.Novel C3N4-CdS Composite Photocatalysts with OrganicInorganic Heterojunctions:in situ Synthesis,Exceptional Activity,High Stability and Photocatalytic Mechanism[J].J Mater Chem A,2013,1(9):3083-3090.
[19]喻胜飞,肖祎,汪艮艮,等.粉煤灰/壳聚糖复合材料的制备及在木材染色废水中的应用[J].林业工程学报,2016,1(6):29-33.(YU Shengfei,XIAO Yi,WANG Gengen,et al.Preparation of Fly Ash/Chitosan Composites and Its Application in the Wastewater of Wood Dyeing[J].Journal of Forestry Engineering,2016,1(6):29-33.)
[20]查艳凤,钱洁,候大寅.CS/PVP复合纳米纤维膜的制备及其表征[J].安徽工程大学学报,2015,30(2):75-79.(ZHA Yanfeng,QIAN Jie,HOU Dayan.Preparation and Performance Characterization of Electrospun the CS/PVP Nanofibrous Membrane[J].Journal of Anhui Polytechnic University,2015,30(2):75-79.)
[21]卜素芳.石墨相氮化碳的结构及其荧光特性研究[D].秦皇岛:燕山大学,2016.(BU Sufang.Study on the Structure and Photoluminescence Properties of Graphitic Carbon Nitride[D].Qinhuangdao:Yanshan University,2016.)
[22]MARTHA S,NASHIMA A,PARIDA K M.Facile Synthesis of Highly Active g-C3N4for Efficient Hydrogen Production under Visible Light[J].J Mater Chem A,2013,1(26):7816-7824.
[23]王浩,赵艺蒙,王愉雄,等.2D/1D复合材料C3N4/CdS的构筑及其光催化制氢性能研究[J].功能材料,2017,48(7):7149-7153.(WANG Hao,ZHAO Yimeng,WANG Yuxiong,et al.Construction of 2D/1D Composite C3N4/CdS Photocatalysts and Study on Photocatalytic Hydrogen Evolution Performance[J].Journal of Functional Materials,2017,48(7):7149-7153.)
[24]王克,王甫丽,薛红丹,等.CdS/石墨烯纳米复合材料的制备及其光催化性能[J].中国陶瓷,2016,52(1):26-29.(WANG Ke,WANG Fuli,XUE Hongdan,et al.Preparation and Photocatalytic Activity of CdS/Graphene Nanocomposites[J].China Ceramics,2016,52(1):26-29.)
[25]彭文毫,陈卓君.g-C3N4/CdS纳米棒复合光催化剂的制备及其光催化性能[J].合成化学,2017,25(6):498-502.(PENG Wenhao,CHEN Zhuojun.Preparation of g-C3N4/CdS Nanotube Composite Photocatalyst and Its Photocatalytic Performances[J].Chinese Journal of Synthetic Chemistry,2017,25(6):498-502.)