SiC/C_3N_4复合材料的光催化降解亚甲基蓝性能研究
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摘要
采用冷却结晶法制备不同配比的SiC与三聚氰胺前驱体,煅烧后得到SiC/C_3N_4复合材料,研究了在白炽灯照射下复合材料对亚甲基蓝的光催化降解性能。结果表明,SiCN100型SiC/C_3N_4复合材料的光催化降解能力最强,光照150 min时亚甲基蓝的降解率达到76%,光降解反应速率常数为0.00757 min~(-1),是纯SiC的6倍,且该催化剂在循环测试中性能稳定。采用X-射线衍射(XRD)、扫描电子显微镜(SEM)、透射电子显微镜(TEM)、紫外可见-漫反射光谱(UV-Vis DRS)和光致发光光谱(PL)表征了SiC/C_3N_4复合材料,并通过活性基团捕获实验,深入分析了亚甲基蓝的光催化降解机理,发现电子在降解过程中起最关键的作用,活性基团对降解率的影响程度依次为e~->h~+>·O■。
SiC/C_3N_4 composites were obtained by calcining the precursor prepared by cooling crystallization method,and the photocatalytic degradation efficiencies of methylene blue were studied by the composites under incandescent lamp.The results showed that SiCN100 composite has the strongest photocatalytic ability,and the degradation efficiency of methylene blue reached 76%for 150 min irradiation.The photo-degradation rate constant of methylene blue was 0.00757 min~(-1 )over SiCN100,which was 6 times higher than that over pure SiC.The photocatalytic performance of the SiCN100 is stable in the cyclic test.SiC/C_3N_4 composites were characterized using X-ray diffraction(XRD),scanning electron microscope(SEM),transmission electron microscopy(TEM),UV-Vis diffuse reflectance spectroscopy(UV-Vis DRS),photoluminescence spectra(PL)and the photocatalytic degradation mechanism of methylene blue was analyzed in detail.The radicals trapping experiments revealed that electrons play an important role in the MB degradation.
SiC/C_3N_4 composites were obtained by calcining the precursor prepared by cooling crystallization method,and the photocatalytic degradation efficiencies of methylene blue were studied by the composites under incandescent lamp.The results showed that SiCN100 composite has the strongest photocatalytic ability,and the degradation efficiency of methylene blue reached 76%for 150 min irradiation.The photo-degradation rate constant of methylene blue was 0.00757 min~(-1 )over SiCN100,which was 6 times higher than that over pure SiC.The photocatalytic performance of the SiCN100 is stable in the cyclic test.SiC/C_3N_4 composites were characterized using X-ray diffraction(XRD),scanning electron microscope(SEM),transmission electron microscopy(TEM),UV-Vis diffuse reflectance spectroscopy(UV-Vis DRS),photoluminescence spectra(PL)and the photocatalytic degradation mechanism of methylene blue was analyzed in detail.The radicals trapping experiments revealed that electrons play an important role in the MB degradation.
引文
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[2]Wang X,Maeda K,Thomas A,et al.A metal-free polymeric photocatalyst for hydrogen production from water under visible light[J].Nat Mater,2009,8(1):76-80.
[3]Lin X,Xu D,Che G,et al.Construction of leaf-like g-C3N4/Ag/BiVO4 nanoheterostructures with enhanced photocatalysis performance under visible-light irradiation[J].Colloids Surfaces A,2017,513(5):117-124.
[4]Yan W,Sun J,Jiang L,et al.Electrospinning preparation of nanostructured g-C3N4/BiVO4 composite films with enhanced photoelectrochemical performance[J].Langmuir,2017,33(19):4694-4701.
[5]Ye W,Shao Y,Hu X,et al.Highly enhanced photoreductive degradation of polybromodiphenyl ethers with g-C3N4/TiO2 under visible light irradiation[J].Nanomater,2017,7(4):76.
[6]Liu Y,Wang R,Yang Z,et al.Enhanced visible-light photocatalytic activity of Z-scheme graphitic carbon nitride/oxygen vacancy-rich zinc oxide hybrid photocatalysts[J].Chin J Catal,2015,36(12):2135-2144.
[7]Xu H,Wu L,Jin L,et al.Combination mechanism and enhanced visible-light photocatalytic activity and stability of CdS/g-C3N4 heterojunctions[J].J Mater Sci Technol,2017,33(1):30-38.
[8]余童,王海飞,王春林,等.复合光催化剂CNNS/CdS QDs的一步法合成及催化性能研究[J].化学研究与应用.2017,29(12):1878-1883.
[9]王鹏飞,桂明生.WO3/g-C3N4复合催化剂的制备及其可见光光催化性能分析[J].重庆大学学报 2016,39(2):114-122.
[10]Liu S,Zhu H,Yao W,et al.One step synthesis of P-doped g-C3N4 with the enhanced visible light photocatalytic activity[J].Appl Surf Sci,2018,430:309-315.
[11]Ai B,Duan X,Sun H,et al.Metal-free graphene-carbon nitride hybrids for photodegradation of organic pollutants in water[J].Catal Today,2015,258:668-675.
[12]Min Y,Qi X F,Xu Q,et al.Enhanced reactive oxygen species on a phosphate modified C3N4/graphene photocatalyst for pollutant degradation[J].Crystengcomm,2014,16(7):1287.
[13]Yu Q,Li X,Zhang L,et al.Significantly improving the performance and dispersion morphology of porous g-C3N4/PANI composites by an interfacial polymerization method[J].E-Polymers,2015,15(2):95-101.
[14]Ge L,Han C,Liu J.In situ synthesis and enhanced visible light photocatalytic activities of novel PANI–g-C3N4 composite photocatalysts[J].J Mater Chem,2012,22(23):11843-11850.
[15]Lu W,Guo L,Jia Y,et al.Significant enhancement in photocatalytic activity of high quality SiC/graphene core-shell heterojunction with optimal structural parameters[J].RSC Advances,2014,4(87):46771-46779.
[16]Zhu K,Guo L,Lin J,et al.Graphene covered SiC powder as advanced photocatalytic material[J].Appl Phys Lett,2012,100(2):023113.
[17]Peng Y,Han G,Wang D,et al.Improved H2 evolution under visible light in heterostructured SiC/CdS photocatalyst:Effect of lattice match[J].Int J Hydrogen Energy,2017,42(21):14409-14417.
[18]Wang D,Guo Z,Peng Y,et al.A simple route to significant enhancement of photocatalytic water oxidation on BiVO4 by heterojunction with SiC[J].Chem Eng J,2015,281:102-108.
[19]Wang D,Guo Z,Peng Y,et al.Visible light induced photocatalytic overall water splitting over micro-SiC driven by the Z-scheme system[J].Catal Commun,2015,61:53-56.
[20]Wang B,Zhang J,Huang F.Enhanced visible light photocatalytic H2 evolution of metal-free g-C3N4/SiC heterostructured photocatalysts[J].Appl Surf Sci,2017,391:449-456.
[21]Xu H,Gan Z,Zhou W,et al.A metal-free 3C-SiC/g-C3N4 composite with enhanced visible light photocatalytic activity[J].RSC Adv,2017,7(63):40028-40033.
[22]Yang J,Peng Y,Yang B,et al.Enhanced photocatalytic degradation of Rhodamine B over metal-free SiC/C3N4 heterostructure under visible light irradiation[J].Mater Res Express,2018,5(8).08551.
[23]杨静静,韦莹莹,何勇平,等.SiC/BiVO4复合材料光催化降解亚甲基蓝[J].西南师范大学学报(自然科学版).2018,(5).31-36.
[24]刘乃亮,庞波,理莎莎,等.BiVO4/rGO的水热控制合成及其光催化性能研究[J].功能材料.2017,48(10):10077-10081+10088.
[25]胡育,宋连香,李琼,等.γ-Bi2MoO6光催化降解次甲基蓝的研究[J].化学研究与应用.2017,(5):706-709.
[26]Peng Y,Guo Z,Yang J,et al.Enhanced photocatalytic H2 evolution over micro-SiC by coupling with CdS under visible light irradiation[J].J Mater Chem A,2014,2(18):6296-6300.
[27]Pan C,Xu J,Wang Y,et al.Dramatic Activity of C3N4/BiPO4 Photocatalyst with core/shell structure formed by self-assembly[J].Adv Funct Mater,2012,22(7):1518-1524.
[28]Li X,Xie J,Jiang C,et al.Review on design and evaluation of environmental photocatalysts[J].Front Env Sci Eng,2018,12(5):14.
[29]Lin X,Xi Y,Zhao R,et al.Construction of C60-decorated SWCNTs(C60-CNTs)/bismuth-based oxide ternary heterostructures with enhanced photocatalytic activity[J].RSC Adv,2017,7(85):53847-53854.
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