石墨相氮化碳的制备与光催化性能
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摘要
石墨相氮化碳(g-C3N4)作为一种半导体材料,它的禁带宽度约为2.7eV,具有优异的物理和化学稳定性,并且其原料来源广泛,无毒,廉价,可以应用于产氢、降解有机染料及CO2的还原等领域。本研究以尿素为原料制备了g-C3N4,研究了热聚合温度、反应时间对制备的g-C3N4光催化降解罗丹明B性能的影响,并考察了对甲基橙、亚甲基蓝等不同染料的光催化降解效果。结果表明:石墨相氮化碳对于罗丹明B和亚甲基蓝的降解效果较好(3h之内几乎完全降解),而对于甲基橙几乎没有降解效果;随着聚合温度的提高(600℃以下),反应时间的延长(9h以内),产物的光催化降解染料的效果越好。
As a semiconductor material,graphitic carbon nitride(g-C_3N_4),its band gap is about 2.7 eV.With excellent physical and chemical stability,g-C_3N_4 has the characteristics of"earth-abundant"nature,non-toxic,cheap and can be applied to hydrogen evolution,degradation of organic dyes,CO2 reduction and other fields.In this paper,the photocatalytic degradation effect of g-C_3N_4 on different dyes has been investigated,as well as the influence of different thermal polymerization temperature and thermal insulation time on photocatalytic performance.In this paper,g-C_3N_4 was made by urea,and the effect of polymerization temperature and reaction time on the photocatalytic degradation of Rhodamine B by g-C_3N_4 was investigated.The photocatalytic degradation effects of different dyes such as methyl orange and methylene blue were also investigated.The results showed that the g-C_3N_4 had great effect on the degradation of Rhodamine B and methylene blue(almost completely degraded within 3 h),but little effect for methyl orange.With the increase of polymerization temperature(below 600 ℃)and the prolongation of the reaction time(within 9 h),the effect ofphotocatalytic degradation of the dye was better.
As a semiconductor material,graphitic carbon nitride(g-C_3N_4),its band gap is about 2.7 eV.With excellent physical and chemical stability,g-C_3N_4 has the characteristics of"earth-abundant"nature,non-toxic,cheap and can be applied to hydrogen evolution,degradation of organic dyes,CO2 reduction and other fields.In this paper,the photocatalytic degradation effect of g-C_3N_4 on different dyes has been investigated,as well as the influence of different thermal polymerization temperature and thermal insulation time on photocatalytic performance.In this paper,g-C_3N_4 was made by urea,and the effect of polymerization temperature and reaction time on the photocatalytic degradation of Rhodamine B by g-C_3N_4 was investigated.The photocatalytic degradation effects of different dyes such as methyl orange and methylene blue were also investigated.The results showed that the g-C_3N_4 had great effect on the degradation of Rhodamine B and methylene blue(almost completely degraded within 3 h),but little effect for methyl orange.With the increase of polymerization temperature(below 600 ℃)and the prolongation of the reaction time(within 9 h),the effect ofphotocatalytic degradation of the dye was better.
引文
[1]NAKATA K,FUJISHIMA A.TiO2photocatalysis:Design and applications[J].Journal of Photochemistry and Photobiology C:Photochemistry Reviews,2012,13(3):169-189.
[2]YU L,WANG Z,SHI L,et al.Photoelectrocatalytic performance of TiO2 nanoparticles incorporated TiO2nanotube arrays[J].Applied Catalysis B:Environmental,2012,(113/114)(1):318-325.
[3]KUBACKA A,FERNANDEZ-GARCIA M,COLON G.Advanced nanoarchitectures for solar photocatalytic applications[J].Chemical Reviews,2012,112(3):1555-1614.
[4]YAN S C,LI Z S,ZOU Z G.Photodegradation performance of g-C3N4fabricated by directly heating melamine[J].Langmuir,2009,25(17):10397-10401.
[5]MANIKANDAN M,TANABE T,LI P,et al.Photocatalytic water splitting under visible light by mixed-valence Sn3O4[J].ACS Applied Materials Interfaces,2014,6(6):3790-3793.
[6]TAHIR M B,NABI G,RAFIQUE M,et al.Nanostructuredbased WO3 photocatalysts:Recent development,activity enhancement,perspectives and applications for wastewater treatment[J].International Journal of Environmental Science and Technology,2017,14(11):2519-2542.
[7]QU X,YI Y,QIAO F,et al.TiO2/BiOI/CQDs:Enhanced photocatalytic properties under visible-light irradiation[J].Ceramics International,2018,44(2):1348-1355.
[8]张宇航,孙艳娟,徐瑾,等.超薄类石墨相氮化碳纳米片剥离技术的研究进展[J].武汉工程大学学报,2017,39(3):223-230.ZHANG Yuhang,SUN Yanjuan,XU Jin,et al.Research progress in exfoliation technology of ultrathin graphite carbon nitride nanosheets[J].Journal of Wuhan Institute of Technology,2017,39(3):223-230.
[9]WANG X,MAEDA K,THOMAS A,et al.A metal-free polymeric photocatalyst for hydrogen production from water under visible light[J].Nature Materials,2009,8(1):76-80.
[10]孟春雷,李镇江,刘晓珑.N-Ag/ZnO纳米复合材料的合成及模拟日光下的光催化性能[J].青岛科技大学学报(自然科学版),2015,36(3):281-285.MENG Chunlei,LI Zhenjiang,LIU Xiaolong.Synthesis and photocatalytic activity of N-doped Ag/ZnO nanocomposites[J].Journal of Qingdao University of Science and Technology(Natural Science Edition),2015,36(3):281-285.
[11]徐赞,于薛刚,张宪明,等.TiO2/g-C3N4复合物的制备及其光催化性能[J].青岛科技大学学报(自然科学版),2017,38(6):50-55.XU Zan,YU Xuegang,ZHANG Xianming,et al.Synthesis of TiO2/g-C3N4 composites with excellent visible-light driven photocatalytic performance[J].Journal of Qingdao University of Science and Technology(Natural Science Edition),2017,38(6):50-55.
[12]YANG S,GONG Y,ZHANG J,et al.Exfoliated graphitic carbon nitride nanosheets as efficient catalysts for hydrogen evolution under visible light[J].Advanced Materials,2013,25(17):2452-2456.
[13]DONG G,ZHANG L.Porous structure dependent photoreactivity of graphitic carbon nitride under visible light[J].Journal of Materials Chemistry,2012,22(3):1160-1166.
[14]JUNG H S,LEE J K,NASTASI M,et al.Enhancing photocatalytic activity by using TiO2-MgO core-shell-structured nanoparticles[J].Applied Physics Letters,2006,88(1):37.
[15]CUI Y,ZHANG J,ZHANG G,et al.Synthesis of bulk and nanoporous carbon nitride polymers from ammonium thiocyanate for photocatalytic hydrogen evolution[J].Journal of Materials Chemistry,2011,21(34):13032-13039.
[16]DONG F,WU L,SUN Y,et al.Efficient synthesis of polymeric g-C3N4layered materials as novel efficient visible light driven photocatalysts[J].Journal of Materials Chemistry,2011,21(39):15171-15174.
[17]NIU P,ZHANG L,LIU G,et al.Graphene-like carbon nitride nanosheets for improved photocatalytic activities[J].Advanced Functional Materials,2012,22(22):4763-4770.
[18]DONG S,CUI Y,WANG Y,et al.Designing three-dimensional acicular sheaf shaped BiVO4/reduced graphene oxide composites for efficient sunlight-driven photocatalytic degradation of dye wastewater[J].Chemical Engineering Journal,2014,249:102-110.
[2]YU L,WANG Z,SHI L,et al.Photoelectrocatalytic performance of TiO2 nanoparticles incorporated TiO2nanotube arrays[J].Applied Catalysis B:Environmental,2012,(113/114)(1):318-325.
[3]KUBACKA A,FERNANDEZ-GARCIA M,COLON G.Advanced nanoarchitectures for solar photocatalytic applications[J].Chemical Reviews,2012,112(3):1555-1614.
[4]YAN S C,LI Z S,ZOU Z G.Photodegradation performance of g-C3N4fabricated by directly heating melamine[J].Langmuir,2009,25(17):10397-10401.
[5]MANIKANDAN M,TANABE T,LI P,et al.Photocatalytic water splitting under visible light by mixed-valence Sn3O4[J].ACS Applied Materials Interfaces,2014,6(6):3790-3793.
[6]TAHIR M B,NABI G,RAFIQUE M,et al.Nanostructuredbased WO3 photocatalysts:Recent development,activity enhancement,perspectives and applications for wastewater treatment[J].International Journal of Environmental Science and Technology,2017,14(11):2519-2542.
[7]QU X,YI Y,QIAO F,et al.TiO2/BiOI/CQDs:Enhanced photocatalytic properties under visible-light irradiation[J].Ceramics International,2018,44(2):1348-1355.
[8]张宇航,孙艳娟,徐瑾,等.超薄类石墨相氮化碳纳米片剥离技术的研究进展[J].武汉工程大学学报,2017,39(3):223-230.ZHANG Yuhang,SUN Yanjuan,XU Jin,et al.Research progress in exfoliation technology of ultrathin graphite carbon nitride nanosheets[J].Journal of Wuhan Institute of Technology,2017,39(3):223-230.
[9]WANG X,MAEDA K,THOMAS A,et al.A metal-free polymeric photocatalyst for hydrogen production from water under visible light[J].Nature Materials,2009,8(1):76-80.
[10]孟春雷,李镇江,刘晓珑.N-Ag/ZnO纳米复合材料的合成及模拟日光下的光催化性能[J].青岛科技大学学报(自然科学版),2015,36(3):281-285.MENG Chunlei,LI Zhenjiang,LIU Xiaolong.Synthesis and photocatalytic activity of N-doped Ag/ZnO nanocomposites[J].Journal of Qingdao University of Science and Technology(Natural Science Edition),2015,36(3):281-285.
[11]徐赞,于薛刚,张宪明,等.TiO2/g-C3N4复合物的制备及其光催化性能[J].青岛科技大学学报(自然科学版),2017,38(6):50-55.XU Zan,YU Xuegang,ZHANG Xianming,et al.Synthesis of TiO2/g-C3N4 composites with excellent visible-light driven photocatalytic performance[J].Journal of Qingdao University of Science and Technology(Natural Science Edition),2017,38(6):50-55.
[12]YANG S,GONG Y,ZHANG J,et al.Exfoliated graphitic carbon nitride nanosheets as efficient catalysts for hydrogen evolution under visible light[J].Advanced Materials,2013,25(17):2452-2456.
[13]DONG G,ZHANG L.Porous structure dependent photoreactivity of graphitic carbon nitride under visible light[J].Journal of Materials Chemistry,2012,22(3):1160-1166.
[14]JUNG H S,LEE J K,NASTASI M,et al.Enhancing photocatalytic activity by using TiO2-MgO core-shell-structured nanoparticles[J].Applied Physics Letters,2006,88(1):37.
[15]CUI Y,ZHANG J,ZHANG G,et al.Synthesis of bulk and nanoporous carbon nitride polymers from ammonium thiocyanate for photocatalytic hydrogen evolution[J].Journal of Materials Chemistry,2011,21(34):13032-13039.
[16]DONG F,WU L,SUN Y,et al.Efficient synthesis of polymeric g-C3N4layered materials as novel efficient visible light driven photocatalysts[J].Journal of Materials Chemistry,2011,21(39):15171-15174.
[17]NIU P,ZHANG L,LIU G,et al.Graphene-like carbon nitride nanosheets for improved photocatalytic activities[J].Advanced Functional Materials,2012,22(22):4763-4770.
[18]DONG S,CUI Y,WANG Y,et al.Designing three-dimensional acicular sheaf shaped BiVO4/reduced graphene oxide composites for efficient sunlight-driven photocatalytic degradation of dye wastewater[J].Chemical Engineering Journal,2014,249:102-110.