AuCo/水滑石复合氧化物的制备及其光催化性能
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摘要
采用浸渍-还原方法将不同比例的金钴(Au、Co)负载到锌铝水滑石(AuCo/ZnAl-LDHs)表面,经焙烧得到具有较高光催化性能的复合氧化物(AuCo/ZnAl-LDO),借助X射线粉末衍射、透射电子显微镜和紫外-可见漫反射光谱技术对样品的晶体结构、表面形貌和光吸收特性进行表征,并考察了材料对邻苯二酚光催化降解性能。实验表明:Au、Co总负载量为2%时,n(Au)/n(Co)摩尔比为5:1,焙烧温度为400℃的光催化剂对邻苯二酚的降解表现出的最佳的性能,5 h对邻苯二酚的降解率达到了94.7%。
Gold and cobalt were loaded on the surface of zinc-aluminum layered double hydroxides at different ratios via an impregnation-reduction process.The composites mental oxides as a high photocatalytic material were derived from AuCo/ZnAl-LDHs after calcination.The crystal structure, morphology and optical performance of samples were characterized by X-ray diffraction, transmission electron microscopy and ultraviolet-visible diffuse-reflectance spectroscopy, respectively.The photocatalytic activities were evaluated via the degradation of catechol under visible light irradiation.The results show that the photocatalyst with a total loading mass of Au/Co of 2% and Au:Co molar ratio of 5:1, calcined at 400 ℃ has an optimum degradation efficiency of catechol.In this case, 94.7% of catechol can be degraded at 5 h.
Gold and cobalt were loaded on the surface of zinc-aluminum layered double hydroxides at different ratios via an impregnation-reduction process.The composites mental oxides as a high photocatalytic material were derived from AuCo/ZnAl-LDHs after calcination.The crystal structure, morphology and optical performance of samples were characterized by X-ray diffraction, transmission electron microscopy and ultraviolet-visible diffuse-reflectance spectroscopy, respectively.The photocatalytic activities were evaluated via the degradation of catechol under visible light irradiation.The results show that the photocatalyst with a total loading mass of Au/Co of 2% and Au:Co molar ratio of 5:1, calcined at 400 ℃ has an optimum degradation efficiency of catechol.In this case, 94.7% of catechol can be degraded at 5 h.
引文
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[25]夏盛杰,邵蒙蒙,倪哲明,等.含Ce水滑石基复合氧化物对混合染料的光催化性能[J].无机化学学报,2016,32(6):983-993.XIA Shengjie,SHAO Mengmeng,NI Zheming,et al.Chin J Inorg Chem(in Chinese),2016,32(6):983-993.
[2]LTA?EF A H,D'ANGELO A,SCIALDONE O,et al.Electrochemical treatment of aqueous solutions of catechol by various electrochemical advanced oxidation processes:Effect of the process and of operating parameters[J].J Electroanal Chem,2017,796:1-8.
[3]LI H,PAN B,LIAO S H,et al.Formation of environmentally persistent free radicals as the mechanism for reduced catechol degradation on hematite-silica surface under UV irradiation[J].Environ Pollut,2014,188:153-158.
[4]LOFRANO G,RIZZO L,GRASSI M,et al.Advanced oxidation of catechol:A comparison among photocatalysis,Fenton and photo-Fenton processes[J].Desalination,2009,249:878-883.
[5]钱萍萍,薛继龙,倪哲明,等.锌铝水滑石对亚甲基蓝光催化降解性能[J].无机化学学报,2012,28(7):1348-1352.QIAN Pingping,XUE Jilong,NI Zheming,et al.Chin J Inorg Chem(in Chinese),2012,28(7):1348-1352.
[6]倪哲明,薛继龙.含Cu水滑石的结构与光催化性能[J].高等学校化学学报,2013,34(3):503-508.NI Zheming,XUE Jilong.Chem J Chin Univ(in Chinese),2013,34(3):503-508.
[7]宋健.焙烧型锌铝水滑石杂化材料的制备与光催化性能研究[D].长沙:中南大学,2014.SONG Jian.Preparation and photocatalytic performance study of calcined hybrid Zn-Al layered double hydroxide material(in Chinese,dissertation).Changsha:Central South University,2014.
[8]袁冰,张新,侯万国.Zn/Al类水滑石及其插层材料的光催化性能[J].应用化工,2012,41(2):195-201.YUAN Bing,ZHANG Xin,HOU Wanguo.Appl Chem Ind(in Chinese),2012,41(2):195-201.
[9]徐敏虹,潘国祥,汪小华,等.Zn-M-Cr三元水滑石的合成及其光催化性能[J].硅酸盐学报,2017,45(8):1175-1182.XU Minhong,PAN Guoxiang,WANG Xiaohua,et al.J Chin Ceram Soc,2017,45(8):1175-1182.
[10]LI D L,FAN Y Y,DING Y Y,et al.Preparation of cobalt-copper-aluminum spinel mixed oxides from layered double hydroxides for total oxidation of benzene[J].Catal Commun,2017,88:60-63.
[11]COJOCARU B,ANDREI V,TUDORACHE M,et al.Enhanced photo-degradation of bisphenol pollutants onto gold-modified photocatalysts[J].Catal Today,2017,284:153-159.
[12]赵宇飞.高分散层状催化剂的制备及其光催化性能研究[D].北京:北京化工大学,2013.ZHAO Yufei.Studies on the preparation and photocatalytic performances of highly dispersed layered structure catalysts(in Chinese,dissertation).Beijing:Beijing University of Chemical Technology,2013.
[13]MIKAMI G,GROSU F,KAWAMURA S,et al.Harnessing self-supported Au nanoparticles on layered double hydroxides comprising Zn and Al for enhanced phenol decomposition under solar light[J].Appl Catal B,2016,199:260-271.
[14]LI Z,ZHANG Q W,LIU X Z,et al.One-step mechanochemical synthesis of plasmonic Ag/Zn-Al LDH with excellent photocatalytic activity[J].Catal Today,2018,53(18):12759-12806.
[15]王丹军,王婵,赵强,等.Au纳米粒子表面等离子共振效应(SPR)增强Au/Bi2WO6异质纳米结构的光催化活性[J].无机材料学报,2018,33(6):659-666.WANG Danjun,WANG Chan,ZHAO Qiang,et al.J Inorg Mater(in Chinese),2018,33(6):659-666.
[16]KIM S H,DURAND P,ANDRE E,et al.Enhanced photocatalytic ability of Cu,Co doped ZnAl based mixed metal oxides derived from layered double hydroxides[J].Colloid Surf A,2017,524:43-52.
[17]郑小刚,杜京城,付孝锦,等.双金属位催化剂Ag-Ni/g-C3N4可见光催化降解亚甲基蓝[J].硅酸盐学报,2018,46(1):85-92.ZHENG Xiaogang,DU Jingcheng,FU Xiaojin,et al.J Chin Ceram Soc,2018,46(1):85-92.
[18]曹根庭,夏盛杰,倪哲明,等.不同阴离子插层锌铝水滑石对亚甲基蓝的光催化性能[J].硅酸盐学报,2016,44(5):726-732.CAO Genting,XIA Shengjie,NI Zheming,et al.J Chin Ceram Soc,2016,44(5):726-732.
[19]LIN Y,ZENG Z K,LIU L,et al.Facile synthesis of ZnAl-layered double hydroxide microspheres with core-shell structure and their enhanced adsorption capability[J].Mater Lett,2015,156:169-172.
[20]YUAN X Y,JING Q Y,CHEN J T,et al.Photocatalytic Cr(VI)reduction by mixed metal oxide derived from ZnAl layered double hydroxide[J].Appl Clay Sci,2017,143:168-174.
[21]钱萍萍.锌系水滑石对亚甲基蓝降解性能的研究[D].杭州:浙江工业大学,2014.QIAN Pingping.Study on degradation of methylene blue with zinc based layered double hydroxides(in Chinese,dissertation).Hangzhou:Zhejiang University of Technology,2014.
[22]APOPEI P,CATRINESCU C,TEODOSIU C,et al.Mixed-phase TiO2photocatalysts:Crystalline phase isolation and reconstruction,characterization and photocatalytic activity in the oxidation of4-chlorophenol from aqueous effluents[J].Appl Catal B,2014,160:374-382.
[23]YANG J L,MOU C Y.Ordered mesoporous Au/TiO2 nanospheres for solvent-free visible-lightdriven plasmonic oxidative coupling reactions of amines[J].Appl Catal B,2018,231:283-291.
[24]赵菲,时林其,林艳红,等.Au纳米粒子负载的ZnO空心球复合材料的光生电荷转移行为及光催化活性[J].物理化学学报,2016,32(8):2069-2076.ZHAO Fei,SHI Linqi,LIN Yanhong,et al.Acta Phys-Chim Sin(in Chinese),2016,32(8):2069-2076.
[25]夏盛杰,邵蒙蒙,倪哲明,等.含Ce水滑石基复合氧化物对混合染料的光催化性能[J].无机化学学报,2016,32(6):983-993.XIA Shengjie,SHAO Mengmeng,NI Zheming,et al.Chin J Inorg Chem(in Chinese),2016,32(6):983-993.