Y和Si共掺杂纳米TiO_2的制备及光催化性能
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摘要
以自制的Gemini表面活性剂为软模板,钛酸四丁酯、正硅酸四乙酯、硝酸钇为原料,采用水热法制备了Y、Si共掺杂TiO_2(Y/Si/TiO_2)纳米颗粒。对Y/Si/TiO_2纳米颗粒的结构、形貌、光吸收范围及价态进行了表征;以甲基橙为模拟污染物,评价了样品的光催化性能。结果表明:TiO_2为单一的锐钛矿相,Y和Si成功的掺杂进入TiO_2晶格中;Y和Si掺杂抑制了晶粒长大,结晶度降低,减少了禁带宽度,从而使样品比表面积增大,提高了可见光的响应范围,降低了光生电子-空穴对的复合几率。当掺杂Y和Si的摩尔比为1:1时,1.0%Y/1.0%Si/TiO_2催化性能最好,500 W氙灯照射90 min,其降解效率达到95.5%。
Y and Si co-doped TiO_2(Y/Si/TiO_2) nanoparticles were synthesized by a hydrothermal method using titanium butoxide,tetraethyl orthosilicate and yttrium nitrate as starting materials, and Gemini surfactant as a soft template. The structure, morphology,light absorption range and valence state of the prepared Y/Si/TiO_2 nanoparticles were investigated. The photocatalytic properties of the samples were evaluated by using methyl orange as a simulated pollutant. The results show that TiO_2 is a single anatase phase, and Y and Si are doped into TiO_2 lattice. Y and Si co-doping inhibits the grain growth and decreases the band gap and crystallinity.Thereby, the specific surface area of the sample increases and the response range of visible light improves, and the recombination probability of the electron–hole pairs reduces. The 1.0%Y/1.0%Si/TiO_2 sample has an optimum catalytic performance, and the degradation efficiency reaches 95.5% after 500 W xenon lamp irradiation for 90 min.
Y and Si co-doped TiO_2(Y/Si/TiO_2) nanoparticles were synthesized by a hydrothermal method using titanium butoxide,tetraethyl orthosilicate and yttrium nitrate as starting materials, and Gemini surfactant as a soft template. The structure, morphology,light absorption range and valence state of the prepared Y/Si/TiO_2 nanoparticles were investigated. The photocatalytic properties of the samples were evaluated by using methyl orange as a simulated pollutant. The results show that TiO_2 is a single anatase phase, and Y and Si are doped into TiO_2 lattice. Y and Si co-doping inhibits the grain growth and decreases the band gap and crystallinity.Thereby, the specific surface area of the sample increases and the response range of visible light improves, and the recombination probability of the electron–hole pairs reduces. The 1.0%Y/1.0%Si/TiO_2 sample has an optimum catalytic performance, and the degradation efficiency reaches 95.5% after 500 W xenon lamp irradiation for 90 min.
引文
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[2]ZHANG X J,CHEN Y,ZHANG S,et al.High photocatalytic performance of high concentration Al-doped ZnO nanoparticles[J].Sep Purif Technol.,2017,172(01):236?241.
[3]侯静静,赵清华,李廷鱼,等.球状MoS2/WO3复合半导体制备及其对RhB的光催化性能[J].无机化学学报,2017,33(9):1527?1536.HOU Jingjing,ZHAO Qinghua,LI Tingyu,et al.Chin J Inorg Chem(in Chinese),2017,33(09):1527?1536.
[4]WANG R R,LIANG H F,HONG J Q,et al.Hydrothermal synthesis of cobalt-doped ZnS for efficient photodegradation of methylene blue[J].J Photochem Photobiol A,2016,325(07):62?67.
[5]POUNGCHAN G,KSAPABUTR B,PANAPOY M.One-step synthesis of flower-like carbon-doped ZrO2 for visible-light-responsive photocatalyst[J].Mater Des,2016,89(01):137?145.
[6]YAN Y H,GUAN H Y,LIU S,et al.Ag3PO4/Fe2O3 composite photocatalysts with an n-n heterojunction semiconductor structure under visible-light irradiation[J].Ceram Int,2014,40(08):9095?9100.
[7]LIN Y M,JIANG Z Y,ZHU C Y,et al.Electronic and optical performances of Si and Fe-codoped TiO2 nanoparticles:Aphotocatalyst for the degradation of methylene blue[J],Appl Catal B-Environ,2013,142(3):38?44.
[8]VASILI?R,STOJADINOVI?S,RADI?N,et al.One-step preparation and photocatalytic performance of vanadium doped TiO2coatings[J].Mater Chem Phys,2015,151(2):337?344.
[9]SANCHEZ-MARTINEZ A,CEBALLOS-SANCHEZ O,KOOP-SANTA C,et al.N-doped TiO2 nanoparticles obtained by a facile coprecipitation method at low temperature[J].Ceram Int,2018,44(4):5273?5283.
[10]ZHAO Y F,LI C,LU S,et al.Electronic,optical and photocatalytic behavior of Mn,N doped and co-doped TiO2:Experiment and simulation[J].J Solid State Chem,2016,235(3):160?168.
[11]POURETEDAL H R.Visible photocatalytic activity of co-doped Ti O2/Zr,N nanoparticles in wastewater treatment of nitrotoluene samples[J].J Alloy Compd,2018,735(2):2507?2511.
[12]RENGIFO-HERRERA J A,BLANCO M,WIST J,et al.Ti O2modified with polyoxotungstates should induce visible-light absorption and high photocatalytic activity through the formation of surface complexes[J].Appl Catal B-Environ,2016,189(7):99?109.
[13]SEDGHI R,MOAZZAMI H R,HOSSEINY DAVARANI S S,et al.A one step electrospinning process for the preparation of polyaniline modified TiO2/polyacrylonitile nanocomposite with enhanced photocatalytic activity[J].J Alloy Compd,2017,695(2):1073?1079.
[14]李跃军,曹铁平,梅泽民,等.Pr掺杂Bi2MoO6/TiO2复合纳米纤维的制备及可见光催化性能[J].高等学校化学学报,2017,38(12):2313?2319.LI Yuejun,CAO Tieping,MEI Zeming,et al.Chem J Chin Univ(in Chinese),2017,38(12):2313?2319.
[15]HU J,LI H S,MUHAMMMAD S,et al.Surfactant-assisted hydrothermal synthesis of Ti O2/reduced graphene oxide nanocomposites and their photocatalytic performances[J].J Solid State Chem,2017,253(9):113?120.
[16]宋永强,张秀玲,张丽娟,等.离子液体辅助水热法制备Ti O2/CoFe2O4复合材料及光催化性能[J].硅酸盐学报,2015,43(4):493?497.SONG Yongqiang,ZHANG Xiuling,ZHANG Lijuan,et al.J Chin Ceram Soc,2015,43(4):493?497
[17]ZHOU P P,LE Z G,XIE Y,et al.Studies on facile synthesis and properties of mesoporous Cd S/TiO2 composite for photocatalysis applications[J].J Alloy Compd,2017,692(1):170?177.
[18]LI Z Y,FANG Y L,XU S.Squaraine dye sensitized TiO2nanocomposites with enhanced visible-light photocatalytic activity[J].Mater Lett,2013,93(2):345?348.
[19]QIN G H,WU Q P,SUN Z,et al.Enhanced photoelectrocatalytic degradation of phenols with bifunctionalized dye-sensitized TiO2film[J].J Hazard Mater,2012,199(1):226?232.
[20]YANG G D,JIANG Z,SHI H H,et al.Study on the photocatalysis of F-S co-doped TiO2 prepared using solvothermal method[J].Appl Catal B-Environ,2010,96(6):458?465.
[21]WANG R F,WANG F M,AN S L,et al.Y/Eu co-doped Ti O2:synthesis and photocatalytic activities under UV-light[J].J Rare Earth,2015,33(2):154-159.
[22]JAISWAL R,BHARAMBE J,PATEL N,et al.Copper and Nitrogen co-doped TiO2 photocatalyst with enhanced optical absorption and catalytic activity[J].Appl Catal B-Environ,2015,168/169:333?341.
[23]CHEN Y,WU Q,ZHOU C,et al.Enhanced photocatalytic activity of La and N co-doped TiO2/diatomite composite[J].Powder Technol,2017,322(12):296?300.
[24]SIDDIQA A,MASIH D,ANJUM D,et al.Cobalt and sulfur co-doped nano-size TiO2 for photodegradation of various dyes and phenol[J].JEnviron Sci,2015,37(11):100?109.
[25]LI J J,CAI S C,XU Z,et al.Solvothermal syntheses of Bi and Zn co-doped TiO2 with enhanced electron-hole separation and efficient photodegradation of gaseous toluene under visible-light[J].J Hazard Mater,2017,325(3):261?270.
[26]ZHANG W,LI X J,JIA G,et al.Preparation,characterization,and photocatalytic activity of boron and lanthanum co-doped TiO2[J].Catal Commun,2014,45(2):144?147.
[27]SHAROTRI N,SUD D.Visible light responsive Mn-S-co-doped TiO2photocatalyst-Synthesis,characterization and mechanistic aspect of photocatalytic degradation[J].Sep Purif Technol,2017,183(8):382?391.
[28]王瑞芬,王福明,宋金玲,等.RE-B共掺杂片层Ti O2的合成及其光催化性能[J].物理化学学报,2016,32(2):536?542.WANG Ruifen,WANG Fuming,RONG Jilin,et al.Acta Phys Chim Sin(in Chinese),2006,32(2):536?542.
[29]高志农,吕波,魏俊超.含酯基季铵盐Gemini表面活性剂的合成及表面活性[J].武汉大学学报(理学版),2006,52(2):159?162.GAO Zhinong,LV Bo,WEI Junchao.Wuhan Univ:Nat Sci Ed(in Chinese),2006,52(2):159?162.
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[32]LI Y L,WANG T J,JIN Y.Surface characteristics of hydrous silica-coated TiO2 particles[J].Powder Technol,2002,123:194?198.
[33]陈其凤,姜东,徐耀,等.溶胶-凝胶-水热法制备Ce-Si/TiO2及其可见光催化性能[J].物理化学学报,2009,25(4):617?623.CHEN Qifeng,JIANG Dong,XU Yao,et al.Acta Phys Chim Sin(in Chinese),2009,25(4):617?623.
[34]YAN X L,HE J,G EVANS D,et al.Preparation,characterization and photocatalytic activity of TiO2 codoped with yttrium and nitrogen[J].Mater Chem Phys,2011,125(1):156?160.
[35]WU Y T,GONG Y Y,LIU J Q,et al.B and Y co-doped TiO2photocatalyst with enhanced photodegradation efficiency[J].J Alloy Compd,2017,695(2):1462?1469.
[36]张宇,王敏,周鑫,等.AgVO3/BiVO4复合光催化剂的制备及可见光催化性能[J].硅酸盐学报,2019,47(1):1?7.ZHANG Yu,WANG Min,ZHOU Xin,et al.J Chin Ceram Soc,2019,47(1):1?7.
[37]马继艳,耿延玲.CeO2/BiOI复合材料的制备与光催化性能[J].硅酸盐学报,2018,46(8):1178?1182.MA Jiyan,GENG Yanling.J Chin Ceram Soc,2018,46(8):1178?1182.