变温陈化法制备TS-1分子筛及其催化性能
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摘要
通过变温陈化步骤,采用水热结晶法制备TS-1分子筛。改变陈化步骤,得到一系列粒径不同的TS-1分子筛,并探究粒径对丙烯醇环氧化反应催化性能的影响。采用FT-IR、UV-Vis、BET、XRD和SEM等表征TS-1分子筛催化剂晶相,结果表明,不同条件制得的TS-1分子筛具有相同的MFI结构,Ti大部分以骨架钛形式存在,也有少量锐钛矿相Ti O2存在。随着反应温度的升高,TS-1粒径逐渐增大。通过后续催化反应发现,TS-1分子筛催化剂的催化活性改变不大,这可能是由于催化剂中活性位点的数目变化不大。从催化剂分离实验可以看出,随着粒径的增大,催化剂回收率从82.4%增至95.3%。
TS-1 molecular sieve was prepared by hydrothermal crystallization method through aging at different temperature. A series of TS-1 with different particle size were obtained by changing aging steps,and effects of particle size on the catalytic performance of epoxidation of propylene alcohol were investigated. The crystalline phases of the obtained catalysts were investigated by FT-IR,UV,BET,XRD,and SEM,the results showed that the TS-1 prepared by different conditions had the same MFI structure. Most Ti was in the framework,some few was anatase Ti O2. As reaction temperature increased,the particle size of TS-1 gradually increased. The catalytic activity changed little,probably due to that the number of active sites in the catalyst did not change much. The catalyst separation experiment showed that the catalyst recovery increased from 82. 4% to 95. 3% with the increasing of particle size.
TS-1 molecular sieve was prepared by hydrothermal crystallization method through aging at different temperature. A series of TS-1 with different particle size were obtained by changing aging steps,and effects of particle size on the catalytic performance of epoxidation of propylene alcohol were investigated. The crystalline phases of the obtained catalysts were investigated by FT-IR,UV,BET,XRD,and SEM,the results showed that the TS-1 prepared by different conditions had the same MFI structure. Most Ti was in the framework,some few was anatase Ti O2. As reaction temperature increased,the particle size of TS-1 gradually increased. The catalytic activity changed little,probably due to that the number of active sites in the catalyst did not change much. The catalyst separation experiment showed that the catalyst recovery increased from 82. 4% to 95. 3% with the increasing of particle size.
引文
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[14]左轶,刘民,郭新闻.钛硅分子筛的合成及其催化氧化反应研究进展[J].石油学报(石油加工),2015,31(2):343-359.Zuo Yi,Liu Min,Guo Xinwen.Recent advances in synthesis and catalytic oxidation reactions of titanium silicates[J].Acta Petrolei Sinica,(Petroleum Processing Section)2015,31(2):343-359.
[15]陈晓晖,范志勇,魏可镁.烯丙醇在Ti-MWW催化剂上的环氧化反应[J].石油化工,2006,35(3):255-259.Chen Xiaohui,Fan Zhiyong,Wei Kemei,et al.Epoxidation of allyl alcohol over Ti-MWW molecular sieve catalyst[J].Petrochemical Technology,2006,35(3):255-259.
[16]成卫国,王祥生,李钢,等.钛硅分子筛挤条成型催化剂研究[J].大连理工大学学报,2004,44(4):482-485.Cheng Weiguo,Wang Xiangsheng,Li Gang,et al.Study on Ti-Si molecular sieve extruded catalyst[J].Journal of Dalian University of Technology,2004,44(4):482-485.
[17]成卫国,王祥生,李钢,等.钛硅分子筛挤条成型催化剂热稳定性能的研究[J].分子催化,2004,18(4):241-247.Cheng Weiguo,Wang Xiangsheng,Li Gang,et al.Study on thermal stability of titanium silicalite zeolite extruded catalyst[J].Journal of Molecular Catalysis,2004,18(4):241-247.
[18]刘国清,夏珺,袁霞,等.喷雾成型TS-1分子筛催化剂的制备及其性能[J].石油学报(石油加工),2015,31(1):126-131.Liu Guoqing,Xia Jun,Yuan Xia,et al.Preparation and characterization of spray forming titanium silicate-1 molecular sieve catalyst[J].Acta Petrolei Sinica(Petroleum Processing Section),2015,31(1):126-131.
[2]陈晓晖,蔡丽蓉,魏可镁.钛硅分子筛膜的合成及其催化性能的研究[J].化工进展,2004,23(11):1222-1226.Chen Xiaohui,Cai Lirong,Wei Kemei.Study on synthesis and catalytic performance of titanium silicate zeolite membrane[J].Chemical Industry and Engineering Progress,2004,23(11):1222-1226.
[3]Liu M,Wei H,Li B,et al.Green and efficient preparation of hollow titanium silicalite-1 by using recycled mother liquid[J].Chemical Engineering Journal,2018,331:194-202.
[4]Zuo Y,Liu M,Ma M,et al.Improved catalytic performance for 1-butene epoxidation over titanium silicalite-1 extrudates by using SBA-15 or carborundum as additives[J].Industrial&Engineering Chemistry Research,2017,56(26):7462-7467.
[5]Zhang T,Zuo Y,Liu M,et al.Synthesis of titanium silicalite-1with high catalytic performance for 1-butene epoxidation by eliminating the extraframework Ti[J].ACS Omega,2016,1(5):1034-1040.
[6]Zuo Y,Wang X,Guo X.Synthesis of titanium silicalite-1with small crystal size by using mother liquid of titanium silicalite-1 as seed[J].Industrial&Engineering Chemistry Research,2011,50(14):8485-8491.
[7]刘红,卢冠忠,郭杨龙,等.TS-1分子筛对固定床中苯酚羟基化反应的催化性能[J].催化学报,2004,25(1):49-54.Liu Hong,Lu Guanzhong,Guo Yanglong,et al.Catalytic performance of titanium silicalite-1 for hydroxylation of phenol in fixed-bed reactor[J].Chinese Journal of Catalysis,2004,25(1):49-54.
[8]张海娇,姚明恺,谢伟,等.TS-1分子筛的无机法合成及其催化苯酚羟基化性能[J].催化学报,2007,28(10):895-899.Zhang Haijiao,Yao Minkai,Xie Wei,et al.Synthesis of TS-1using inorganic Si O2-Ti O2precursor and its catalytic performance for hydroxylation of phenol[J].Chinese Journal of Catalysis,2007,28(10):895-899.
[9]Uguina M A,Ovejero G,Van Grieken R,et al.Synthesis of titanium silicalite-1 from an Si O2-Ti O2cogel using a wetness impregnation method[J].Journal of the Chemical Society,Chemical Communications,1994,(1):27-28.
[10]Hao L,Qian L,Zhang X,et al.Synthesis,characterization,and catalytic performance of bifunctional titanium silicalite-1[J].Chinese Journal of Catalysis,2013,34(7):1363-1372.
[11]Alonso-Fagúndez N,Agirrezabal-Telleria I,Arias P L,et al.Aqueous-phase catalytic oxidation of furfural with H2O2:high yield of maleic acid by using titanium silicalite-1[J].RSC Advances,2014,4(98):54960-54972.
[12]Deng X,Wang Y,Shen L,et al.Low-cost synthesis of titanium silicalite-1(TS-1)with highly catalytic oxidation performance through a controlled hydrolysis process[J].Industrial&Engineering Chemistry Research,2013,52(3):1190-1196.
[13]Huang D G,Zhang X,Liu T W,et al.Synthesis of highperformanced titanium silicalite-1 zeolite at very low usage of tetrapropyl ammonium hydroxide[J].Industrial&Engineering Chemistry Research,2013,52(10):3762-3772.
[14]左轶,刘民,郭新闻.钛硅分子筛的合成及其催化氧化反应研究进展[J].石油学报(石油加工),2015,31(2):343-359.Zuo Yi,Liu Min,Guo Xinwen.Recent advances in synthesis and catalytic oxidation reactions of titanium silicates[J].Acta Petrolei Sinica,(Petroleum Processing Section)2015,31(2):343-359.
[15]陈晓晖,范志勇,魏可镁.烯丙醇在Ti-MWW催化剂上的环氧化反应[J].石油化工,2006,35(3):255-259.Chen Xiaohui,Fan Zhiyong,Wei Kemei,et al.Epoxidation of allyl alcohol over Ti-MWW molecular sieve catalyst[J].Petrochemical Technology,2006,35(3):255-259.
[16]成卫国,王祥生,李钢,等.钛硅分子筛挤条成型催化剂研究[J].大连理工大学学报,2004,44(4):482-485.Cheng Weiguo,Wang Xiangsheng,Li Gang,et al.Study on Ti-Si molecular sieve extruded catalyst[J].Journal of Dalian University of Technology,2004,44(4):482-485.
[17]成卫国,王祥生,李钢,等.钛硅分子筛挤条成型催化剂热稳定性能的研究[J].分子催化,2004,18(4):241-247.Cheng Weiguo,Wang Xiangsheng,Li Gang,et al.Study on thermal stability of titanium silicalite zeolite extruded catalyst[J].Journal of Molecular Catalysis,2004,18(4):241-247.
[18]刘国清,夏珺,袁霞,等.喷雾成型TS-1分子筛催化剂的制备及其性能[J].石油学报(石油加工),2015,31(1):126-131.Liu Guoqing,Xia Jun,Yuan Xia,et al.Preparation and characterization of spray forming titanium silicate-1 molecular sieve catalyst[J].Acta Petrolei Sinica(Petroleum Processing Section),2015,31(1):126-131.
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