分子筛固载化三氯化铁的制备及催化性能研究
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摘要
采用萘与异丙醇的烷基化合成路线,考察了改性分子筛的催化性能以及反应条件对异丙基化反应的影响。以分子筛为载体,采用离子交换法制备了固载FeCl_3的HM(H-SAPO-11、HZSM-5)分子筛催化剂,采用XRD、扫描电镜/X射线能谱仪(SEM/EDS)、BET、FT-IR对催化剂做了表征;在微分反应器上考察了改性分子筛的催化性能和反应条件对萘异丙基化反应的影响。当FeCl_3在HM上的固载量(质量分数,下同)从10%增至50%时,萘的转化率也随之增大。对50%Fe/HM分子筛催化剂,在原料配比为n(萘)∶n(异丙醇)∶n(环己烷)=1∶2∶10、催化剂质量为2 g、质量空速为1 h-1、反应温度为280℃的条件下,萘转化率为61.4%,2,6-DIPN的收率为38.4%,β,β-DIPN选择性为84.6%。
The alkylation route of naphthalene and isopropanol was used to investigate the effects of catalytic performance and reaction conditions of the modified molecular sieve on the isopropylation reaction.Using molecular sieve as carrier,HM(H-SAPO-11 and HZSM-5) zeolite catalysts supported on FeCl_3 were prepared by ion exchange method.The above catalysts were characterized by means of X-ray diffraction(XRD),scanning electron microscope/energy dispersion spectrometer(SEM/EDS),Brunauer-Emmett-Teller(BET),Fourier transform infrared spectroscopy(FT-IR).The effects of catalytic properties and reaction conditions of modified molecular sieve on isopropylation of naphthalene were carried out with fixed-bed flow microreactor.The conversion of naphthalene increased substantially with the increase of FeCl_3 on HM loading from 10% to 50%(mass fraction).The ratio of raw materials was[n(naphthalene)∶n(isopropanol)∶n(cyclohexane)=1∶2∶10],the mass of the catalyst was 2 g,the mass space velocity was 1 h-1,and the reaction temperature was 280 ℃. Under the conditions,for the 50% Fe/HM,the conversion of naphthalene reached 61.4%,the yield of 2,6-DIPN was 38.4% and the selectivity of β,β-DIPN was 84.6%.
The alkylation route of naphthalene and isopropanol was used to investigate the effects of catalytic performance and reaction conditions of the modified molecular sieve on the isopropylation reaction.Using molecular sieve as carrier,HM(H-SAPO-11 and HZSM-5) zeolite catalysts supported on FeCl_3 were prepared by ion exchange method.The above catalysts were characterized by means of X-ray diffraction(XRD),scanning electron microscope/energy dispersion spectrometer(SEM/EDS),Brunauer-Emmett-Teller(BET),Fourier transform infrared spectroscopy(FT-IR).The effects of catalytic properties and reaction conditions of modified molecular sieve on isopropylation of naphthalene were carried out with fixed-bed flow microreactor.The conversion of naphthalene increased substantially with the increase of FeCl_3 on HM loading from 10% to 50%(mass fraction).The ratio of raw materials was[n(naphthalene)∶n(isopropanol)∶n(cyclohexane)=1∶2∶10],the mass of the catalyst was 2 g,the mass space velocity was 1 h-1,and the reaction temperature was 280 ℃. Under the conditions,for the 50% Fe/HM,the conversion of naphthalene reached 61.4%,the yield of 2,6-DIPN was 38.4% and the selectivity of β,β-DIPN was 84.6%.
引文
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[3]Cai T X,He M,Shi X Z,et al.New approaches to immobilization of aluminium chloride onγ-Al2O3[J].Chemical Journal of Chinese Universities,2001(8)1385-1387.
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[5]吴同旭.负载活性组分对载体孔结构的影响[J].无机盐工业,2017,49(6):94-96.
[6]Zi J F,Zhu L.Synthesis of iso-amylacetate catalyzed by ferric chloride supported on activated carbon[J].Industrial Catalysis,2004,12(9):31-33.
[7]Tan J,Fan H.Bu Zh Y,et al.Study on redistribution of methyltrichlorosilane and trimethylchlorosilane over AlCl3supported catalyst[J].Chemical Reaction Engineering and Technology,2005,21(4):315-319.
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