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    磷氧化物改性 HMCM-22催化剂的制备及其择形催化合成对二甲苯

    时时彩提前开奖作弊 www.sw4ac.com 收稿日期:2014‐06‐06

    基金项目:国家自然科学基金(21076027)、江苏省高校自然科学基金(12KJB 530002)和江苏省精细石油化工重点实验室开放课题(KF 1104)资助第一作者:薛冰,男,副研究员,博士,主要从事择形催化剂的研究;T el :0519‐86330135;E ‐mail :xuebing @cczu .edu .cn

    通讯联系人:李永昕,男,教授,博士,主要从事石油加工过程新型催化剂的研究;E ‐mail :13584372755@163.com 文章编号:1001‐8719(2015)05‐1057‐06

    磷氧化物改性HMCM ‐22催化剂的制备及其

    择形催化合成对二甲苯

    薛 冰,吴 晟,宋 小,柳 娜,苏 进,李永昕

    (常州大学石油化工学院江苏省绿色催化材料与技术重点实验室,江苏常州213164)

    摘要:以磷酸三乙酯为磷氧化物前驱物,采用浸渍法制备了一系列磷改性HMCM ‐22催化剂,在固定床反应器上考察了它们在甲苯与碳酸二甲酯烷基化合成对二甲苯反应中的择形催化性能。采用N 2吸附‐脱附、N H 3‐T PD 和Py ‐IR 手段对催化剂进行了表征,并考察了反应温度、空速及反应时间对甲苯烷基化反应的影响。结果表明,以磷酸三乙酯为磷氧化物的前驱物制备的磷改性HMCM ‐22催化剂在甲苯烷基化合成对二甲苯反应中,不仅表现出优异的择形性能,而且还保持了较高的催化活性。这主要是由于磷酸三乙酯有较大的分子尺寸,浸渍过程中可覆盖

    分子筛外表面酸性位,并可保证分子筛孔内的酸性位不受影响。

    关 键 词:对二甲苯;择形催化;磷酸三乙酯;HMCM ‐22

    中图分类号:T Q 241.1 文献标识码:A doi :10.3969/j .issn .1001‐8719.2015.05.004Preparation of Phosphorous Modified HMCM ‐22Catalyst and Its Shape ‐selectivity Catalytic Performance in Synthesis of p ‐Xylene

    XUE Bing ,WU Sheng ,SONG Xiao ,LIU Na ,SU Jin ,LI Yongxin

    (School o f Petrochemical En g ineering ,Chan g z hou Univ ersit y ,Jian g su K e y L aborator y o f A dv anced Catal y tic M aterials and

    Technolo gy ,Chan g z hou 213164,China )Abstract :A series of phosphorous modified HMCM ‐22catalysts were prepared by impregnation with triethyl phosphate (T EP )as the precursor of phosphorous oxide .T he catalytic performance of the phosphorous modified HMCM ‐22catalysts in the synthesis of p ‐xylene (PX )by alkylation of toluene with dimethyl carbonate was investigated in a fixed bed reactor .T he catalysts were characterized by means of N 2adsorption ‐desorption ,N H 3‐T PD and Py ‐IR .T he effects of reaction temperature ,M HSV and time ‐on ‐stream on the catalytic toluene alkylation were also investigated .T he results indicated that the phosphorous modified HMCM ‐22catalysts prepared by using T EP as the precursor of phosphorous oxide exhibited an excellent shape ‐selectivity along with a high catalytic activity ,w hich could be attributed to the large molecular size of T EP .T he T EP molecules could not diffuse into the po
    res of HM CM ‐22zeolite due to their large size and only well covered the acid sites on the external surface of HM CM ‐22zeolite .Key words :p ‐Xylene ;shape ‐selective catalysis ;triethyl phosphate ;HMCM ‐22

    Technolo gy ,Chan g z hou 213164,China )Abstract :A series of phosphorous modified HMCM ‐22catalysts were prepared by impregnation with triethyl phosphate (T EP )as the precursor of phosphorous oxide .T he catalytic performance of the phosphorous modified HMCM ‐22catalysts in the synthesis of p ‐xylene (PX )by alkylation of toluene with dimethyl carbonate was investigated in a fixed bed reactor .T he catalysts were characterized by means of N 2adsorption ‐desorption ,N H 3‐T PD and Py ‐IR .T he effects of reaction temperature ,M HSV and time ‐on ‐stream on the catalytic toluene alkylation were also investigated .T he results indicated that the phosphorous modified HMCM ‐22catalysts prepared by using T EP as the precursor of phosphorous oxide exhibited an excellent shape ‐selectivity along with a high catalytic activity ,w hich could be attributed to the large molecular size of T EP .T he T EP molecules could not diffuse into the pores of HM CM ‐22zeolite due to their large size and only well covered the acid sites on the external surface of HM CM ‐22zeolite .Key words :p ‐Xylene ;shape ‐selective catalysis ;triethyl phosphate ;HMCM ‐22

    对二甲苯(p ara ‐Xylene ,PX )是合成聚酯的重要

    原料[1]。目前,工业上主要通过甲苯歧化、混合二石油学报(石油加工)2015年10月 ACT A PET ROLEI SINICA (PET ROLEU M PROCESSING SECT IO N ) 第31卷第5期

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