新型乙苯脱氢催化剂PED-06的制备与性能评价
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摘要
以氧化铁红、K_2CO_3、草酸铈、钼酸铵、CaO,MgO等为原料,采用干混捏合法制备出乙苯脱氢催化剂PED-06。在100 mL等温装置上,考察了主活性相铁酸钾(K_2Fe_(22)O_(34))的焙烧温度、钙源种类及主要助剂组分MgO,K_2O含量对催化剂性能的影响,并在4 L绝热负压侧线装置上进行了催化剂性能评价。结果表明:在等温装置上,于主活性相的焙烧温度为750℃,以CaO为钙源,催化剂中MgO,K_2O质量分数分别为1.5%,14.0%的条件下,乙苯转化率为81.50%,苯乙烯选择性为96.00%;在绝热负压侧线装置上,于第1、第2反应器入口温度分别为610,615℃,乙苯液体空速为0.42 h~(-1),水与乙苯质量比为1.5,第2反应器出口压力为40 kPa的条件下,催化剂连续运行1 000 h后,乙苯转化率大于68.00%,苯乙烯选择性高于97.00%。
The PED-06 ethylbenzene dehydrogenation catalyst was prepared by the dry kneading method,with the iron oxide red,K_2CO_3,cerous oxalate,ammonium molybdate,CaO,MgO,etc,as raw materials. The effects of calcination temperature and calcium type of main active phase( K_2 Fe_(22) O_(34))and main auxiliary MgO,K_2 O on properties of catalyst were investigated in a 100 mL isothermal unit and the properties of catalyst were evaluated in a 4 L adiabatic side line device. The results showed that under the conditions of the calcination temperature of main active phase 750 ℃,CaO as calcium source,the mass fraction of MgO,K_2 O in catalyst was 1. 5%,14. 0% respectively,the ethylbenzene conversion was 81. 50%,styrene selectivity 96. 00%in the isothermal unit; under the conditions of the inlet temperature of the first and the second reactor610,615 ℃ respectively,the liquid space velocity of ethylbenzene 0. 42 h~(-1),the water to ethylbenzene1. 5( mass fraction),the outlet pressure of the second reactor 40 kPa,after the catalyst had been running for 1 000 h,the ethylbenzene conversion was above 68. 00%,and the styrene selectivity was more than 97. 00%.
The PED-06 ethylbenzene dehydrogenation catalyst was prepared by the dry kneading method,with the iron oxide red,K_2CO_3,cerous oxalate,ammonium molybdate,CaO,MgO,etc,as raw materials. The effects of calcination temperature and calcium type of main active phase( K_2 Fe_(22) O_(34))and main auxiliary MgO,K_2 O on properties of catalyst were investigated in a 100 mL isothermal unit and the properties of catalyst were evaluated in a 4 L adiabatic side line device. The results showed that under the conditions of the calcination temperature of main active phase 750 ℃,CaO as calcium source,the mass fraction of MgO,K_2 O in catalyst was 1. 5%,14. 0% respectively,the ethylbenzene conversion was 81. 50%,styrene selectivity 96. 00%in the isothermal unit; under the conditions of the inlet temperature of the first and the second reactor610,615 ℃ respectively,the liquid space velocity of ethylbenzene 0. 42 h~(-1),the water to ethylbenzene1. 5( mass fraction),the outlet pressure of the second reactor 40 kPa,after the catalyst had been running for 1 000 h,the ethylbenzene conversion was above 68. 00%,and the styrene selectivity was more than 97. 00%.
引文
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[2]Ma L P,Ning P,Zheng S C,et al.Reaction mechanism and kinetic analysis of the decomposition of phosphogypsum via a solidstate reaction[J].Industrial and Engineering Chemistry Research,2010,49(8):3597-3602.
[3]Othman I,Al-Masri M S.Impact of phosphate industry on the environment:A case study[J].Applied Radiation and Isotopes,2007,65(1):131-141.
[4]董英.苯乙烯的生产技术及市场分析[J].炼油与化工,2013,24(3):44-46.
[5]薛祖源.乙苯/苯乙烯生产工艺技术进展(上)[J].上海化工,2008(33):24-27.
[6]薛祖源.乙苯/苯乙烯生产工艺技术进展(下)[J].上海化工,2008(33):18-22.
[7]吴荣安,白玉珩.DC型乙苯脱氢催化剂的性能与工业应用[J].石油化工,1993(22):465-470.
[8]祝以湘,戴深峻,沈若范,等.氧化铁系脱氢催化剂的催化活性本质[J].厦门大学学报,1994(33):173-178.
[9]祝以湘,雷德斌,戴深峻,等.Mg对氧化铁系脱氢催化剂相变温度的影响[J].厦门大学学报,1994(33):180-183.
[10]祝以湘,封雷,陈荣钦,等.乙苯脱氢催化剂中Ca O助催化作用的穆斯堡尔谱学表征[J].化学物理学报,1999(12):491-498.
[11]祝以湘,柴运宇,刘正阳,等.钾助催化剂与Fe3O4相互作用行为的XRD表征[J].物理化学学报,2000(16):125-132.