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Catalysts phase transition in pre-fluorination of MOx/Al2O3 (M=Ni,Mg,Co,Ce) and catalytic pyrolysis performance of HFC-134a to trifluoroethylene

ZHAO Yang1,ZHANG Xuanyu1,ZHOU Qiang2,WU Zhou’an2,WANG Shuhua2,LUO Mengfei1   

  1. 1Zhejiang Key Laboratory for Reactive Chemistry on Solid Surfaces,Institute of Physical Chemistry,Zhejiang Normal University,Jinhua 321004,Zhejiang,China;2Technology Center of Juhua Group,Quzhou 324004,Zhejiang,China
  • Online:2014-08-25 Published:2014-08-05

MOx/Al2O3(M=Ni、Mg、Co、Ce)催化剂氟化预处理过程的 物相转变和HFC-134a裂解制三氟乙烯性能

赵洋1,章轩语1,周强2,吴周安2,王树华2,罗孟飞1   

  1. 1浙江师范大学物理化学研究所,浙江省固体表面反应化学重点实验室,浙江 金华 321004; 2巨化集团技术中心,浙江 衢州 324004

Abstract: A series of MOx/Al2O3(M=Ni,Mg,Co,Ce) catalysts were prepared by the deposition-precipitation method,and the effect of different additives on catalytic pyrolysis was studied. The catalysts were characterized by X-ray diffraction (XRD),and transformation of Al species in the MOx/Al2O3 catalysts after pre-fluorination was investigated. The catalysts were used in catalytic pyrolysis of 1,1,1,2-tetrafluoroethane (HFC-134a) to trifluoroethylene (TrFE),and the results showed that the addition of Ni,Co,Ce to AlF3 could improve catalytic performance for the pyrolysis of HFC-134a,while that of Mg could cause inhibition of catalytic performance. High activity was obtained on NiFx/AlF3 catalyst. The conversion of 1,1,1,2-tetrafluoroethane was higher than 21.4% and the selectivity to trifluoroethylene was 99.7% at reaction temperature of 400℃,and NiFx/AlF3 catalyst exhibited a longer life span.

Key words: 1,1,1,2-tetrafluoroethane , catalysis, trifluoroethylene, alumina, deposition-precipitation, stability

摘要: 采用沉积沉淀法制备了MOx/Al2O3(M=Ni、Mg、Co、Ce)催化剂,研究了不同助剂对催化剂反应性能的影响,应用X射线衍射(XRD)考察了氟化预处理前后MOx/Al2O3催化剂中Al物种的转变,并应用于HFC-134a(1,1,1,2-四氟乙烷)裂解制备三氟乙烯(TrFE)反应。结果表明,Ni、Co、Ce添加能有效提高AlF3催化剂的HFC-134a裂解性能,而Mg对AlF3催化性能起抑制作用。其中,NiFx/AlF3催化剂催化性能最高,当反应温度为400℃时,HFC-134a的转化率最高可达21.4%,三氟乙烯的选择性在99.7%以上,且反应较为稳定。

关键词: 四氟乙烷, 催化, 三氟乙烯, 氧化铝, 沉积沉淀法, 稳定性