物理化学学报 >> 2009, Vol. 25 >> Issue (02): 336-340.doi: 10.3866/PKU.WHXB20090224

研究论文 上一篇    下一篇

气相氟化合成1,1,1,2-四氟乙烷的CrOx-Y2O3催化剂的表征与性能

钱林; 邢丽琼; 毕庆员; 李洪芳; 陈科峰; 张学良; 鲁继青; 罗孟飞   

  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; 浙江衢化氟化学有限公司, 浙江 衢州 324004
  • 收稿日期:2008-10-30 修回日期:2008-12-02 发布日期:2009-01-16
  • 通讯作者: 罗孟飞 E-mail:mengfeiluo@zjnu.cn

Characterization and Performance of CrOx-Y2O3 Catalysts for the Synthesis of 1,1,1,2-Tetrafluoroethane

QIAN Lin; XING Li-Qiong; BI Qing-Yuan; LI Hong-Fang; CHEN Ke-Feng; ZHANG Xue-Liang; LU Ji-Qing; LUO Meng-Fei   

  1. Zhejiang Key Laboratory for Reactive Chemistry on Solid Surfaces, Institute of Physical Chemistry, Zhejiang Normal University, Jinhua 321004, Zhejiang Province, P. R. China; Zhejiang Qu Hua Fluor-Chemistry Company Limited, Quzhou 324004, Zhejiang Province, P. R. China
  • Received:2008-10-30 Revised:2008-12-02 Published:2009-01-16
  • Contact: LUO Meng-Fei E-mail:mengfeiluo@zjnu.cn

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摘要： 制备了一系列CrOx-Y2O3催化剂用于气相氟化1,1,1-三氟-2-氯乙烷(HCFC-133a)合成1,1,1,2-四氟乙烷(HFC-134a), 并考察了Y(OH)3、YCl3和Y(NO3)3前躯体对催化剂性能的影响. XRD和UV-Vis光谱实验结果表明, Y前躯体对催化剂表面Cr物种有影响, 其中采用Y(OH)3前躯体的催化剂有利于以高分散的Cr6+形式存在. 研究表明CrOx-Y2O3催化剂在预处理和反应过程中, 部分高价CrOx可转化为CrF3. 催化剂中CrF3含量增加, 导致其转化为活性物种的含量相对减少, 所以其催化活性下降.

关键词: 1,1,1,2-四氟乙烷, 氟化, CrOx-Y2O3催化剂, CrOx物种

Abstract: The synthesis of 1,1,1,2-tetrafluoroethane from 2-chloro-1,1,1-trifluoroethane was performed over CrOx-Y2O3 catalysts prepared by a co-precipitation method. The effect of yttrium precursor on the CrOx species was investigated. The catalysts were prepared using hydroxide, chloride, and nitrate yttrium precursors and were denoted as CrYO-H, CrYO-Cl, and CrYO-N, respectively. After the pre-fluorination these catalycts were denoted as CrYF-H, CrYF-Cl, and CrYF-N, respectively. Catalytic activity decreased in the following order: CrYF-H>CrYF-Cl>CrYF-N. The highest activity obtained for the CrYF-H catalyst could be attributed to the highest content of Cr(VI) on the catalyst surface. This species then transformed into an active species such as CrOxFy or Cr(OH)xFy during the activation process. The presence of CrF3, which originated fromthe Cr(VI), resulted in decreased activity.

Key words: 1,1,1,2-Tetrafluoroethane, Fluorination, CrOx-Y2O3 catalyst, Chromiumoxide species