Chemical Industry and Engineering Progress ›› 2021, Vol. 40 ›› Issue (1): 242-246.DOI: 10.16085/j.issn.1000-6613.2020-0510

• Industrial catalysis • Previous Articles     Next Articles

Preparation of chlorine-free CuY catalysts by vapour impregnation and their application for oxidative carbonylation

Yuchun WANG1(), Zhaorong LIU1, Chao TAN2, Hong SUN1, Zhong LI3   

  1. 1.Department of Applied Chemistry, Yuncheng University, Yuncheng 044000, Shanxi, China
    2.Key Lab of Process Analysis and Control of Sichuan Universities, Yibin University, Yibin 644000, Sichuan, China
    3.Key Laboratory of Coal Science and Technology, Ministry of Education and Shanxi Province, Taiyuan University of Technology, Taiyuan 030024, Shanxi, China
  • Received:2020-04-03 Online:2021-01-12 Published:2021-01-05
  • Contact: Yuchun WANG

蒸气浸渍法制备完全无氯CuY催化剂及其氧化羰基化性能

王玉春1(), 刘赵荣1, 谭超2, 孙鸿1, 李忠3   

  1. 1.运城学院应用化学系,山西 运城 044000
    2.宜宾学院过程分析与控制四川省高校重点实验室,四川 宜宾 644000
    3.太原理工大学煤科学与技术教育部和山西省重点实验室,山西 太原 030024
  • 通讯作者: 王玉春
  • 作者简介:王玉春(1980—),女,副教授,从事碳一化学及多相催化研究。E-mail:wyc0104@126.com
  • 基金资助:
    过程分析与控制四川省高校重点实验室项目(2019004);运城学院应用基础研究项目(CY-2019032);运城学院博士科研启动项目(YQ-2019024);运城学院学科研究项目(XK-2019018)

Abstract:

CuY catalysts were prepared by vapour impregnation with copper acetylacetonate as the copper source and NH4Y zeolite as the support. The performance of the catalysts was evaluated by using direct vapor-phase oxidative carbonylation of methanol to dimethyl carbonate (DMC) as a model reaction. The surface dispersion, active component content, acid strength and concentration of the as-prepared catalysts were characterized by X-ray diffraction (XRD), H2-temperature programmed reduction (H2-TPR) and NH3-temperature programmed desorption (NH3-TPD), respectively. It was found that copper species were highly dispersed on the Y zeolite and the crystal structure of the Y zeolite remained intact. For the CuY/250 catalyst activated at 250℃ and in the atmosphere of N2∶H2=12∶1, the active component content was the highest and the catalytic activity was excellent. The obtained methanol conversion, space time yield and selectivity of dimethyl carbonate were 11.1%, 200.5mg/(g·h) and 60.3% respectively.

Key words: vapour impregnation, CuY catalyst, preparation, oxidative carbonylation of methanol, dimethyl carbonate

摘要:

以具有升华性质且易分解的乙酰丙酮铜为铜源,NH4Y分子筛为载体,采用蒸气浸渍法制备了CuY催化剂,考察了其对甲醇氧化羰基化合成碳酸二甲酯的催化性能,并采用XRD、H2-TPR和NH3-TPD等表征手段研究了催化剂上铜物种的分散状态、催化活性中心的含量及催化剂的酸强度和浓度,发现铜物种在Y分子筛载体上高度分散,且Y分子筛载体的晶体结构保持完好。在N2∶H2=12∶1的气氛中,250℃还原得到的催化剂CuY/250催化活性中心含量最高,催化活性也达到了最佳,其甲醇转化率为11.1%,碳酸二甲酯的时空收率和选择性分别为200.5mg/(g·h)和60.3%。

关键词: 蒸气浸渍, CuY催化剂, 制备, 甲醇氧化羰基化, 碳酸二甲酯

CLC Number: 

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