高等学校化学学报 ›› 2020, Vol. 41 ›› Issue (4): 765-764.doi: 10.7503/cjcu20190573

• 物理化学 • 上一篇    下一篇

磷酸铈对磷化镍催化苯酚转移加氢的促进作用

孟繁星1,遇治权1,景文文1,王瑶1,2,孙志超1,王安杰1,2,*()   

  1. 1. 大连理工大学精细化工国家重点实验室, 大连 116024
    2. 辽宁省省级高校石油化工技术与装备重点实验室, 大连 11602
  • 收稿日期:2019-11-05 出版日期:2020-04-10 发布日期:2020-02-21
  • 通讯作者: 王安杰 E-mail:ajwang@dlut.edu.cn
  • 基金资助:
    国家自然科学基金(21972014, 21473017, 21603024, U1508205);中央高校基本科研业务费(DUT19GJ205);科技部国家重点研发计划项目(批准号: )资助.(2016YFE0109800)

Promoting Effect of Cerous Phosphate on the Phenol Catalytic Transfer Hydrogenation over Nickel Phosphide Catalyst

MENG Fanxing1,YU Zhiquan1,JING Wenwen1,WANG Yao1,2,SUN Zhichao1,WANG Anjie1,2,*()   

  1. 1. State Key Laboratory of Fine Chemical, Dalian University of Technology, Dalian 116024, China
    2. Liaoning Key Laboratory of Petrochemical Technology and Equipment, Dalian 116024, China
  • Received:2019-11-05 Online:2020-04-10 Published:2020-02-21
  • Contact: Anjie WANG E-mail:ajwang@dlut.edu.cn
  • Supported by:
    † Supported by the National Natural Science Foundation of China(21972014, 21473017, 21603024, U1508205);the Fundamental Research Funds for the Central Universities, China(DUT19GJ205);the National Key Research and Development Project, China(2016YFE0109800)

摘要:

通过氢气原位程序升温还原法制备了一系列不同Ce/Ni摩尔比的CePO4-Ni3P及Ni3P催化剂, 考察了其在苯酚催化转移加氢反应的催化性能. 研究了Ce/Ni摩尔比、 供氢溶剂、 反应温度和反应时间对催化剂性能的影响, 并初步考察了苯酚转移加氢的反应动力学. 研究结果表明, CePO4的加入能显著提升体相Ni3P催化苯酚转移加氢的转化率, 且Ce/Ni摩尔比为0.2时促进作用最显著; 在所考察的供氢溶剂中异丙醇展现出最好的性能; 使用CePO4(0.2)-Ni3P作为反应催化剂, 异丙醇作为供氢溶剂, 220 ℃下反应6 h, 苯酚转化率和环己醇选择性分别可达93.1%和92.0%.

关键词: 磷化镍, 磷酸铈, 转移加氢, 苯酚, 异丙醇

Abstract:

A series of CePO4-Ni3P and Ni3P catalysts with various Ce/Ni molar ratio were prepared by in-situ H2 temperature-programmed reduction, and utilized to catalyze the transfer hydrogenation of phenol. The effects of Ce/Ni molar ratio, hydrogen donors, reaction temperature and reaction time on the catalytic perfor-mance were investigated. What’s more, the reaction kinetic parameters were calculated. The reaction results showed that the addition of CePO4 could significantly improve the phenol conversion. The promoting effect was the most obvious when the Ce/Ni molar ratio was 0.2. 2-Propanol exhibited the best catalytic activity among all the screened solvents. A high cyclohexanol selectivity of 92.0% and phenol conversion of 93.1% could be obtained at 220 ℃ for 6 h over the CePO4(0.2)-Ni3P catalyst using 2-propanol as the hydrogen donor and solvent.

Key words: Ni3P, CePO4, Transfer hydrogenation, Phenol, 2-Propanol

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