石油化工高等学校学报

石油化工高等学校学报 ›› 2021, Vol. 34 ›› Issue (2): 29-34.DOI: 10.3969/j.issn.1006-396X.2021.02.005

• 能源化工 • 上一篇    下一篇

RuHI(CO)(i⁃Pr⁃Imidazole)(PPh3)2催化甲醇水重整产氢

齐卫卫1秦雷2周明东1郑智平2   

  1. 1. 辽宁石油化工大学 石油化工学院,辽宁 抚顺 113001; 2. 南方科技大学 化学系,广东 深圳 518055
  • 收稿日期:2020-04-14 修回日期:2020-10-23 出版日期:2021-04-30 发布日期:2021-05-20
  • 通讯作者: 周明东(1980-),女,博士,教授,博士生导师,从事金属有机化学研究;E-mail:mingdong.zhou@lnpu.edu.cn。
  • 作者简介:齐卫卫(1992-),女,硕士研究生,从事金属有机化学研究;E-mail:1044462577@qq.com。
  • 基金资助:
    中国博士后科学基金项目(2018M640226)。

Hydrogen Production by RuHI(CO)(i⁃Pr⁃Imidazole)(PPh3)2 Catalyzed Aqueous Methanol Reforming

Qi Weiwei1Qin Lei2Zhou Mingdong1Zheng Zhiping2   

  1. 1. School of Petrochemical Engineering, Liaoning Petrochemical University, Fushun Liaoning 113001,China; 2. South University of Science and Technology, Shenzhen Guangdong 518055,China
  • Received:2020-04-14 Revised:2020-10-23 Published:2021-04-30 Online:2021-05-20

摘要: H2的高效储存和输运是限制整个氢能源体系发展的瓶颈。一种有效解决这一难题的方法是将H2存储于液体有机载体甲醇中,需要时通过水和甲醇的液相重整反应,原位释放H2,而这一过程能够实现的关键在于高效甲醇水重整催化剂的开发。以1⁃异丙基咪唑和RuHCl(CO)(PPh3)3为原料,合成了化合物RuHI(CO)(i⁃Pr⁃Imidazole)(PPh3)2,对其进行了元素分析、红外光谱和X射线单晶衍射表征,并将其用于均相催化甲醇重整产氢。单晶结构表明,该配合物为单核,中心离子Ru2+为六配位,呈现扭曲的八面体配位构型。通过对催化反应条件的筛选,发现反应温度、碱的类型以及V(MeOH)/V(H2O)等对催化效率具有极大的影响。经反应条件优化,在反应温度为110 ℃,8 mol/L KOH和V(MeOH) /V(H_2 O)=9∶1,催化剂物质的量为4 μmol的条件下持续反应14 d,TON达到了7 911。

关键词: 催化剂, 甲醇重整, H2,

Abstract: Efficient storage and transportation of hydrogen are the bottlenecks limiting the development of hydrogen economy. One effective way to solve this problem is to store hydrogen in liquid organic hydrogen carriers, such as methanol, which can be released from the organic hydrogen carriers as H2 gas after catalyzed reforming process. The main challenge during this procedure is the development of catalysts capable of executing such a decomposition process. In this work, a novel organometallic compound RuHI(CO)(i⁃Pr⁃Imidazole)(PPh3)2 was synthesized and explored its catalytic applications for hydrogen production during aqueous methanol reforming. The compound was characterized by elemental analysis, infrared spectroscopy, and single⁃crystal X⁃ray diffraction for determining its cystalline structure. The results indicate that the organometallic compound, shows mononuclear structure with six⁃coordinated ruthenium ion in its network, forming the twisted octahedral configuration in the compound. It has been found that reaction conditions such as temperature, the type of alkali, the volume ratio of MeOH and H2O, have profound effects on the reaction efficiencies. Under optimized conditions (110 ℃, 8 mol/L KOH, V(MeOH)/V(H2O)=9∶1),4 μmol the catalyst produces a accumulated TON of 7 9:1 after a 14-day reaction.

Key words: Catalyst, Methanol reforming, Hydrogen, Ruthenium

引用本文

齐卫卫, 秦雷, 周明东, 郑智平. RuHI(CO)(i⁃Pr⁃Imidazole)(PPh3)2催化甲醇水重整产氢[J]. 石油化工高等学校学报, 2021, 34(2): 29-34.

Qi Weiwei, Qin Lei, Zhou Mingdong, Zheng Zhiping. Hydrogen Production by RuHI(CO)(i⁃Pr⁃Imidazole)(PPh3)2 Catalyzed Aqueous Methanol Reforming[J]. Journal of Petrochemical Universities, 2021, 34(2): 29-34.

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