Li Xiaomin, Du Zhengjiang, Wu Yi, Zhen Yadong, Shao Rixin, Li Bingqi, Chen Chengmeng, Liu Quansheng, Zhou Huacong
College of Chemical Engineering, Inner Mongolia University of Technology, Inner Mongolia Key Laboratory of High-Value Functional Utilization of Low Rank Carbon Resources Hohhot 010051 Inner Mongolia China
CAS Key Laboratory of Carbon Materials, Institute of Coal Chemistry, Chinese Academy of Sciences China.
RSC Adv. 2020 Mar 9;10(17):9985-9995. doi: 10.1039/c9ra10795a. eCollection 2020 Mar 6.
Construction and application of novel hydrogenation catalysts is important for the conversion of carbonyl or aldehyde compounds into alcohols in the field of biomass utilization. In this work, a novel, efficient, and easily prepared hafnium-graphite oxide (Hf-GO) catalyst was constructed the coordination between Hf and the carboxylic groups in GO. The catalyst was applied into the hydrogenation of biomass derived carbonyl compounds the Meerwein-Ponndorf-Verley (MPV) reaction. The catalyst gave high efficiency under mild conditions. An interesting phenomenon was found whereby the activity of the catalyst increased gradually in the initial stage during reaction. The solvent, isopropanol, was proved to have an activation effect on the catalyst, and the activation effect varied with different alcohols and temperatures. Further characterizations showed that isopropanol played the activation effect replacing the residual solvent (DMF) in micro- and mesopores during the preparation process, which was hard to be completely removed by common drying process.
新型氢化催化剂的构建与应用对于生物质利用领域中羰基或醛类化合物转化为醇类至关重要。在本工作中,通过铪与氧化石墨烯(GO)中羧基之间的配位作用,构建了一种新型、高效且易于制备的铪-氧化石墨烯(Hf-GO)催化剂。该催化剂被应用于生物质衍生羰基化合物的氢化反应——迈耶-庞多夫-韦利(MPV)反应。该催化剂在温和条件下具有高效率。发现了一个有趣的现象,即在反应初始阶段催化剂的活性逐渐增加。事实证明,溶剂异丙醇对催化剂具有活化作用,且活化作用随不同醇类和温度而变化。进一步表征表明,异丙醇通过在制备过程中取代微孔和介孔中的残留溶剂(DMF)发挥活化作用,而残留溶剂难以通过常规干燥过程完全去除。