Liquid-phase glycerol hydrogenolysis to 1,2-propanediol under nitrogen pressure using 2-propanol as hydrogen source
Liquid-phase glycerol hydrogenolysis to 1,2-propanediol under nitrogen pressure using 2-propanol as hydrogen source
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DOI：
10.1016/j.jcat.2011.06.020
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发表时间：
2011-08
影响因子：
7.3
通讯作者：
I. Gandarias;P. Arias;J. Requies;M. E. Doukkali;M. B. Güemez
中科院分区：
文献类型：
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作者：
I. Gandarias;P. Arias;J. Requies;M. E. Doukkali;M. B. Güemez
研究了异丙醇作为供氢分子，在氮气压力下，以Al_2O_3为载体负载镍和铜的转移加氢反应，选择性地将甘油转化为1，2-丙二醇。并与相同操作条件下H_2压力下的结果进行了比较。活性测试和催化剂表征技术(氮气物理吸附、氢气化学吸附、NH3的TPD、TPR、TPO和XPS)的结果表明，甘油氢解生成1，2-丙二醇是通过不同的氢物种来源的机理进行的。当溶解的分子氢解离产生原子氢时，甘油首先脱水为丙醇，然后加氢为1，2-丙二醇。另一方面，当异丙醇脱氢产生氢原子时，甘油通过中间醇生成直接转化为1，2-丙二醇。
2-Propanol was studied as a hydrogen donor molecule in the transfer hydrogenation process to selectively convert glycerol into 1,2-propanediol under N2pressure and using Ni or/and Cu supported on Al2O3catalysts. The results were compared to those obtained under the same operating conditions but under H2pressure. The results of the activity tests and catalyst characterization techniques (N2-physisorption, H2-chemisorption, TPD of NH3, TPR, TPO and XPS) suggest that glycerol hydrogenolysis to yield 1,2-propanediol occurred through a different mechanism regarding the origin of the hydrogen species. When atomic hydrogen came from dissolved molecular hydrogen dissociation, glycerol was first dehydrated to acetol and then hydrogenated to 1,2-propanediol. On the other hand, when the hydrogen atoms were produced from 2-propanol dehydrogenation, glycerol was directly converted to 1,2-propanediol through intermediate alkoxide formation.