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An ordinary nickel catalyst becomes completely selective for partial hydrogenation of 1,3-butadiene when coated with tributyl(methyl)phosphonium methyl sulfate
Applied Catalysis A: General ( IF 5.5 ) Pub Date : 2018-06-15 , DOI: 10.1016/j.apcata.2018.06.016
Ahsan Jalal , Alper Uzun

Performance of an ordinary supported nickel catalyst was tuned to reach an almost complete selectivity for partial hydrogenation of 1,3-butadiene by coating it with a phosphonium-type ionic liquid (IL), tributyl(methyl)phosphonium methyl sulfate, [P4441][MeSO4]. Thanks to high chemical and thermal stability of [P4441][MeSO4], the reaction conditions could be pre-optimized for high partial hydrogenation performance before the deposition of the IL coating. When the catalyst was coated with IL, it provided a total butene selectivity of 99.5 ± 0.2%, a record high partial hydrogenation selectivity ever reported for a nickel-based catalyst. X-ray photoelectron spectroscopy results illustrated that the IL donates electrons to nickel sites and makes them selective for partial hydrogenation. The conductor like screening model for realistic solvents (COSMO-RS) calculations indicated that the IL coating also exerts a filter effect, which helps to maintain this high partial hydrogenation selectivity at all conversion levels.



中文翻译:

当用三丁基(甲基)phosph甲基硫酸盐涂覆时,普通的镍催化剂对1,3-丁二烯的部分加氢具有完全的选择性。

通过用with型离子液体(IL),三丁基(甲基)methyl甲基硫酸甲酯,[P 4441 ]涂覆,可以调节普通负载型镍催化剂的性能,以实现几乎完全的1,3-丁二烯部分加氢的选择性。[MeSO 4 ]。由于[P 4441 ] [MeSO 4的高化学稳定性和热稳定性可以在沉积IL涂层之前预先优化反应条件以实现较高的部分氢化性能。当用IL涂覆催化剂时,它提供的总丁烯选择性为99.5±0.2%,这是镍基催化剂所记录的最高的部分氢化选择性。X射线光电子能谱的结果表明,IL将电子提供给镍位,并使它们对部分氢化具有选择性。用于实际溶剂的类似导体的筛选模型(COSMO-RS)计算表明,IL涂层也具有过滤作用,这有助于在所有转化水平下均保持较高的部分氢化选择性。

更新日期:2018-06-15
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