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Control of selectivity, activity and durability of simple supported nickel catalysts for hydrolytic hydrogenation of cellulose

机译:控制纤维素水解加氢的简单负载型镍催化剂的选择性,活性和耐久性

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摘要

Efficient conversion of cellulose to sorbitol and mannitol by base metal catalysts is a challenge in green and sustainable chemistry, but typical supported base metal catalysts have not given good yields of hexitols or possessed durability. In this study, it has been demonstrated that a simple carbon-supported Ni catalyst affords up to 67% yield of hexitols in the conversion of cellulose, and that the catalyst is durable in the reuse experiments 7 times. In addition, the catalyst can be separated by a magnet thanks to a high content of Ni. Physicochemical analysis has indicated that the use of carbon supports has two benefits: no basicity and high water-tolerance. CeO2, ZrO2, gamma-Al2O3 and TiO2 cause side-reactions due to basicity, and SiO2, gamma-Al2O3 and CeO2 are less stable in hot water. Another important factor is high Ni loading as the increase of Ni content from 10 wt% to 70 wt% significantly improves the yield of hexitols and the durability of catalysts. Larger crystalline Ni particles are more resistant to sintering of Ni and surface coverage by Ni oxide species.
机译:贱金属催化剂有效地将纤维素转化为山梨糖醇和甘露醇是绿色和可持续化学领域的挑战,但是典型的负载型贱金属催化剂不能提供良好的己糖醇收率或耐久性。在这项研究中,已证明简单的碳载Ni催化剂在纤维素转化中可提供高达67%的己糖醇收率,并且该催化剂在重复使用实验中具有7倍的耐用性。此外,由于镍含量高,催化剂可以用磁铁分离。物理化学分析表明,使用碳载体有两个好处:无碱和高耐水性。 CeO2,ZrO2,γ-Al2O3和TiO2由于碱性而引起副反应,而SiO2,γ-Al2O3和CeO2在热水中不稳定。另一个重要因素是高Ni负载量,因为Ni含量从10 wt%增加到70 wt%可以显着提高己糖醇的收率和催化剂的耐久性。较大的结晶Ni颗粒更能抵抗Ni的烧结和Ni氧化物物种的表面覆盖。

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