One-step synthesis of ethanol from glycerol in a gas phase packed bed reactor over hierarchical alkali-treated zeolite catalyst materials,Green Chemistry

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One-step synthesis of ethanol from glycerol in a gas phase packed bed reactor over hierarchical alkali-treated zeolite catalyst materials
Green Chemistry ( IF 9.3 ) Pub Date : 2019/12/19 , DOI: 10.1039/c9gc03262b
Andrii Kostyniuk _{1,

2,

3,

4} , David Bajec _{1,

2,

3,

4} , Blaž Likozar _{1,

2,

3,

4}

Affiliation

The gas-phase conversion of glycerol into ethanol in a “green” one-step synthesis over a cesium metal-promoted zeolite catalyst has been reported for the first time. To our knowledge, the CsZSM-5 based catalyst presented in this work showed one of the best yields of ethanol in the gas-phase glycerol conversion. The catalyst sample's structure, texture, and acid–base properties were characterized using numerous materials characterization techniques. The catalytic evaluation was carried out in a packed-bed continuous flow reactor. The highest ethanol yield achieved was 99.6 mol% over a 20 wt% CsZSM-5 catalyst with SiO₂/Al₂O₃ = 1500, 10 wt% glycerol feed concentration, 350 °C reaction temperature, and GHSV_total = 625 h⁻¹. It was demonstrated that the best catalytic performance was related to the ample amount of surface basic sites, synergistic interaction between Cs species and the HZSM-5 zeolite and to its smaller crystallite size obtained from XRD analysis. The achieved results exhibit great potential of utilizing the alkali-treated CsZSM-5 catalyst for the gas-phase conversion of glycerol into bio-based ethanol. The possible reaction route from glycerol to renewable ethanol was proposed based on direct glycerol conversion to ethanol via the thermal monodehydration, radical fragmentation, methylation and transfer hydrogenation reactions. Finally, for the first time, methanol was directly converted into ethanol in the gas-phase continuous flow packed-bed reactor over a 20 wt% CsZSM-5 catalyst.

中文翻译：

在分级碱处理的沸石催化剂材料上的气相填充床反应器中由甘油一步合成乙醇

首次报道了在铯金属促进的沸石催化剂上以“绿色”一步合成法将甘油气相转化为乙醇。据我们所知，这项工作中介绍的基于CsZSM-5的催化剂显示出气相甘油转化中乙醇的最佳收率之一。使用多种材料表征技术对催化剂样品的结构，质地和酸碱性质进行了表征。催化评估是在填充床连续流反应器中进行的。在具有SiO ₂ / Al ₂ O ₃ = 1500，甘油进料浓度为10 wt％，反应温度为350°C和GHSV _total = 625 h ^-1的20 wt％CsZSM-5催化剂上，获得的最高乙醇产率为99.6 mol％。。结果表明，最佳的催化性能与大量的表面碱性位点，Cs物种与HZSM-5沸石之间的协同相互作用以及通过XRD分析获得的较小的晶粒尺寸有关。所获得的结果显示出利用碱处理的CsZSM-5催化剂将甘油气相转化为生物基乙醇的巨大潜力。基于甘油通过热单脱水，自由基裂解，甲基化和转移加氢反应的直接转化为乙醇，提出了从甘油到可再生乙醇的可能反应路线。最后，第一次，在气相连续流填充床反应器中，在20 wt％CsZSM-5催化剂上将甲醇直接转化为乙醇。

更新日期：2020-02-13

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