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Transformation of CO2 with glycerol to glycerol carbonate by a novel ZnWO4-ZnO catalyst
Journal of CO2 Utilization ( IF 7.7 ) Pub Date : 2018-05-30 , DOI: 10.1016/j.jcou.2018.05.025
Jiaxiong Liu , Dehua He

ZnWO4-ZnO catalysts with different W content were prepared by conventional hydrothermal and wet impregnation methods and applied in the direct synthesis of glycerol carbonate from CO2 and glycerol. The crystallite structure, texture property, morphology, redox and acid-base properties and the surface chemical situation of the catalysts were characterized by XRD, BET, TEM, H2-TPR, NH3/CO2-TPD and XPS. The possible activation routes of CO2 and glycerol were analyzed with DRIFTS and FTIR. ZnWO4-ZnO composite catalysts showed better catalytic performances with respect to ZnO in the carbonylation of glycerol with CO2. The improved activity of ZnWO4-ZnO catalysts was associated with the formation of ZnWO4, the interaction between ZnWO4 and ZnO, and the enhanced moderate acidic property. DIRFTS results showed that chelating bidentate carbonate species was the main adsorption pattern for CO2 on ZnO, while the introduction of W led to the bridged bidentate carbonate, which became the main adsorption pattern on ZnWO4-ZnO. As for the activation of glycerol, zinc glycerolate played an important role in the reaction process. Based on the reaction and characterization results, a plausible reaction route involved a seven-membered ring esters intermediate was suggested for the reaction of CO2 and glycerol over ZnWO4-ZnO catalysts.



中文翻译:

新型ZnWO 4 -ZnO催化剂将甘油将CO 2转化为碳酸甘油酯。

采用常规的水热湿法浸渍法制备了不同W含量的ZnWO 4 -ZnO催化剂,并将其用于由CO 2和甘油直接合成碳酸甘油酯。通过XRD,BET,TEM,H 2 -TPR,NH 3 / CO 2 -TPD和XPS对催化剂的微晶结构,织构性质,形貌,氧化还原和酸碱性质以及表面化学性质进行了表征。用DRIFTS和FTIR分析了CO 2和甘油的可能活化途径。ZnWO 4 -ZnO复合催化剂在甘油与CO 2羰基化反应中表现出比ZnO更好的催化性能。。ZnWO的改善的活性4 -ZnO催化剂用ZnWO的形成相关联的4,ZnWO之间的相互作用4和ZnO,和增强的温和酸性。DIRFTS结果表明,螯合碳酸二齿碳酸盐种类是ZnO上CO 2的主要吸附模式,而W的引入导致桥接的碳酸二齿碳酸盐,这成为ZnWO 4 -ZnO上的主要吸附模式。至于甘油的活化,甘油酸锌在反应过程中起重要作用。根据反应和表征结果,提出了一种可行的反应路线,该路线涉及七元环酯中间体,用于CO 2的反应。甘油和ZnWO 4 -ZnO催化剂上的甘油。

更新日期:2018-05-30
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