Thermodynamic Analysis and Experimental Study of Selective Dehydrogenation of 1,2-cyclohexanediol over Cu<sub>2+1</sub>O/MgO Catalysts

The dehydrogenation of 1,2-cyclohexanediol (CHD) helps in the effective utilization of not only fossil derivatives but also vicinal diols and polyols from sustainable biomass-derived resources. A thermodynamic analysis of CHD dehydrogenation was computed with density functional theory (DFT) calculat...

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Bibliographic Details
Main Authors: Haiou Wang, Qiusheng Yang, Yucong Song, Yanji Wang
Format: Article
Language:English
Published: MDPI AG 2019-02-01
Series:Sustainability
Subjects:
Online Access:https://www.mdpi.com/2071-1050/11/3/902
Description
Summary:The dehydrogenation of 1,2-cyclohexanediol (CHD) helps in the effective utilization of not only fossil derivatives but also vicinal diols and polyols from sustainable biomass-derived resources. A thermodynamic analysis of CHD dehydrogenation was computed with density functional theory (DFT) calculation using Gaussian 09. The result indicates that CHD can be converted to 2-hydroxy cyclohexanone (HCO), 2-hydroxy-2-cyclohexen-1-one (HCEO) and pyrocatechol depending on the degree of dehydrogenation. HCO and HCEO are the stable products of the primary and secondary dehydrogenation. Experimentally, Cu/MgO catalysts were prepared using glucose as a reductant, and were characterized by SEM, TEM, XRD, XPS, TPR, BET and ICP. Furthermore, their catalytic performance regarding the oxygen-free dehydrogenation of CHD was investigated. The results indicate that the primary active crystalline phase of Cu/MgO was Cu<sub>2+1</sub>O, and that the dehydrogenation products were mainly HCO and HCEO, in accordance with thermodynamic predictions. Upon optimizing the reaction conditions, the total selectivity of HCO and HCEO exceeded 90% and the conversion of CHD was approximately 95%.
ISSN:2071-1050