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贵金属催化的木质素热解油及相关模型化合物的水相加氢和加氢脱氧反应。

Noble metal catalyzed aqueous phase hydrogenation and hydrodeoxygenation of lignin-derived pyrolysis oil and related model compounds.

机构信息

School of Chemical and Biomolecular Engineering, Renewable Bioproducts Institute, Georgia Institute of Technology, Atlanta, GA 30318, United States.

Department of Chemistry and Biochemistry, Institute of Paper Science and Technology, Georgia Institute of Technology, Atlanta, GA 30318, United States.

出版信息

Bioresour Technol. 2014 Dec;173:6-10. doi: 10.1016/j.biortech.2014.09.067. Epub 2014 Sep 22.

DOI:10.1016/j.biortech.2014.09.067
PMID:25280108
Abstract

Aqueous phase hydrodeoxygenation of lignin pyrolysis oil and related model compounds were investigated using four noble metals supported on activated carbon. The hydrodeoxygenation of guaiacol has three major reaction pathways and the demethylation reaction, mainly catalyzed by Pd, Pt and Rh, produces catechol as the products. The presence of catechol and guaiacol in the reaction is responsible for the coke formation and the catalysts deactivation. As expected, there was a significant decrease in the specific surface area of Pd, Pt and Rh catalysts during the catalytic reaction because of the coke deposition. In contrast, no catechol was produced from guaiacol when Ru was used so a completely hydrogenation was accomplished. The lignin pyrolysis oil upgrading with Pt and Ru catalysts further validated the reaction mechanism deduced from model compounds. Fully hydrogenated bio-oil was produced with Ru catalyst.

摘要

采用四种负载在活性炭上的贵金属对木质素热解油及相关模型化合物的水相加氢脱氧进行了研究。愈创木酚的加氢脱氧有三条主要反应途径,其中脱甲基反应主要由 Pd、Pt 和 Rh 催化,生成邻苯二酚作为产物。反应中邻苯二酚和愈创木酚的存在是导致积碳和催化剂失活的原因。正如预期的那样,由于积碳,Pd、Pt 和 Rh 催化剂在催化反应过程中的比表面积显著下降。相比之下,当使用 Ru 时,不会从愈创木酚中生成邻苯二酚,因此可以完成完全加氢。用 Pt 和 Ru 催化剂对木质素热解油进行升级进一步验证了从模型化合物推断出的反应机制。用 Ru 催化剂得到了完全加氢的生物油。

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Molecular modeling approach to elucidate gas phase hydrodeoxygenation of guaiacol over a Pd(111) catalyst within DFT framework.在密度泛函理论(DFT)框架内,采用分子模拟方法阐明愈创木酚在Pd(111)催化剂上的气相加氢脱氧反应。
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