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Hydrodeoxygenation of Lignin‐Derived Monomers and Dimers over a Ru Supported Solid Super Acid Catalyst for Cycloalkane Production
Advanced Sustainable Systems ( IF 7.1 ) Pub Date : 2020-06-30 , DOI: 10.1002/adsu.201900136
Xing Zhang 1 , Hui Yan 1 , Lingjun Zhu 1 , Tian Li 1 , Shurong Wang 1
Affiliation  

The monomers and dimers produced via lignin depolymerization are a promising alternative to transportation fuels after hydrodeoxygenation (HDO). However, these compounds contain numerous oxygen‐containing functional groups that are strongly bonded to aromatic rings. Therefore, the conventional HDO of lignin‐derived compounds faces serious problems of catalyst deactivation due to coke deposition and low hydrocarbon yields. A metal–solid super acid catalyst, i.e., Ru(SO42−)/ZrO2–CeO2, is synthesized, characterized, and evaluated for the HDO of various lignin‐derived monomers and dimers in a biphasic n‐dodecane/H2O system. A high cyclohexane yield of 98.5% is obtained by the HDO of phenol performed at 200 °C and 5 MPa. The “hydrated” configuration can be formed between the hydrogenation intermediates and H2O on the Ru sites. In addition, the anionic vacancies of ZrO2–CeO2 can be occupied by H derived from the heterolytic cleavage of H2, leading to the formation of metal hydrides. The strong acidity of SO42−/ZrO2–CeO2 is beneficial for the subsequent deoxygenation of the hydrotreated products. In addition, the biphasic system can minimize the side reactions induced by the strong acidity of the catalyst. The catalytic system also exhibits a good catalytic performance for the HDO of other lignin‐derived monomers and dimers to produce cycloalkanes.

中文翻译:

木质素衍生的单体和二聚体在Ru负载的固体超强酸催化剂上进行环烷烃加氢脱氧

通过木质素解聚生产的单体和二聚体是加氢脱氧(HDO)后运输燃料的有前途的替代品。但是,这些化合物包含许多与芳环牢固结合的含氧官能团。因此,由于焦炭沉积和低烃产率,木质素衍生化合物的常规HDO面临催化剂失活的严重问题。在双相十二烷/ H中合成,表征并评估了金属-固体超强酸催化剂,即Ru(SO 4 2-)/ ZrO 2 -CeO 2,并评估了各种木质素衍生的单体和二聚物的HDO。2O系统。通过在200°C和5 MPa下进行的苯酚HDO,可获得98.5%的高环己烷收率。可以在Ru部位的氢化中间体和H 2 O之间形成“水合”构型。此外,的ZrO的阴离子空位2 -CeO 2可以由H被占用-从H的异裂衍生2,导致的金属氢化物的形成。SO 4 2− / ZrO 2 –CeO 2的强酸性对于加氢产物的后续脱氧是有利的。另外,双相体系可以使由催化剂的强酸性引起的副反应最小化。该催化体系对其他木质素衍生单体和二聚体的HDO表现出良好的催化性能,可生产环烷烃。
更新日期:2020-06-30
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