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Vapor-Phase Hydrodeoxygenation of Guaiacol to Aromatics over Pt/HBeta: Identification of the Role of Acid Sites and Metal Sites on the Reaction Pathway

机译:Pt / hbeta芳族酚对芳烃的气相加氢脱氧:鉴定酸性位点和金属位点对反应途径的作用

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A comparative study of the hydrodeoxygenation of guaiacol, a phenolic compound derived from the lignin fraction of biomass with both hydroxyl and methoxyl functional groups, was performed on HBeta, Pt/SiO2, and Pt/HBeta at 350 degrees C and atmospheric pressure. The reaction pathway and the roles of the acid and metal sites were studied. Acid sites catalyze transalkylation and dehydroxylation reactions to produce monohydroxyl phenolics (phenol, cresols, and xylenols) as the major final products. Pt sites catalyze demethylation to result in catechol as the primary product, which can either be deoxygenated to phenol followed by phenol to benzene, or decarbonylated to cyclopentanone and further to butane. The close proximity of Pt and acid sites in bifunctional Pt/HBeta improves transalkylation and deoxygenation (or dehydroxylation) reactions and inhibits demethylation and decarbonylation reactions significantly, which leads to aromatics as the major final products with a total yield 85%. Both the activity and stability of bifunctional Pt/HBeta during the hydrodeoxygenation of guaiacol are improved compared to those of HBeta and Pt/SiO2. The addition of water to the feed further improves the activity and stability through the hydrolysis of the O-CH3 bond of guaiacol on acid sites and the removal of coke around Pt.
机译:在Hbeta,Pt / SiO 2和350℃下的Hbeta,Pt / SiO 2和Pt / Hbeta上进行GuaiaCol的水冰醇的比较研究,衍生自羟基和甲氧基官能团的生物质的木质素级分,在350℃和大气压下进行。研究了反应途径和酸和金属位点的作用。酸性位点催化烷基化和脱羟基化反应,以生产单羟基酚醛(苯酚,甲酚和木糖)作为主要的最终产物。 Pt位点催化去甲基化以导致儿茶酚作为初级产物,其可以是脱氧为苯酚,然后是苯酚,或脱羰基环戊酮并进一步向丁烷。 Pt和酸部位在双官能Pt / hbeta中的紧密接近改善了烷基化和脱氧(或脱羟基化)反应,并显着抑制去甲基化和脱羰反应,这导致芳烃作为主要最终产物,总产量& 85%。与Hbeta和Pt / SiO2相比,Guaiacol加氢脱氧过程中双官能Pt / hbeta的活性和稳定性均得到改善。进料中的水进一步通过水解Guaiacol对酸性位点的O-CH3键的活性和稳定性,并在Pt周围除去焦炭。

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