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Selective Vanillin Hydrodeoxygenation on Synthetic Takovite Derived NiAlO x Mixed Oxide
Topics in Catalysis ( IF 3.6 ) Pub Date : 2020-04-01 , DOI: 10.1007/s11244-020-01261-8
Luis F. Vázquez-Fuentes , M. A. Cortés-Jacome , E. López-Salinas , Jaime S. Valente , P. Morales Gil , J. G. Hernández-Cortez , José A. Toledo-Antonio

Abstract

A mixed metal-oxide (NiAlOx) obtained from the annealing of a synthetic takovite clay, [(Ni6Al2(OH)16]CO3·4H2O, was used as a catalyst in the hydrodeoxygenation reaction of vanillin, as a model molecule, to simulate deoxygenation of lignin's moieties. The catalysts were characterized by XRD, TPR, XPS and textural analyses and were tested at between 413 and 573 K and 1.2 MPa H2, using a 300 ml batch reactor. The reaction products were analyzed using a gas-chromatograph coupled to a mass detector (GC–MS). The active site is visualized as a Niδ+–O–Al3+ moieties able to dissociate molecular H2 into highly reactive species (H and H+) for hydrogenation reactions. Depending on the reaction temperature, decarbonylation, hydrogenation, demethoxylation and dehydroxylation reactions occurred in three stages as clearly indicated by Van-Krevelen O/C* vs. H/C* plots. Our study points out that total deoxygenation can be attained at 553 K with a 100% selectivity to products like methyl-cyclohexane and cyclohexane.

Graphic Abstract



中文翻译:

合成Takovite衍生NiAlO x混合氧化物的选择性香兰素加氢脱氧

摘要

在香兰素的加氢脱氧反应中,将合成的塔科维粘土的[[(Ni 6 Al 2(OH)16 ] CO 3 ·4H 2 O )退火得到的混合金属氧化物(NiAlO x)被用作催化剂。用XRD,TPR,XPS和结构分析对催化剂进行了表征,并使用300 ml分批反应器在413和573 K和1.2 MPa H 2之间进行了测试。使用与质谱检测器(GC-MS)联用的气相色谱仪进行分析,将活性位点可视化为能够解离分子H 2的Niδ+ -O-Al 3+部分成高反应性物质(H -和H +)用于氢化反应。Van-Krevelen O / C *与H / C *曲线清楚地表明,取决于反应温度,脱羰,氢化,脱甲氧基和脱羟基反应分三个阶段进行。我们的研究指出,可以在553 K下实现完全脱氧,并且对甲基环己烷和环己烷等产品具有100%的选择性。

图形摘要

更新日期:2020-04-22
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