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Au/ZrO 催化剂上 5-羟甲基糠醛选择性氢解制备 2-己醇

Selective Hydrogenolysis of 5-Hydroxymethylfurfural to 2-Hexanol over Au/ZrO Catalysts.

机构信息

Guangzhou Institute of Energy Conversion, Chinese Academy of Sciences, Guangzhou, 510640, P. R. China.

CAS Key Laboratory of Renewable Energy, Guangdong Provincial Key Laboratory of New and Renewable Energy Research and Development, Guangzhou, 510640, P. R. China.

出版信息

ChemSusChem. 2022 Jul 7;15(13):e202200092. doi: 10.1002/cssc.202200092. Epub 2022 May 13.

Abstract

2-Hexanol (2-HOL) is a versatile biomass-derived platform molecule for synthesis of liquid transportation fuels, lubricants, or detergents. Herein, a one-step preparation of 2-HOL using 5-hydroxymethylfurfural (HMF) as a substrate was reported for the first time. Several Au-based catalysts supported on different metal oxides were prepared to explore the relationship between carrier and catalytic activity. The results showed that the highest 2-HOL yield of 65.8 % was obtained at complete HMF conversion over the 5 %Au/ZrO catalyst. The 5 %Au/ZrO catalyst exhibited excellent durability after five consecutive recycling runs, while confirming its remarkable ring-opening hydrogenolysis on other biomass-derived furanics, furfural, with a total yield of 1-pentanol and 2-pentanol of 67.4 %. The distinguished ring-opening hydrogenolysis performance of the Au/ZrO catalyst originated from a synergistic effect between the interfacial Au-O-Zr oxygen vacancies-induced Lewis acidic sites (activating C-OH/C=O bonds) and metallic Au (activating H ). This work provides a possibility for producing 2-HOL from HMF with high yield, expanding the sustainable application of lignocellulosic biomass.

摘要

2-己醇(2-HOL)是一种多功能的生物质衍生平台分子,可用于合成液体运输燃料、润滑剂或清洁剂。本文首次报道了以 5-羟甲基糠醛(HMF)为底物一步法制备 2-HOL 的方法。制备了几种负载在不同金属氧化物上的 Au 基催化剂,以探究载体与催化活性之间的关系。结果表明,在完全转化 HMF 的情况下,5%Au/ZrO 催化剂上 2-HOL 的最高收率为 65.8%。5%Au/ZrO 催化剂在连续五次循环回收后表现出优异的稳定性,同时在其他生物质衍生呋喃类化合物糠醛的开环氢解反应中也表现出了优异的总收率 1-戊醇和 2-戊醇为 67.4%。Au/ZrO 催化剂的开环氢解性能优异源于界面 Au-O-Zr 氧空位诱导的路易斯酸性位(活化 C-OH/C=O 键)和金属 Au(活化 H)之间的协同作用。这项工作为高收率地从 HMF 生产 2-HOL 提供了可能,扩展了木质纤维素生物质的可持续应用。

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