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合成气制备高级醇的现状与展望。

Status and prospects in higher alcohols synthesis from syngas.

机构信息

Institute for Chemical and Bioengineering, Department of Chemistry and Applied Biosciences, ETH Zurich, HCI E125, Vladimir-Prelog-Weg 1, CH-8093 Zurich, Switzerland.

Total Research & Technology Feluy, Zone Industrielle Feluy C, B-7181 Seneffe, Belgium.

出版信息

Chem Soc Rev. 2017 Mar 6;46(5):1358-1426. doi: 10.1039/c6cs00324a.

Abstract

Higher alcohols are important compounds with widespread applications in the chemical, pharmaceutical and energy sectors. Currently, they are mainly produced by sugar fermentation (ethanol and isobutanol) or hydration of petroleum-derived alkenes (heavier alcohols), but their direct synthesis from syngas (CO + H) would comprise a more environmentally-friendly, versatile and economical alternative. Research efforts in this reaction, initiated in the 1930s, have fluctuated along with the oil price and have considerably increased in the last decade due to the interest to exploit shale gas and renewable resources to obtain the gaseous feedstock. Nevertheless, no catalytic system reported to date has performed sufficiently well to justify an industrial implementation. Since the design of an efficient catalyst would strongly benefit from the establishment of synthesis-structure-function relationships and a deeper understanding of the reaction mechanism, this review comprehensively overviews syngas-based higher alcohols synthesis in three main sections, highlighting the advances recently made and the challenges that remain open and stimulate upcoming research activities. The first part critically summarises the formulations and methods applied in the preparation of the four main classes of materials, i.e., Rh-based, Mo-based, modified Fischer-Tropsch and modified methanol synthesis catalysts. The second overviews the molecular-level insights derived from microkinetic and theoretical studies, drawing links to the mechanisms of Fischer-Tropsch and methanol syntheses. Finally, concepts proposed to improve the efficiency of reactors and separation units as well as to utilise CO and recycle side-products in the process are described in the third section.

摘要

高级醇是一类具有广泛应用的重要化合物,在化学、制药和能源领域都有应用。目前,它们主要通过糖发酵(乙醇和异丁醇)或石油衍生烯烃的水合(更重的醇)来生产,但如果能直接从合成气(CO+H)合成,将是一种更环保、更通用、更经济的替代方法。自 20 世纪 30 年代以来,该反应的研究工作一直随着石油价格的波动而波动,而在过去十年中,由于有兴趣利用页岩气和可再生资源来获得气态原料,其研究工作大大增加。然而,迄今为止,没有报道的催化体系表现得足够好,无法证明其具有工业实施的可行性。由于设计高效催化剂将强烈受益于建立合成-结构-功能关系,并深入了解反应机制,因此,这篇综述从三个主要部分全面概述了基于合成气的高级醇合成,突出了最近取得的进展以及仍然存在的挑战,并激发了即将开展的研究活动。第一部分批判性地总结了四类主要材料(铑基、钼基、改性费托和改性甲醇合成催化剂)的制备配方和方法。第二部分综述了从微观动力学和理论研究中得出的分子水平见解,并将这些见解与费托合成和甲醇合成的机制联系起来。最后,第三部分描述了提高反应器和分离单元效率以及在该过程中利用 CO 和回收副产物的概念。

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