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 + H2) 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 CO2 and recycle side-products in the process are described in the third section.

Status and prospects in higher alcohols synthesis from syngas

Bimetallic CoCu model catalysts were investigated for the synthesis of higher alcohols using catalytic CO hydrogenation according to the Fischer–Tropsch technology. Emphasis was placed on revealing the influence of the activation conditions. Accordingly, catalyst precursors were activated in argon, hydrogen, syngas (CO/H2), and CO under atmospheric conditions and at elevated temperatures (370 °C). All catalyst precursors were prepared via oxalate coprecipitation in the absence of a classic support. Alcohol selectivities between 30 and ∼40% (up to ∼50% for the sum of alcohols and alkenes) were obtained with an Anderson–Schulz–Flory (ASF) chain lengthening probability maximizing the slate up to C6. Detailed catalysis and characterization studies were performed using a Co2Cu1 catalyst composition. The catalytic performances of the H2- and syngas-activated Co2Cu1 catalyst were similar. While the CO-activated catalyst shows significantly higher catalytic activity and ASF chain lengthening probability, the alco...

Higher Alcohols through CO Hydrogenation over CoCu Catalysts: Influence of Precursor Activation

CeO2 nanorods supported Co–CoOx catalysts showed high selectivity for higher alcohol synthesis (HAS) from syngas. The selectivity has found to increase with lowering the Co loadings, and the value over Co1/CeO2 (19.86%) is twice higher than that over Co5/CeO2 (8.67%). The active sites at the interfaces between Co0 and CoOx, or to say, Co–CoOx pairs, have evidenced to be responsible for HAS. The strong metal–support interactions between Co and CeO2 retard the reduction of CoOx and stabilize the intermediates such as CO–Coδ+. Likely, CO favors dissociating on the metallic Co surface to form CHx species, while CO is associatively activated on Coδ+ sites. Moreover, the structure evolution of the Co–CoOx interface was revealed during calcination, reduction, and reaction using in situ X-ray diffraction (XRD), in situ Raman spectroscopy, X-ray absorption spectroscopy (XAS), and in situ diffuse reflectance infrared fourier transform spectroscopy (CO-DRIFTS). The structure–performance relationship of HAS over Co/C...

Structure Evolution of Co–CoOx Interface for Higher Alcohol Synthesis from Syngas over Co/CeO2 Catalysts

Higher alcohols synthesis from syngas over CoCu/SiO2 catalysts: Dynamic structure and the role of Cu

On the nature of active phases and sites in CO and CO2 hydrogenation catalysts

Kinetic study of higher alcohol synthesis directly from syngas over CoCu/SiO2 catalysts

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