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

CeO2 is an excellent potential material for CO2 hydrogenation attributed to the highly tunable properties including metal–support interaction and abundant oxygen vacancy. In this work, four CeO2 su...

Insights into the Influence of CeO2 Crystal Facet on CO2 Hydrogenation to Methanol over Pd/CeO2 Catalysts

The present work elucidated the size effect of Pt nanoparticles on the activity of Pt/CeO2 catalysts toward catalytic oxidation of toluene. Size-controllable Pt nanoparticles, ranging from 1.3 to 2.5 nm, were successfully loaded on CeO2 nanorod support by the adsorption method. The structure and chemical properties of Pt/CeO2 catalysts are much dependent on Pt particle size. As size increases, the Pt dispersion declines while more Pt-O Ce bonds, Ce3+ and oxygen vacancies exist on ceria. The catalytic activity test of toluene oxidation shows that Pt/CeO2-1.8 sample exhibits the best catalytic performance due to the balance of both Pt dispersion and oxygen vacancy concentration of ceria. Three types of TOFs values based on Pt dispersion, oxygen vacancy concentration and both of them are calculated respectively, and the result demonstrates that the reaction rate is controlled by both of the exposed Pt atom and oxygen vacancies. In addition, the Pt/CeO2-1.8 catalyst could work properly for 120 h with various inlet toluene concentration and be completely negligible for 5 vol% water vapour at 155 °C.

Size effect of Pt nanoparticles on the catalytic oxidation of toluene over Pt/CeO2 catalysts

Preferential oxidation of CO (PROX) is an important reaction for removing small amounts of CO to a parts-per-million level from the hydrogen-rich stream, which will be ultimately supplied as a fuel to polymer–electrolyte membrane fuel cells. The key to the application of PROX is to develop a highly active and selective catalyst that operates well in a wide temperature window (e.g., 80–180 °C) and has good resistance to CO2 and steam. In the past decades, various catalyst formulations have been developed, among which platinum group metal catalysts, including Pt, Ru, and Ir—in particular, those modified with promoters such as alkali metals and reducible metal oxides—have received a great deal of attention for their significantly improved catalytic activities in the low-temperature range. In this minireview, the recent advances of the platinum group metal catalysts for the PROX reaction are summarized, including performances of unpromoted and promoted catalysts, reaction mechanisms, and kinetics. In addition...

Recent Advances in Preferential Oxidation of CO Reaction over Platinum Group Metal Catalysts

A novel template-free oxalate route was applied to synthesize mesoporous manganese oxides with high surface area (355 m2 g−1) and well-defined mesopores which can be obtained in large quantities. The physicochemical properties of the materials were characterized by means of TG, XRD, SEM, TEM, H2-TPR and XPS techniques. All catalysts were tested on catalytic deep oxidation of benzene, and the effects of calcination temperature on the features of catalyst structure and catalytic activity were investigated. Manganese oxides prepared by oxalate route exhibited better catalytic activities for complete oxidation of benzene, toluene and o-xylene as compared with related manganese oxides prepared by other different methods (NaOH route, NH4HCO3 route and nanocasting strategy), and especially the temperature for benzene conversion of 90% on the oxalate-derived manganese oxide catalysts was 209 °C, which is 132 °C lower than required for the catalyst prepared by NaOH route. The catalytic performance of manganese oxide is correlated with surface area, pore size, low-temperature reducibility and distribution of surface species. The mole ratio of Mn4+/Mn2+ on the samples which performed with better catalytic activity was close to 1.0. This is good for the redox process of Mn4+ ↔ Mn3+ ↔ Mn2+ which is the key factor in determining the activity on MnOx, further indicating that the oxalate route is good for keeping the distribution of manganese oxidation states at an appropriate degree. A possible process of VOCs’ complete oxidation on manganese oxide catalysts is discussed. In addition, the best catalyst was highly stable with prolonged time on stream and was resistant to water vapor.

Oxalate route for promoting activity of manganese oxide catalysts in total VOCs’ oxidation: effect of calcination temperature and preparation method

Operando and kinetic studies of lean-burn methane combustion were preformed on a Pd(3.3 wt %)/γ-Al2O3 catalyst in a low temperature range of 473–673 K. The reaction order with respect to oxygen decreased with temperature, and the order with respect to methane remained constant. The working catalyst is characterized using operando Raman spectroscopy and in situ diffuse reflectance infrared Fourier transform spectroscopy of CO adsorption (DRIFTS), and the Pd chemical states were measured with X-ray photoelectron spectroscopy (XPS). Partial oxidation of Pd atoms during reaction was identified by Raman and XPS spectroscopies. In particular, the DRIFT spectra revealed that ∼45% of Pd atoms at the top layers were transferred into PdOx species above 523 K. The reaction was assumed to occur primarily on the metallic Pd sites below 673 K, proceeding through the Langmuir–Hinshelwood mechanism, and Pd oxide may affect the adsorption and activation of reactants.

Operando and Kinetic Study of Low-Temperature, Lean-Burn Methane Combustion over a Pd/γ-Al2O3 Catalyst

Operando Raman spectroscopy and kinetic study of low-temperature CO oxidation on an α-Mn2O3 nanocatalyst

The α-Mn2O3 nanocrystals with uniform morphology prepared by calcining a self-assembly Mn3O4 precursor show higher activity toward CO oxidation. Operando Raman spectroscopy is used to probe the near-surface structure of α-Mn2O3 nanocrystals during the adsorption and oxidation of CO for the first time. A surface phase-transformation from α-Mn2O3 to MnO-like species, as evidenced by the formation of a single band at 498 cm–1, was observed only at or above 300 °C in the presence of CO. This modification is probably due to the loss of lattice oxygen at high temperatures that leads to the surface reconstruction. Very interestingly, a reversible phase-transformation was observed with decreasing the temperature to 25 °C. The shift of the symmetric stretching of Mn2O3 groups (632 → 649 cm–1) due to the adsorption of CO was observed even at room temperature. In addition, the results of the temperature-programmed desorption of O2 (TPD-O2) and temperature-programmed surface reaction (TRSR) indicate that the oxidizin...

Probing the Surface Structure of α-Mn2O3 Nanocrystals during CO Oxidation by Operando Raman Spectroscopy

Mechanistic study of preferential CO oxidation on a Pt/NaY zeolite catalyst

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

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