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

Luminescent carbon quantum dots (CQDs) represent a new form of nanocarbon materials which have gained widespread attention in recent years, especially in chemical sensor, bioimaging, nanomedicine, solar cells, light-emitting diode (LED), and electrocatalysis. CQDs can be prepared simply and inexpensively by multiple techniques, such as the arc-discharge method, microwave pyrolysis, hydrothermal method, and electrochemical synthesis. CQDs show excellent physical and chemical properties like high crystallization, good dispersibility, photoluminescence properties. In particular, the small size, superconductivity, and rapid electron transfer of CQDs endow the CQDs-based composite with improved electric conductivity and catalytic activity. Besides, CQDs have abundant functional groups on the surface which could facilitate the preparation of multi-component electrical active catalysts. The interactions inside these multi-component catalysts may further enhance the catalytic performance by promoting charge transfer which plays an important role in electrochemistry. Most recent researches on CQDs have focused on their fluorescence characteristics and photocatalytic properties. This review will summarize the primary advances of CQDs in the synthetic methods, excellent physical and electronic properties, and application in electrocatalysis, including oxygen reduction reaction (ORR), oxygen evolution reaction (OER), hydrogen evolution reduction (HER), and CO2 reduction reaction (CO2RR).

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A Mini Review on Carbon Quantum Dots: Preparation, Properties, and Electrocatalytic Application.

Electrochemical water splitting is an appealing and promising approach for energy conversion and storage. As a key half-reaction of electricity-driven water splitting, the oxygen evolution reaction (OER) is a sluggish process due to the transfer of four protons and four electrons. Therefore, development of low-cost and robust OER electrocatalysts is of great importance for improving the efficiency of water splitting. Based on the merits of high surface area, rich pore structure, diverse composition and well-defined metal centers, metal-organic frameworks (MOFs) and their derivatives have been widely exploited as OER electrocatalysts. Herein, the current progress on MOFs and their derivatives for OER electrolysis is summarized, highlighting the design principle, synthetic methods and performance for MOF-based materials. In addition, the structure-performance relationships of MOFs and their derivatives toward the OER are discussed, providing valuable insights into rationally developing OER catalysts with high efficiency. The current scientific and technological challenges and future perspectives towards the purpose of sustainable industrial applications are addressed at the end.

Metal–organic frameworks and their derivatives as electrocatalysts for the oxygen evolution reaction

The gradual depletion of oil resources and the necessity to reduce greenhouse gas emissions portray a concerning image of our contemporary security of liquid transportation fuels in the event of a global crisis. Despite a vast amount of natural gas resources that we have and the huge economic incentive, the conversion of gas to liquid fuels or chemicals is still very limited because of the high technological complexity and capital cost for facilities. However, with the anticipated depletion of liquid petroleum and the soaring price of crude oil, the conversion of natural gas to liquid feedstock or fuels will become more and more important. Higher alcohols are important feedstocks for the chemical and pharmaceutical industries and have wide applications as potential fuel additives or hydrogen carriers for fuel cells for clean energy delivery. There is a long-standing interest in the synthesis of higher alcohols from syngas, an important Fischer–Tropsch technology for natural gas conversion. The purpose of ...

Peng Wang

Papers

Carbon quantum dots for advanced electrocatalysis

Ternary FeCoNi alloy nanoparticles embedded in N-doped carbon nanotubes for efficient oxygen evolution reaction electrocatalysis

Facile preparation of CoSe2 nano-vesicle derived from ZIF-67 and their application for efficient water oxidation

Design and synthesis of spherical-platelike ternary copper-cobalt-manganese catalysts for direct conversion of syngas to ethanol and higher alcohols

The evolutions of carbon and iron species modified by Na and their tuning effect on the hydrogenation of CO2 to olefins