ABSTRACT
Catalytic transformations of syngas (a mixture of H2 and CO), which is one of the most important C1-chemistry platforms, and CO2, a greenhouse gas released from human industrial activities but also a candidate of abundant carbon feedstock, into chemicals and fuels have attracted much attention in recent years. Fischer-Tropsch (FT) synthesis is a classic route of syngas chemistry, but the product selectivity of FT synthesis is limited by the Anderson-Schulz-Flory (ASF) distribution. The hydrogenation of CO2 into C2+ hydrocarbons involving C-C bond formation encounters similar selectivity limitation. The present article focuses on recent advances in breaking the selectivity limitation by using a reaction coupling strategy for hydrogenation of both CO and CO2 into C2+ hydrocarbons, which include key building-block chemicals, such as lower (C2-C4) olefins and aromatics, and liquid fuels, such as gasoline (C5-C11 hydrocarbons), jet fuel (C8-C16 hydrocarbons) and diesel fuel (C10-C20 hydrocarbons). The design and development of novel bifunctional or multifunctional catalysts, which are composed of metal, metal carbide or metal oxide nanoparticles and zeolites, for hydrogenation of CO and CO2 to C2+ hydrocarbons beyond FT synthesis will be reviewed. The key factors in controlling catalytic performances, such as the catalyst component, the acidity and mesoporosity of the zeolite and the proximity between the metal/metal carbide/metal oxide and zeolite, will be analysed to provide insights for designing efficient bifunctional or multifunctional catalysts. The reaction mechanism, in particular the activation of CO and CO2, the reaction pathway and the reaction intermediate, will be discussed to provide a deep understanding of the chemistry of the new C1 chemistry routes beyond FT synthesis.
ABSTRACT
High temperature water-gas shift reaction was demonstrated for the first time on a CuFe2O4-mesoporous alumina nanocomposite between 350 and 550 °C with 70-80% CO-conversion using simulated waste derived syngas under realistic conditions. Despite high Al-content, the catalyst exhibited stable activity, which was attributed to the nano-architectured robust porous nature of alumina integrated with surrounding CuFe2O4.
ABSTRACT
Co(3)O(4) nanorods (diameters approximately 6-8 nm and lengths approximately 20-30 nm) were synthesized for the first time through a simple co-precipitation/digestion method by calcination of cobalt hydroxyl carbonate in air and their CO gas sensing properties were investigated. The Co(3)O(4) nanorods exhibited outstanding gas sensing characteristics such as, higher gas response (approximately 6.55-50 ppm CO gas at 250 degrees C), extremely rapid response (approximately 3-4s), fast recovery (approximately 5-6s), excellent repeatability, good selectivity and lower operating temperature (approximately 250 degrees C). Furthermore, the Co(3)O(4) nanorods are able to detect up to 5 ppm for CO with reasonable sensitivity (approximately 3.32) at an operating temperature 250 degrees C and they can be reliably used to monitor the concentration of CO over the range (5-50 ppm). The experimental results clearly demonstrate the potential of using the Co(3)O(4) nanorods as sensing material in the fabrication of CO sensors. Plausible CO sensing mechanism of the Co(3)O(4) nanorods is also discussed.
