As the main component of lignocelluloses, cellulose is a biopolymer consisting of many glucose units connected through β-1,4-glycosidic bonds. Breakage of the β-1,4-glycosidic bonds by acids leads to the hydrolysis of cellulose polymers, resulting in the sugar molecule glucose or oligosaccharides. Mineral acids, such as HCl and H 2 SO 4 , have been used in the hydrolysis of cellulose. However, they suffer from problems of product separation, reactor corrosion, poor catalyst recyclability and the need for treatment of waste effluent. The use of heterogeneous solid acids can solve some of these problems through the ease of product separation and good catalyst recyclability. This review summarizes recent advances in the hydrolysis of cellulose by different types of solid acids, such as sulfonated carbonaceous based acids, polymer based acids and magnetic solid acids. The acid strength, acid site density, adsorption of the substance and micropores of the solid material are all key factors for effective hydrolysis processes. Methods used to promote reaction efficiency such as the pretreatment of cellulose to reduce its crystallinity and the use of ionic liquids or microwave irradiation to improve the reaction rate are also discussed.
In many organic reactions, the O(2) activation process involves a key step where inert ground triplet O(2) is excited to produce highly reactive singlet O(2). It remains elusive what factor induces the change in the electron spin state of O(2) molecules, although it has been discovered that the presence of noble metal nanoparticles can promote the generation of singlet O(2). In this work, we first demonstrate that surface facet is a key parameter to modulate the O(2) activation process on metal nanocrystals, by employing single-facet Pd nanocrystals as a model system. The experimental measurements clearly show that singlet O(2) is preferentially formed on {100} facets. The simulations further elucidate that the chemisorption of O(2) to the {100} facets can induce a spin-flip process in the O(2) molecules, which is achieved via electron transfer from Pd surface to O(2). With the capability of tuning O(2) activation, we have been able to further implement the {100}-faceted nanocubes in glucose oxidation. It is anticipated that this study will open a door to designing noble metal nanocatalysts for O(2) activation and organic oxidation. Another perspective of this work would be the controllability in tailoring the cancer treatment materials for high (1)O(2) production efficiency, based on the facet control of metal nanocrystals. In the cases of both organic oxidation and cancer treatment, it has been exclusively proven that the efficiency of producing singlet O(2) holds the key to the performance of Pd nanocrystals in the applications.
The development of new catalytic systems for the conversion of biomass-derived molecules into liquid fuels has attracted much attention. We propose a non-noble bimetallic catalyst based on nickel-tungsten carbide for the conversion of the platform molecules 5-(hydroxymethyl)furfural into the liquid-fuel molecule 2,5-dimethylfuran (DMF). Different catalysts, metal ratios and reaction conditions have been tested and give rise to a 96% yield of DMF. The catalysts have been characterized and are discussed. The reaction mechanism is also explored through capture of reaction intermediates. The analysis of the reaction mixture over different catalysts is presented and helps to understand the role of nickel and tungsten carbide during the reaction.
A catalytic transfer hydrogenation process was developed for the production of γ-valerolactone (GVL) from ethyl levulinate (EL) and a H-donor at room temperature. Ethyl levulinate was almost quantitatively converted to γ-valerolactone. Further, a two step process for producing GVL from biomass derived platform molecules was also reported.
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