Effects of water in the heterogeneous catalytic valorization of levulinic acid into γ-valerolactone and its derivatives

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Abstract

A critical review on the effects of water solvent that contribute to the sustainable development of biomass-derived levulinic acid valorization systems.

Abstract

Levulinic acid (LA), which is considered a versatile biomass-derived molecular platform, typically occupies a core position in the cellulosic biorefinery system. The heterogeneous catalytic valorization of LA for the synthesis of various value-added chemicals and biofuels has been extensively investigated over the past decade, in which the solvent strategy has been reported to exert a significant impact on the overall transformation process. Specifically, water, which typically participates as an essential green solvent in biomass conversion reactions, has exhibited promising application prospects. However, although the crucial role of water has been distinctly recognized in the literature, its specific effects have not been systematically revealed to date. Accordingly, herein, the effects of water on the LA valorization process are summarized and discussed in detail. The kinetic processes in the water-phase conversion of LA are presented, and the potential effects of water on the catalytic reactivity, product distribution and catalytic stability are thoroughly analysed. Also, several feasible suggestions concerning improvement strategies are proposed for the challenges in enhancing the water-assisted catalytic performance. Moreover, this work will potentially contribute to bolstering the rational applications of water solvent in sustainable cellulose biorefineries.

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Single-atom catalysis of CO oxidation using Pt1/FeOx.

Botao Qiao, Aiqin Wang, Xiaofeng Yang … (2011)

Platinum-based heterogeneous catalysts are critical to many important commercial chemical processes, but their efficiency is extremely low on a per metal atom basis, because only the surface active-site atoms are used. Catalysts with single-atom dispersions are thus highly desirable to maximize atom efficiency, but making them is challenging. Here we report the synthesis of a single-atom catalyst that consists of only isolated single Pt atoms anchored to the surfaces of iron oxide nanocrystallites. This single-atom catalyst has extremely high atom efficiency and shows excellent stability and high activity for both CO oxidation and preferential oxidation of CO in H2. Density functional theory calculations show that the high catalytic activity correlates with the partially vacant 5d orbitals of the positively charged, high-valent Pt atoms, which help to reduce both the CO adsorption energy and the activation barriers for CO oxidation.

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David Alonso, Stephanie G Wettstein, James Dumesic (2012)

Research interest in biomass conversion to fuels and chemicals has increased significantly in the last decade as the necessity for a renewable source of carbon has become more evident. Accordingly, many different reactions and processes to convert biomass into high-value products and fuels have been proposed in the literature. Special attention has been given to the conversion of lignocellulosic biomass, which does not compete with food sources and is widely available as a low cost feedstock. In this review, we start with a brief introduction on lignocellulose and the different chemical structures of its components: cellulose, hemicellulose, and lignin. These three components allow for the production of different chemicals after fractionation. After a brief overview of the main reactions involved in biomass conversion, we focus on those where bimetallic catalysts are playing an important role. Although the reactions are similar for cellulose and hemicellulose, which contain C(6) and C(5) sugars, respectively, different products are obtained, and therefore, they have been reviewed separately. The third major fraction of lignocellulose that we address is lignin, which has significant challenges to overcome, as its structure makes catalytic processing more challenging. Bimetallic catalysts offer the possibility of enabling lignocellulosic processing to become a larger part of the biofuels and renewable chemical industry. This review summarizes recent results published in the literature for biomass upgrading reactions using bimetallic catalysts.

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As petroleum prices continue to increase, it is likely that biofuels will play an ever-increasing role in our energy future. The processing of biomass-derived feedstocks (including cellulosic, starch- and sugar-derived biomass, and vegetable fats) by catalytic cracking and hydrotreating is a promising alternative for the future to produce biofuels, and the existing infrastructure of petroleum refineries is well-suited for the production of biofuels, allowing us to rapidly transition to a more sustainable economy without large capital investments for new reaction equipment. This Review discusses the chemistry, catalysts, and challenges involved in the production of biofuels.