The development of precious-metal-free catalysts to promote the sustainable production of fuels and chemicals from biomass remains an important and challenging target. Here, we report the efficient hydrogenolysis of biomass-derived 5-hydroxymethylfurfural to 2,5-dimethylfuran over a unique core-shell structured catalyst, Co@CoO that affords the highest productivity among all catalysts, including noble-metal-based catalysts, reported to date. Surprisingly, we find that the catalytically active sites reside on the shell of CoO with oxygen vacancies rather than the metallic Co. The combination of various spectroscopic experiments and computational modelling reveals that the CoO shell incorporating oxygen vacancies not only drives the heterolytic cleavage, but also the homolytic cleavage of H2 to yield more active Hδ- species, resulting in the exceptional catalytic activity. Co@CoO also exhibits excellent activity toward the direct hydrodeoxygenation of lignin model compounds. This study unlocks, for the first time, the potential of simple metal-oxide-based catalysts for the hydrodeoxygenation of renewable biomass to chemical feedstocks. 

/pdf/a-unique-co-coo-catalyst-for-hydrogenolysis-of-biomass-3oewyqae.pdf

A unique Co@CoO catalyst for hydrogenolysis of biomass-derived 5-hydroxymethylfurfural to 2,5-dimethylfuran

The development of renewable energy resources is strongly urged to recoup the shortage of fossil-based energy and its associated pollution issues. Energy production from carbohydrate materials has recently been of great interest due to the availability, reliability, and abundance of carbohydrate sources. Significantly, the catalytic transformation of waste carbohydrates into furan-based biofuels, specifically 2,5-dimethylfuran (DMF), appears to be an attractive solution to the aforementioned energy and environmental issues. The potential of DMF as a renewable fuel is prospective, with its physicochemical properties that are similar to those of fossil fuels. Therefore, the current work focuses on the production of DMF, with the important aspects for enhanced DMF yield being summarized herein. Notably, the significant catalysts derived from zeolite, noble-metal, non-noble-metal, metal–organic framework, and electrocatalytic materials are discussed, alongside their effects in deriving carbohydrates to DMF. Furthermore, the mechanisms of DMF production were clarified too, followed by the scrutinization of the effects from reaction conditions, solvents, and hydrogen donors onto the DMF yield. Finally, the purification process, commercialization potential, and economic feasibility of DMF production were incorporated too, with insightful future directions being identified at the end of our review. This review is expected to advocate DMF production from carbohydrate materials, which could alleviate the energy and environmental problems encountered presently. 

/pdf/catalyst-based-synthesis-of-25-dimethylfuran-from-2qqbdbsx.pdf

Catalyst-Based Synthesis of 2,5-Dimethylfuran from Carbohydrates as a Sustainable Biofuel Production Route

Climate change, socioeconomical pressures, and new policy and legislation are driving a decarbonization process across industries, with a critical shift from a fossil-based economy toward a biomass-based one. This new paradigm implies not only a gradual phasing out of fossil fuels as a source of energy but also a move away from crude oil as a source of platform chemicals, polymers, drugs, solvents and many other critical materials, and consumer goods that are ubiquitous in our everyday life. If we are to achieve the United Nations’ Sustainable Development Goals, crude oil must be substituted by renewable sources, and in this evolution, biorefineries arise as the critical alternative to traditional refineries for producing fuels, chemical building blocks, and materials out of non-edible biomass and biomass waste. State-of-the-art biorefineries already produce cost-competitive chemicals and materials, but other products remain challenging from the economic point of view, or their scaled-up production processes are still not sufficiently developed. In particular, lignin’s depolymerization is a required milestone for the success of integrated biorefineries, and better catalysts and processes must be improved to prepare bio-based aromatic simple molecules. This review summarizes current challenges in biorefinery systems, while it suggests possible directions and goals for sustainable development in the years to come.

/pdf/biorefineries-achievements-and-challenges-for-a-bio-based-uqhvpggz.pdf

Biorefineries: Achievements and challenges for a bio-based economy

Recent advances in polyoxometalates acid-catalyzed organic reactions

Levulinic acid (LA) is one of the most prominent biomass‐derived chemical building blocks that can be transformed into specialty chemicals like fuels, solvents, monomers for polymers, plasticizers, surfactants, agrochemicals, and pharmaceuticals. Over the past three decades, an enormous amount of research data have been acquired on the preparation and downstream value addition of LA, and these works have been reviewed. However, considering the astonishing number of publications appearing every year on LA derivatives, the periodical review of recent works focusing on unique aspects of chemistry must be undertaken to critically evaluate the achievements to date, reassess the challenges, and recognize new opportunities. This review discusses the chemical‐catalytic synthesis of various derivatives of LA by focusing on its functionalities and reactivity patterns. Recent literature on some crucial derivatives such as γ‐valerolactone, 4,4’‐diphenolic acid, and ethyl levulinate have been tabulated and discussed. The synthetic interconversion between various derivatives, mechanistic insights, critical analysis of the reaction parameters toward selective preparation of various derivatives, and their potential commercial applications have been elaborated using predominantly heterogeneous catalysts. A critical assessment of the relative advantages and shortcomings of the existing synthetic strategies for various derivatives of LA has been presented to enkindle fresh ideas.

Recent Advances in the Value Addition of Biomass-Derived Levulinic Acid: A Review Focusing on its Chemical Reactivity Patterns

This work reports the synthesis of a series of alkyl levulinates from biomass-derived 5-(halomethyl)furfural (X = Cl, Br), furfuryl alcohol, and angelica lactone using silica-supported perchloric acid (HClO4-SiO2) as a heterogeneous acid catalyst. The solvent-free, one-pot preparation afforded levulinate esters in excellent isolated yields (> 84%). The reactions were performed at 120 °C for 6 h in a batch-type glass pressure reactor using XMF and furfuryl alcohol in presence of excess of the alcohol reagent and 4 wt.% of the HClO4-SiO2 catalyst (0.028 mmol HClO4). Furthermore, the reaction protocol was extended for the synthesis of ALs starting with angelica lactone at 90 °C for 2 h in a round-bottomed flask by using excess alcohol and 4 wt.% of the HClO4-SiO2 catalyst.

Preparation of alkyl levulinates from biomass-derived 5-(halomethyl)furfural (X = Cl, Br), furfuryl alcohol, and angelica lactone using silica-supported perchloric acid as a heterogeneous acid catalyst

Catalytic conversion of glucose and its biopolymers into renewable compounds by inducing C–C bond scission and formation

In this work, biomass-derived furfural has been selectively oxidized to 2(5H)-furanone using aqueous hydrogen peroxide as the green oxidant. Among various homogeneous acid catalysts screened for the transformation, trifluoroacetic acid (TFA) was found to be the most suitable candidate that afforded up to 52% isolated yield of 2(5H)-furanone under mild conditions (RT, 1 h). In addition, succinic acid was recovered in nearly 20% yield from the aqueous layer. The organic solvent-free, gram-scale reaction was optimized on temperature, the molar ratio of H2O2 and furfural, and the amount of TFA used.

https://link.springer.com/content/pdf/10.1007/s13399-021-01297-0.pdf

Selective oxidation of biomass-derived furfural to 2(5H)-furanone using trifluoroacetic acid as the catalyst and hydrogen peroxide as a green oxidant

Efficient Preparation of Alkyl Benzoates by Heteropolyacid‐Catalysed Esterification of Benzoic Acid under Solvent‐Free Condition

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