Efficient transfer hydrogenation of levulinic acid (LA) to γ-valerolactone (GVL) over Ni/NiO–MC (MC = mesoporous carbon)

Liu, Xinyu; Li, Zhaohui

doi:10.1039/d1se00228g

Cited by 12 publications

(3 citation statements)

References 83 publications

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“…In a separate study, Liu et al using Ni and NiO supported on mesoporous carbon, observed the TOF of 10.8 h −1 in LA hydrogenation. 64 In our studies, we obtained the TOF values of 27 h −1 for 5 wt% Cu/OMS-2 (Pre-Dep) and 10.6 h −1 for 5 wt% Cu/OMS-2 (Wet-Imp).…”

Section: Resultsmentioning

confidence: 95%

Structure sensitivity of Cu supported on manganese oxide catalysts in levulinic acid hydrogenation

Mazumdar,

Kumar,

Arredondo-Arechavala

et al. 2024

Catal. Sci. Technol.

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Section: Resultsmentioning

confidence: 95%

Structure sensitivity of Cu supported on manganese oxide catalysts in levulinic acid hydrogenation

Mazumdar,

Kumar,

Arredondo-Arechavala

et al. 2024

Catal. Sci. Technol.

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“… The prominent platform chemical LA, obtained through the hydrolysis of the cellulosic part of biomass, serves as a direct precursor to the production of GVL. Consequently, there has been a significant increase in research and development efforts focused on enhancing the synthesis of GVL from LA. , Furfural (FA) in comparison to levulinic acid holds great promise as a C5 substance for producing GVL, as it can be directly obtained from raw biomass . FA undergoes a transformation to furfuryl alcohol (FOL), which can be hydrolyzed to yield levulinic acid (LA) or levulinic esters (LE) in water or alcoholic solvents.…”

Section: Introductionmentioning

confidence: 99%

Synthesis of γ-Valerolactone from Levulinic Acid with Co/NC, and from Furfural via Cascade Reaction Using Co/NC and H-Beta

Chauhan,

Bal,

Srivastava

2024

Energy Fuels

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γ-Valerolactone (GVL) has transpired as an ecofriendly solvent, a promising fuel additive, and a precursor to valuable chemicals. The study explores an approach to GVL synthesis by employing non-noble metals in contrast to conventional methods involving noble metals. The selective hydrogenation of levulinic acid (LA) and levulinate esters offers a pathway to GVL production, while the direct transformation from furfural (FA) enhances its potential. The study focuses on 3d transition metal-based N-doped carbon catalysts, highlighting Co/ NC as the most effective catalyst for LA to GVL hydrogenation, yielding ∼100% GVL. The catalyst was also employed in a one-pot, three-step cascade reaction: FA hydrogenation to furfuryl alcohol (FOL) was performed using 10% Co/NC, ethanolysis of FOL to ethyl levulinate (EL) was facilitated by H-β, and EL hydrogenation to GVL was performed using 10% Co/NC. Each step was optimized independently. The cascade reaction was executed at 140 °C for 12 h through a comprehensive approach, achieving a noteworthy 92.1% GVL yield from FA, which was further upcycled to the gram scale, offering 86% of the final GVL yield. The catalyst characterization, catalytic activity data, and control experiments culminate in the proposed LA to GVL transformation mechanisms and the one-pot, three-step cascade FA to GVL conversion. The research significantly contributes to advancing sustainable GVL production and its multifaceted applications.

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“…The growing demand for sustainable chemicals and fuels produced by renewable resources has attracted much attention with the overexploitation of fossil energy in recent years. , Biomass, the renewable carbon reservoir, is considered a potential alternative to the depleting fossil feedstocks and expected to achieve the goals of carbon neutrality and low-carbon economy. − As one of the highest potential biomass derivatives, levulinic acid (LA) produced by acid hydrolysis of cellulose or hemicellulose can be converted to value-added γ-valerolactone (GVL) via a two-step reaction pathway including hydrogenation and intramolecular dehydration or the opposite reaction sequence (Scheme ). , GVL can be widely utilized as a potential additive to transportation fuels, a green solvent, a food ingredient, and an important intermediate for various fine chemicals. − Thus, great endeavors have been devoted to the efficient conversion of LA to value-added GVL in recent years. − However, although the efficient production of GVL from LA can be achieved, using precious metal catalysts or rigorous reaction conditions is unavoidable, and the high energy expenditure required in expediting the hydrogenolysis of LA prevents the practical application of these catalysts. Therefore, it is necessary to rationally design highly efficient non-noble metal catalysts that can promote the hydrogenation activity of LA under mild conditions.…”

Section: Introductionmentioning

confidence: 99%

In Situ Construction of a Co/ZnO@C Heterojunction Catalyst for Efficient Hydrogenation of Biomass Derivative under Mild Conditions

Shao

Zhou

et al. 2022

ACS Appl. Mater. Interfaces

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The efficient hydrogenation of biomass-derived levulinic acid (LA) to value-added γ-valerolactone (GVL) based on nonprecious metal catalysts under mild conditions is crucial challenge because of the intrinsic inactivity and instability of these catalysts. Herein, a series of highly active and stable carbon-encapsulated Co/ZnO@C-X (where X = 0.1, 0.3, 0.5, the molar ratios of Zn/(Co+Zn)) heterojunction catalysts were obtained by in situ pyrolysis of bimetal CoZn MOF-74. The optimal Co/ZnO@C-0.3 catalyst could achieve 100% conversion of LA and 98.35% selectivity to GVL under mild conditions (100 °C, 5 bar, 3 h), which outperformed most of the state-of-the-art catalysts reported so far. Detailed characterizations, experimental investigations, and theoretical calculations revealed that the interfacial interaction between Co and ZnO nanoparticles (NPs) could promote the dispersibility and air stability of the active Co0 for the activation of H2. Moreover, the strong Co–ZnO interaction also enhanced the Lewis acidity of the Co/ZnO interface, contributing to the adsorption of LA and the esterification of intermediates. The synergy between the hydrogenation sites and the Lewis acid sites at the Co/ZnO interface enabled the conversion of LA to GVL with high efficiency. In addition, benefiting from the Co–ZnO interfacial interaction as well as the unique carbon-encapsulated structure of the heterojunction catalyst, the recyclability was also greatly improved and the yield of GVL was nearly unchanged even after six cycles.

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Efficient transfer hydrogenation of levulinic acid (LA) to γ-valerolactone (GVL) over Ni/NiO–MC (MC = mesoporous carbon)

Abstract: Ni/NiO-MC (MC=Mesoporous carbon), in which Ni and NiO nanoparticles well distributed on MC, has been successfully synthesized by a pyrolysis of Ni/mesostructured polymer framework precursor prepared via an ion-exchange process...

Cited by 12 publications

References 83 publications

Structure sensitivity of Cu supported on manganese oxide catalysts in levulinic acid hydrogenation

Structure sensitivity of Cu supported on manganese oxide catalysts in levulinic acid hydrogenation

Synthesis of γ-Valerolactone from Levulinic Acid with Co/NC, and from Furfural via Cascade Reaction Using Co/NC and H-Beta

In Situ Construction of a Co/ZnO@C Heterojunction Catalyst for Efficient Hydrogenation of Biomass Derivative under Mild Conditions

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