Molecular Catalysis
·
2025
·
IF 4.9
Ying Yang,Shuo Wang,Yuhang Sun,Jihuan Song,Chenmeng Cui,Sungsik Lee
The hydrogenation of levulinic acid (LA) to γ-valerolactone (GVL) is significant for producing chemicals and fuels from renewable resources, a promising direction in biomass refining. Currently, non-precious metal catalysts suffer from low activity due to a single electronic structure, which is incapable of effectively activating both C O in LA and H 2 . Herein we report in situ fabricated Co nanoclusters within positive and metallic Co sites on N-doped carbon, which can simultaneously activate LA's C O and H 2 , enhancing the activity and selectivity for GVL production. Urea-assisted Co dispersion coupled with variation of pyrolysis temperature, Co nanoclusters were formed via direct conversion of Co-containing zinc trimesic acid fibers. The resulting Co nanoclusters possess dual active sites of Co-N x and metallic Co, with adjustable electronic structures. Under the reaction conditions of 200 °C and 4.5 MPa H 2 for 4 h, LA was completely converted, achieving 95 % yield of GVL. The outstanding catalytic activity is attributed to the Co-N x and metallic Co active sites, which facilitate the activation of C O and H 2 , respectively. This research provides a new concept for converting N-free metal-organic frameworks into non-precious metal nanoclusters, offering valuable insights for designing high-performance non-precious metal catalysts for biomass-derived chemical and fuel production.
研究领域:
催化化学
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材料科学
·
可再生能源
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DOI
高影响因子
ACS Catalysis
·
2022
·
IF 13.7
Anon Bunrit,Teera Butburee,Meijiang Liu,Zhipeng Huang,Keerati Meeporn,Chaiyasit Phawa,Jian Zhang,Sanchai Kuboon,Huifang Liu,Kajornsak Faungnawakij,Feng Wang
Herein, we developed photo–thermo-dual catalytic strategies for the production of γ-valerolactone (GVL) from levulinic acid (LA) and its ester using platinum-loaded TiO2 as a dual-functional catalyst. Both catalytic systems were evaluated under mild reaction conditions. In the photocatalysis system, a base plays crucial roles in the conversion of LA and EL to GVL. The control experiments reveal that plausible mechanistic pathways of both systems proceed via the hydrogenation of the ketone group of LA to the corresponding alcohol as a major intermediate followed by a subsequent cyclization step to GVL. This dual-functional catalyst provides alternative strategies for the conversion of LA and its ester into GVL, which could pave the way for biomass utilization in a more effective and practical manner.
研究领域:
催化
·
生物质转化
·
化学工程
·
可持续化学
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DOI
高影响因子
JOURNAL OF CATALYSIS
·
2026
·
IF 6
Xiaolong Fang,Shangsong Feng,Jin Huang,Hao Li,Jinhui Zhang,Weiyi Wang,Fengjun Zhang,Yong Yang
Homogeneous selective hydrogenation often relies on sophisticated yet fragile ligands to improve catalytic performance. This not only complicates the process but also increases costs, thereby severely impeding its industrial application. In this work, we report a novel ligand-free strategy for the homogeneous conversion of levulinic acid using Ru 3 (CO) 12 , which proceeds via a substrate-promoted pathway. Under mild reaction conditions, excellent turnover numbers (up to 99000) and turnover frequencies (up to 2750 h −1 ) were achieved for the production of γ-valerolactone. Mechanistic insights reveal that a levulinic acid-derived Ru 2 (CO) 4 sawhorse-type unit was formed in situ, and a catalytic cycle is proposed based on this key intermediate, outlining a new paradigm for practical and sustainable catalysis.
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DOI
高影响因子
Catalysts
·
2020
·Vol. 10
·期 6
·692
·
IF 3.52
Yan Du,Xiao Chen,Ji Qi,Pan Wang,Changhai Liang
The electrocatalytic hydrogenation (ECH) of biomass-derived levulinic acid (LA) is a promising strategy to synthetize fine chemicals under ambient conditions by replacing the thermocatalytic hydrogenation at high temperature and high pressure. Herein, various metallic electrodes were investigated in the ECH of LA in a H-type divided cell. The effects of potential, electrolyte concentration, reactant concentration, and temperature on catalytic performance and Faradaic efficiency were systematically explored. The high conversion of LA (93%) and excellent “apparent” selectivity to valeric acid (VA) (94%) with a Faradaic efficiency of 46% can be achieved over a metallic lead electrode in 0.5 M H2SO4electrolyte containing 0.2 M LA at an applied voltage of −1.8 V (vs. Ag/AgCl) for 4 h. The combination of adsorbed LA and adsorbed hydrogen (Hads) on the surface of the metallic lead electrode is key to the formation of VA. Interestingly, the reaction performance did not change significantly after eight cycles, while the surface of the metallic lead cathode became rough, which may expose more active sites for the ECH of LA to VA. However, there was some degree of corrosion for the metallic lead cathode in this strong acid environment. Therefore, it is necessary to improve the leaching-resistance of the cathode for the ECH of LA in future research.Keywords:electrocatalytic hydrogenation;levulinic acid;valeric acid;lead
研究领域:
化学工程
·
可再生能源
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF APPLIED POLYMER SCIENCE
·
2020
·Vol. 138
·期 1
·49611
·
IF 2.52
Zongqi Zhang,Yuanfeng Wu,Lijing Gao,Guomin Xiao
This work aims at investigating the special application of ZSM-5/polydimethylsiloxane (PDMS) membrane being used for pervaporation separation of levulinic acid aqueous solutions. The effects of temperature, downstream pressure, feed concentration, and raw material ratio on the separation performance are investigated by self-made flat-sheet films. When the flow rate of feed pump remained at 0.4 ml/min (10 wt% levulinic acid), a levulinic acid permeation flux of 334.13 g/(m 2 h) and a separation factor of 2.382 at 75°C are observed over the composite membrane doped with 10 wt% ZSM-5. In addition, the acid resistance is enhanced after the PDMS membranes are doped with ZSM-5. Besides, the functionalized process also makes the membranes increase in its hydrophobicity. The results demonstrate that the ZSM-5/PDMS-based membranes show profound prospects for separating levulinic acid aqueous solution.
研究领域:
化学工程
·
材料科学
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产品关联
DOI
高影响因子
CELLULOSE
·
2017
·Vol. 24
·期 3
·1383-1394
·
IF 3.417
Wang Kui,Ye Jun,Zhou Minghao,Liu Peng,Liang Xinyu,Xu Junming,Jiang Jianchun
Direct conversion of cellulose into levulinic acid and furfural in sulfolane media with the aid of water and H 2 SO 4 was performed at 140–220 °C under the pressures of 0–1.5 MPa. This approach could obtain 72.5 mol% levulinic acid and 11.5 mol% furfural formation under an optimal condition in which the mass ratio of sulfolane, water and H 2 SO 4 was 90:10:1. It was found that the decrease of water content led to an increasing yield of furfural and that the maximum furfural yield (51.1 mol%) could be obtained in the absence of water. The synergism of sulfolane and water in the selective liquefied system was demonstrated to be responsible for not only reinforced effect of optimizing and isolating the target products but also for reducing re-polymerization and side reactions. Furthermore, sulfolane in our case could be recycled and re-used for the conversion of cellulose with the same yield, which shed light on the remarkable potential for future industrial application.
研究领域:
化学工程
·
可再生资源与环境科学
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产品关联
DOI
高影响因子
RSC Advances
·
2016
·Vol. 6
·期 76
·72744-72749
·
IF 3.289
Fei Xia,Zhongtian Du,Junxia Liu,Yangyang Ma,Jie Xu
Recently, obtaining value-added chemicals from biomass resources has attracted considerable attention. Levulinic acid is one of the most important biomass platform compounds, which could be obtained from carbohydrate biomass. In this work, levulinic acid was selectively converted into C4 product, including succinic anhydride, via catalytic oxidation with a manganese catalyst in acetic anhydride. Moreover, an unexpected product of maleic anhydride was obtained, which greatly differs from that of levulinate ester. The pathway for formation of maleic anhydride was studied by monitoring and confirming intermediates α-angelica lactone and its derivative 2-methyl-5-oxotetrahydro-2-furanyl acetate. Based on the obtained mechanistic information, the different behaviour between the oxidative cleavage of levulinic acid and levulinate ester was further discussed.
研究领域:
化学工程
·
可再生资源化学
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产品关联
DOI
高影响因子
CATALYSIS SURVEYS FROM ASIA
·
2018
·Vol. 22
·期 3
·129-135
·
IF 3.081
Zhang Di,Zhao Yun-Peng,Fan Xing,Liu Zhong-Qiu,Wang Rui-Yu,Wei Xian-Yong
A series of Ni/HZSM-5 catalysts with different Ni-loadings and Si/Al ratios were prepared by incipient wetness impregnation and employed for catalytic hydrogenation of levulinic acid (LA) to gamma-valerolactone (GVL). Their physicochemical properties were characterized by X-ray diffraction, nitrogen adsorption–desorption, X-ray photoelectron spectrometer, temperature-programmed desorption of ammonia,transmission electron microscopy, temperature-programmed reduction of hydrogen, and pyridine-adsorbed infrared spectroscopy. The diffraction peaks assigned to Ni phase were not observed, implying that nickel particles were small and had a high dispersion on the supports. The catalysts with a strong acidity and the appropriate ratio of Brönsted (B) acid sites to Lewis (L) acid sites (B/L = 4.9) show an excellent activity and selectivity for the hydrogenation of LA to GVL. High conversion of LA and selectivity towards GVL were achieved over 5 wt% Ni/HZSM-5-50. The maximum GVL yield of 100% over 5 wt% Ni/HZSM-5-50 was obtained under the optimized reaction conditions of 210 °C, 2 h, and 3 MPa initial hydrogen pressure.
研究领域:
催化化学
·
材料科学
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产品关联
DOI
高影响因子
RENEWABLE ENERGY
·
2023
·
IF 8.7
Ronghua Zhang,Wenhao Zhang,Jianchun Jiang,Junming Xu,Kui Wang,Junfeng Feng,Hui Pan
Methyl levulinate (ML) and levulinic acid (LA), important platform chemicals derived from biomass carbohydrates, are potential candidates for use as fuel additives and chemicals. In this work, bifunctional solid acid catalysts were prepared by impregnation via an environmentally friendly method and used for the conversion of glucose to ML and LA. In the conversion of glucose to levulinate, the isomeric conversion of glucose into fructose mainly utilized the Lewis acid sites properties exhibited by chromium, and the dehydration of fructose to 5-hydroxymethylfurfural and its degradation to levulinate mainly exploited the Brønsted acid sites properties exhibited by A15 . The yield of ML and LA was 43.1 % and 1.2 %, respectively, and glucose was completely transformed into methanol within 2.0 h at 200 °C. The excellent activity of the best catalyst may be due to the sufficient total acidity and suitable ratio of the number of Lewis acid sites to that of Brønsted acid sites. The results for five catalysis cycles proved that the catalyst has good stability and reusability . In addition, the catalyst prepared was effective for the conversion of other carbohydrates, namely, sucrose, cellobiose, and 5-hydroxymethylfurfural to ML with yields of 83.3 %, 77.7 %, and 57.4 %, respectively.
研究领域:
化学工程
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催化
·
生物化学
·
可再生能源
✓ 已验证
产品关联
DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2024
·
IF 3.8
Ruixue Zhang,Weiyao Yang,Hongda Zhang,Le Sang,Zhiping Zhao
This work presents the efficient, safe, and continuous production of 5-hydroxymethylfurfural (HMF) and levulinic acid (LA) from inulin in micropacked bed reactors (μPBRs) over HND-580. Through optimization reaction conditions, the highly selective production of fructose and LA from aqueous inulin and HMF from an inulin DMSO-water mixed solution can be achieved with respect to other reactor technologies. The highest yields of 89% for fructose, 81% for HMF, and 84% for LA can be obtained within a reaction time of 7.26 min. Polysaccharide inulin is used as the reaction substrate, and the space-time yield (STY) of HMF and LA in μPBRs is at least an order higher than that in conventional batch reactors. Subsequently, an intrinsic kinetic model for inulin conversion is established. The most predicted values show good agreement with the experimental results with a relative error of ±20%.
研究领域:
化学工程
·
催化
·
生化工程
·
可再生能源
✓ 已验证
产品关联
DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2026
·Vol. 65
·期 34
·18084-18092
·
IF 3.9
Xu Cuiwei,Jia Jinjie,Ouyang Sufang,Wu Jianguo,Li Xin,Liu Xiaolei,Qian Jun,Cao Dong,Cheng Daojian
Regulating
the size of the active metal is crucial to change the
electronic structure and catalytic activity. Here, five Ru/CN-ZrO 2 catalysts with different sizes are precisely constructed
via a two-step wet chemical synthesis method. Remarkably, a volcano
trend between the size of Ru and hydrogenation activity for levulinic
acid (LA) is disclosed. The Ru nanoclusters with an average size of
∼2.7 nm (Ru/CN-ZrO 2 -2) exhibit the highest catalytic
activity for LA hydrogenation, achieving an LA conversion of 99.4%
and a γ-valerolactone (GVL) selectivity of 99.3%. Besides, the
corresponding turnover frequency (TOF) is 4860.1 h –1 , which far surpasses that most reported for Ru-based catalysts.
Mechanism studies reveal Ru/CN-ZrO 2 -2 with moderate size
is beneficial to enhance the interaction between Ru and support, directly
promoting the adsorption of LA, and thereby exhibiting the lowest
activation energy. This work emphasizes the size effect to improve
the catalytic activity, which is an important guidance for the rational
design of hydrogenation catalysts.
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DOI
高影响因子
ACS Sustainable Chemistry & Engineering
·
2021
·
IF 8.198
Zuojun Wei,Qing Li,Yuran Cheng,Mei Dong,Zuyi Zhang,Xinmiao Zhu,Yingxin Liu,Yong Sun
CoRe bimetallic catalysts with low loading were designed for hydrodeoxygenation of levulinic acid to γ-valerolactone. Results show that the 1 wt % Co0.5Re0.5/TiO2 catalyst achieved the highest yield of γ-valerolactone (>99%) at 220 °C, 3 h, a 1,4-dioxane solvent and Co/levulinic acid molar ratio of 1:1760, with a turnover frequency (TOF) of 1328 h–1. The catalyst can be reused four times with only slight activity loss. The catalyst was characterized with various physicochemical measurements, and its adsorption styles with H2 and levulinic acid were calculated by density functional theory. The results reveal that four main factors are related to its excellent catalytic performance. First, the Re oxides synergize with Co by spillover of the dissociated H atoms, which increases the apparent dispersion of Co and promotes the reaction. Second, the low loading of 1 wt % allowed the metal nanoparticles to be well dispersed with a very fine size of ca. 1.24 nm, which may expose more active sites to the substrate and result in a higher catalytic efficiency. Third, CoRe formed an amorphous alloy with the formula Co-ReO1.6, which showed a synergistic effect during the reaction. Finally, the TiO2 support was nonporous and hydrophilic, which would be beneficial for the mass diffusion of the reaction components to be adsorbed/desorbed onto the vicinity of the metallic active sites and lead to a high TOF in the hydrodeoxygenation process.
研究领域:
化学工程
·
催化科学
✓ 已验证
产品关联
DOI
高影响因子
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