APPLIED CATALYSIS B-ENVIRONMENTAL
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2019
·
IF 14.229
Xiaoqing Gao,Shanhui Zhu,Mei Dong,Jianguo Wang,Weibin Fan
Highly efficient synthesis of valuable γ-valerolactone (GVL) by levulinic acid (LA) hydrogenation is still a challenge for Ru-based catalysts under mild condition. In this work, we have reported that ultrathin TiO 2 nanosheets supported Ru nanoparticles showed extraordinarily high catalytic activity, GVL yield (99.1%) and reusability owing to the formation of Ru O Ti interfacial structure. The turnover frequency (TOF) reached as high as 19,045 h −1 at 100 °C, much higher than those of Ru/SiO 2 , Ru/GO, Ru/MoS 2 , and commercial Ru/C. DFT calculation elucidates that the dominant reaction pathway of LA hydrogenation to GVL is preferentially hydrogenated to CH 3 CHOCH 2 CH 2 COOH*, followed by cyclization to CH 3 (OH)C 4 OH 4 OH* (GVL − OH) and final dehydroxylation, irrespective of surface structure. Compared to Ru (0 0 2) facet, Ru/TiO 2 interfacial structure changes the rate-determining step from initial hydrogenation to cyclization, which greatly declines the activation barrier from 0.81 eV to 0.48 eV.
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JOURNAL OF CHEMICAL THERMODYNAMICS
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2016
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IF 2.196
Dongshun Deng,Yaotai Jiang,Xiaobang Liu,Zhiliang Zhang,Ning Ai
Solubilities of CO 2 have been determined in five deep eutectic solvents (DESs) at temperatures (303.15–333.15) K with 10 K intervals under a pressure of (0–600.0) kPa using isochoric saturation method. These DESs were prepared from levulinic acid (LA) and quaternary ammonium salt (acetylcholine chloride, ACC; tetraethylammonium chloride, TEAC; tetraethylammonium bromide, TEAB; tetrabutylammonium chloride, TBAC; and tetrabutylammonium bromide, TBAB) with the mole ratio of 3:1. Henry’s constants and thermodynamic properties such as Gibbs energy, enthalpy and entropy of dissolution were deduced by correlating the solubility data. Results demonstrated that the solubility of CO 2 in DESs increased with the increasing pressure or the decreasing temperature. The enthalpies of dissolution were all exothermal in each condition. The Henry’s law constants based on mole fraction and molality of CO 2 in DESs vary from (12.30 to 28.66) MPa and (1.79 to 3.94) MPa, respectively.
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RSC Advances
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2014
·Vol. 4
·期 29
·14985-14992
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IF 3.708
Jiang Li,Dao-jun Ding,Lu-jiang Xu,Qing-xiang Guo,Yao Fu
A biphasic system consisting of THF and water was studied to achieve the integrated conversion of cellulose and hemicellulose in lignocellulosic biomass to levulinic acid. As compared to previous studies using GVL as solvent, the utilization of a lower boiling point solvent, THF, also achieves the simultaneous hydrolysis of C6 and C5 carbohydrates in lignocellulosic biomass, and the results of simultaneous hydrolysis are comparable. Furthermore, it offers an alternative operation procedure after the hydrolysis. A distillation process is not only used to achieve the effective separation of the solid residue from the desired products, but it also helps in the complete isolation of furfural and formic acid from levulinic acid. Consequently, the utilization of by-product formic acid in the hydrogenation of furfural to furfuryl alcohol is explored, and the process is achieved with both model substrates and the feed from the lignocellulosic biomass feedstock. The hydrolysis of furfuryl alcohol gave C5 carbohydrate-derived levulinic acid. We finally explored the integrated conversion with five biomass raw materials, and the total yield of levulinic acid was quite obviously promoted by the additional conversion of pentose.
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BIORESOURCE TECHNOLOGY
·
2024
·
IF 9.7
Huanhuan Zhang,Liutao Hou,Weihong Zhang,Yucheng Lin,Xueli Liu,Shiqiang Zhao,Chun Chang
The purpose of this study is to design and investigate two coupling processes for acid-catalyzed hydrolysis of corncob, achieving the simultaneous preparation of biomass-based furfural and levulinic acid (LA). Meanwhile, high concentration and yield of LA were obtained through a situ feeding strategy of pretreated furfural residue with high solids loading (20%, w/v). In Scenario A, 2-methyltetrahydrofuran was selected as the solvent for the LA extraction process compared with the neutralization process in Scenario B. Techno-economic assessment results show that Scenario A is technically feasible and cost-competitive, with an internal rate of return of 21.92%, a net present value of 121 million US dollars, a carbon efficiency of 72%, an environmental factor of 4.38, and a process mass intensity of 32.19. This study will provide new insights for fully utilizing lignocellulosic biomass to prepare renewable energy resources, comprehensively evaluating the economic feasibility, and promoting green and low-carbon development.
研究领域:
生物化学
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可再生资源
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环境科学
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PubMed
高影响因子
FUEL
·
2024
·
IF 6.7
Yaqi Duan,Conghao Ku,Yuping Lv,Yantao Wang,Weiran Yang
Due to its unique physical and chemical properties, applying activated carbon nanomaterials as catalysts gradually become a hot research topic. Herein, the synergistic catalytic effect of activated carbon nanoparticles and CaO for highly selective oxidation of levulinic acid to citramalic acid was first reported. Among various activated carbons tested (commercially available and biomass-derived), the one obtained from Nanjing Chemical Reagent Co., Ltd. exhibits the best catalytic activity due to its large surface area, suitable pore structure, abundant active sites, and excellent O 2 activation ability. The levulinic acid conversion and citramalic acid selectivity respectively reached 100 % and 82.8 % at 90 °C for 0.5 h under 0.5 Mpa O 2 . Further, the 3D flower-like CaO/carbon composite (CaO/CF) was developed, which also showed excellent catalytic activity for the selective oxidation of levulinic acid to citramalic acid, with 91 % levulinic acid conversion and 81.8 % citramalic acid selectivity under otherwise the same reaction condition. The mechanistic study indicated that superoxide anion radical ( O 2 – ), Ca 2+ and OH – all play a crucial role in levulinic acid oxidation. This work may promote the application of activated carbon nanomaterial as an effective catalyst for selective oxidation reactions.
研究领域:
化学工程
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材料科学
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SEPARATION AND PURIFICATION TECHNOLOGY
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2026
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IF 9.1
Jiaxin Tang,Jingke Liu,Xinhui Chen,Quanyuan Qiu,Wanqi Peng,Xinyuan Fu,Chenxi Shi,Xiaoqing Lin
Efficient separation of levulinic acid (LA) from biomass hydrolysates remains a major challenge, particularly at high LA concentrations where conventional fixed-bed adsorption suffers from increased competitive adsorption, long cycle times, and high solvent consumption. This study developed a four-zone continuous chromatographic separation process using the hyper-cross-linked resin SY-01 for the recovery of high-concentration LA from simulated biomass hydrolysates. Adsorption equilibrium, competitive adsorption, and kinetic behaviors were first investigated, followed by optimization of fixed-bed adsorption and construction of a continuous chromatographic system. The separation performances of the two operating modes were then quantitatively compared under identical conditions. SY-01 exhibited high adsorption capacity and rapid adsorption kinetics toward LA, while the continuous system achieved stable operation with a peak LA concentration of 321.15 g/L (3.21-fold enrichment). Compared with conventional fixed-bed adsorption, continuous operation reduced cycle time by 86.8%, ethanol consumption by 65.7%, and water consumption by 40.0%, while substantially increasing process throughput. These results demonstrate that integrating SY-01 with four-zone continuous chromatography provides an efficient, economical, and environmentally friendly strategy for industrial recovery of high-concentration levulinic acid.
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LWT-FOOD SCIENCE AND TECHNOLOGY
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2026
·
IF 7.1
Guohua Teng,Min Zhou,Initizar Anwar,Yang Liu,Fuyi Li,Yanxu Chang,Yidan Wang,Yuefei Wang,Fei Tian
Flavonoids in Scutellaria Radix ( SR ) exhibit significant pharmacological activities, yet conventional extraction methods often suffer from low efficiency and poor selectivity. Here, a green and effective strategy was developed using deep eutectic solvent (DES)-functionalized magnetic nanoparticles for selective flavonoid enrichment. Forty-eight DESs were screened, and levulinic acid/L-proline (2:1) was identified as the optimal system. The selected DES was employed to synthesize Fe 3 O 4 @SiO 2 @DES, which demonstrated high specificity and adsorption performance in magnetic solid-phase extraction. Under optimized conditions, adsorption efficiencies for four representative flavonoids ranged from 0.770 ± 0.01 to 0.983 ± 0.002, with desorption recoveries of 0.551 ± 0.003 to 0.919 ± 0.019. The method showed excellent linearity (R 2 ≥ 0.9998) and low limits of detection and quantification (0.01-0.35 μg mL −1 and 0.03-0.98 μg mL −1 , respectively). Moreover, the adsorbent retained high adsorption efficiency after six reuse cycles, demonstrating stability and reusability. This work provides a sustainable and selective approach for flavonoid enrichment from SR and highlights the potential of DES-functionalized magnetic nanomaterials as an eco-friendly alternative to conventional organic solvent-based extraction.
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MOLECULES
·
2024
·Vol. 29
·期 16
·3779
·
IF 4.2
Pan Hou,Haopeng Su,Keyan Jin,Qiang Li,Wenfu Yan
γ-valerolactone (GVL), derived from biomass, is a crucial platform compound for biofuel synthesis and various industrial applications. Current methods for synthesizing GVL involve expensive catalysts and high-pressure hydrogen, prompting the search for greener alternatives. This study focuses on a novel zirconium phosphate (ZrP)-pillared zeolite MCM-36 derivative catalyst for converting levulinic acid (LA) to GVL using alcohol as a hydrogen source. The incorporation of ZrP significantly contributes to mesoporosity and greatly enhances the acidity of the catalysts. Additionally, we employed31P MAS NMR to comprehensively investigate the influence of phosphorus species on both the acidity and the catalytic conversion of LA to GVL. By adjusting the Zr-to-P ratios, we synthesized catalysts with enhanced acidity, achieving high conversion of LA and selectivity for GVL. The catalyst exhibited high recyclability, showing only minor deactivation over the course of five cycles. Furthermore, the catalyst was successfully applied to the one-pot conversion of furfural to GVL, showcasing its versatility in biomass conversion. This study highlights the potential of the MCM-ZrP1 catalyst for sustainable biomass conversion and offers insights for future research in renewable energy technologies.
研究领域:
化学工程
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可再生能源
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催化科学
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DOI
PubMed
高影响因子
JOURNAL OF CATALYSIS
·
2024
·
IF 6.5
Xiaoqing Gao,Shanhui Zhu,Mei Dong,Hongyan Zheng,Yanfeng Xue,Xiaojing Cui,Yulan Niu,Weibin Fan
Highly efficient synthesis of valuable γ-valerolactone (GVL) by levulinic acid (LA) hydrogenation is of interest for biomass refinery, but it suffers from great challenge to design highly active Ru-based catalyst at low temperature. ZIF-8 derived ZnO@NC nanocomposite can firmly anchor Ru nanoparticles to create strong Ru-ZnO interfacial structure, as revealed by characterization techniques and DFT calculations. By optimizing Ru content and ZnO particle size, Ru/ZnO@NC achieved excellent reaction activity with a turnover frequency (TOF) of 6032 h −1 at low temperature of 40 °C, which is never reported before. After etching the accessible ZnO, the TOF value was significantly declined to 125 h −1 on Ru/ZnO@NC-HF owing to the lack of effective Ru-ZnO interface. DFT calculation results demonstrate that the Ru-ZnO interfacial structure can facilitate the activation of intermediate CH 3 CHOCH 2 CH 2 COOH* and remarkably decline the activation energy barrier of rate-determining step (CH 3 CHOCH 2 CH 2 COOH + H = HPA) from 1.28 eV to 0.82 eV, thus leading to excellent activity of LA hydrogenation at low temperature.
研究领域:
催化化学
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生物质能
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材料科学
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高影响因子
Molecular Catalysis
·
2022
·
IF 5.089
Canshuo Gu,Lungang Chen,Yong Liu,Xinghua Zhang,Jianguo Liu,Qi Zhang,Chenguang Wang,Longlong Ma
The production of furanic biofuel 2-methyltetrahydrofuran (2-MTHF) has been studied by hydrodeoxygenation of biomass-derived levulinic acid (LA) over bimetallic NiCo/γ-Al 2 O 3 catalyst. The contents of Ni and Co in NiCo/γ-Al 2 O 3 were investigated. The Ni 5 Co 25 /γ-Al 2 O 3 catalyst gave high activity in hydrodeoxygenation of LA with a 73.4% yield of 2-MTHF under optimal conditions. The crystal phase, valence states, acidity and basicity of catalysts were measured by multiple characterizations to understand the relationships among 2-MTHF yields and catalyst properties. XPS characterization revealed that the number of metal oxides increased on bimetallic catalysts while the reduced metals occupied on monometallic catalysts. The bimetallic catalysts also presented increased acidity than that of monometallic catalysts. These distinct properties were also observed among bimetallic catalysts with different contents of Ni and Co, which were responsible for different performances. Besides, the solvent effect on the structure of 1,4-pentanediol, which was further converted to 2-methyltetrahydrofuran, was disclosed by molecular dynamics simulations.
研究领域:
化学工程
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催化
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生物燃料
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材料科学
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高影响因子
FUEL
·
2022
·
IF 8.035
Puxiang Yan,Haiyong Wang,Yuhe Liao,Pengyao Sun,Chenguang Wang
Catalytic valorization of biomass into chemicals and fuels plays a key role in order to achieve net-zero greenhouse gas emissions. Herein, a series of hierarchical ZSM-5 zeolites were synthesized by the post-treatment method to transform furfural alcohol (FAL) to levulinic acid (LA). ZSM-5 obtained from tandem alkaline treatment (0.2 M NaOH) and acid washing (0.1 M HCl), denoted as ZSM-5-OH 0.2 -H, exhibited the highest activity, affording 76.2% LA yield in 9:1 acetone–water mixed solvents at 393 K for 0.5 h. The enhanced adsorption capacity and acid accessibility of FAL on zeolite mediated by the introduction of mesopores, as well as the reduced secondary reactions of the generated LA due to few Al atoms in straight and sinusoidal channels (as confirmed by UV–vis diffuse reflectance), were responsible for the outstanding catalytic performance of ZSM-5-OH 0.2 -H. The structure–activity relationship revealed that regulating the porous structure and Al distribution of ZSM-5 was an effective strategy to enhance its hydrolytic performance of FAL to LA. Moreover, ZSM-5-OH 0.2 -H could be reused for three reaction cycles without significant loss in catalytic activity.
研究领域:
化学工程
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催化
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生物质转化
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可持续化学
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DOI
高影响因子
ChemSusChem
·
2023
·Vol. 16
·期 21
·e202300754
·
IF 8.4
Jing Guo,Feng Li,Yuting Chu,Peng Zou,Chuang Li
Graphical The 10 % Ni@CeOx catalyst exhibits excellent catalytic efficiency in the reduction amination of levulinic acid to prepare 1,5-dimethyl-2-pyrrolidone. 1,5-dimethyl-2-pyrrolidone (MNMP), as a highly efficient green solvent, can be obtained from biomass-derived levulinic acid and its esters with 100 % conversion and 96.8 % yield over a 10 % Ni@CeOx catalyst at 140 °C, 2 MPa H 2 , 8 h, and with water as the solvent. Structure-property correlation investigations were performed with diverse characterization methods, including BET, XRD, XPS, TEM, HAADF-STEM, H 2 -TPR, NH 3 -TPD, CO 2 -TPD and FT-IR, and the results revealed that the excellent catalytic performance of the 10 % Ni@CeOx catalyst was mainly resulted from the strong interaction between Ni and CeOx, which formed more catalytic active sites and contributed to higher reductive amination efficiency. Besides, the 10 % Ni@CeOx catalyst had a chemisorption effect on LA. This was also the key to the excellent catalytic activity of the 10 % Ni@CeOx catalyst. The 10 % Ni@CeOx catalyst exhibited great stability throughout 6 reaction runs and excellent catalytic efficiency in the kilogram scale preparation of MNMP. This work provides a low-cost, efficient, and environmentally friendly heterogeneous catalytic system for the production of MNMP.
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