EUROPEAN POLYMER JOURNAL
·
2026
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IF 6.8
Mingtao Ding,Song Feng,Tongjun Yang,Yuanlong Guo,Lihua Zhang,Haibo Xie
Chitin dissolution is prerequisite to allow its homogeneous processing and develop value-added regenerated/derivative chitin-based materials. In this work, in combination of [EMIM][OAc] ionic liquids, biomass-derived γ -valerolactone (GVL) was delicately screened as a co-solvent to construct benign organic electrolyte solutions (OESs) for chitin dissolution and homogeneous processing. Kamlet-Taft parameters ( α , β , and π*) of [EMIM][OAc]/GVL OESs with varying molar ratios are examined. Introduction of [EMIM][OAc] into GVL can notably increase the polarity, supported by the increased E T (30) values. The NMR studies of N -acetylglucosamine (GlcNAc, the repeating unit of chitin) solvation further indicate that the hydrogen bonding between GlcNAc and both the anions and cations of the ILs. Rheological properties of chitin/[EMIM][OAc]/GVL solutions are studied, and lower viscous activation energy ( E η ) accompanies the increase of GVL content in the OESs, as the addition of GVL reduces the energy barrier for viscous flow and facilitates the mobility of chitin molecular chains. Furthermore, the potential of the chitin solutions for homogeneous processing into films is primarily demonstrated via a conventional solution casting approach using water as the coagulation bath. Regenerated chitin films are systematically characterized by FTIR, NMR, XRD, TGA, UV–vis, SEM and tensile tests. Thus, it seems that the [EMIM][OAc]/GVL OESs present a green platform for fabricating chitin-based materials.
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高影响因子
INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
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2025
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IF 8.5
Tianyuan Xiao,Jiahui Song,Wenchao Jia,Yanning Sun,Yanzhu Guo,Pedram Fatehi,Haiqiang Shi
The chemical bond cleavage of lignin is a research focus for achieving depolymerized lignin for such applications as adhesives, fuels, fertilizers, etc. The depolymerization of an industrially available sustainable material, i.e., industrial alkali lignin, in LiBr·3H 2 O/HBr-γ-valerolactone (GVL) was systematically investigated in this study. It was observed that using 3/1 mL/g of HBr/lignin and 8/1 mL/g of GVL/lignin at 110 °C for 90 min, i.e., optimized conditions, resulted in lignin derivatives with an M w of 1889 g/mol and M n of 895 g/mol. The characteristics of the products were studied using FTIR, NMR, SEM, and DLS techniques. The results confirmed that the Hibbert-ketone end group was formed, while the structure of the aromatic ring was not changed on the depolymerized lignin. After the depolymerization process, the hydroxyl content in lignin increased from 1.91 mmol/g to 2.96 mmol/g. The product derived from the LiBr·3H 2 O/HBr-GVL depolymerization system displayed a spherical particle morphology. The addition of GVL to lignin depolymerization processes improved the bonding between lignin and inorganic molten salts, thereby promoting the acid-catalyzed cleavage of aryl ether bonds in lignin. Current research supports the conclusion that LiBr·3H 2 O/HBr-GVL lignin depolymerization is a sustainable and effective chemical pathway for generating depolymerized lignin.
研究领域:
化学工程
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材料科学
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DOI
PubMed
高影响因子
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
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2024
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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
RENEWABLE ENERGY
·
2020
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IF 6.274
Han Chen,Qiong Xu,Du Zhang,Wenzhu Liu,Xianxiang Liu,Dulin Yin
A series of mesoporous nickel catalysts with different molar ratios of citric acid and nickel nitrate were synthesized via a simple two-step method by solid-state grinding and in-situ reduction; these catalysts were further employed for the catalytic transfer hydrogenation of levulinate esters to γ-valerolactone (GVL) with 2-propanol as the hydrogen donor. The effects of C 6 H 8 O 7 /Ni molar ratios , catalyst dosage, reaction temperature and time on the catalytic performance were investigated. An excellent GVL selectivity of 99.1% and an ethyl levulinate (EL) conversion of 100% could be achieved at 180 °C in 6 h over Ni-1.0 catalyst with a 1.0:1 M ratio of C 6 H 8 O 7 /Ni. The characterization results showed that the Ni-1.0 catalyst was composed of mesoporous metallic Ni bulk and a surface Ni–NiO composite, and the acid sites of NiO played a synergistic catalytic role in producing GVL from EL. The superior mesoporous structure and large surface area of Ni-1.0 increased the atomic utilization rate of nickel metallic active centers. Moreover, Ni-1.0 catalyst could be easily separated and reused ten times, with an EL conversion above 95% remaining in each recycle. This work provids a highly efficient and environmentally friendly catalytic procedure for the conversion of biomass into GVL, a fuel additive compound.
研究领域:
化学工程
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可再生资源与环境科学
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高影响因子
RSC Advances
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2017
·Vol. 7
·期 48
·29916-29924
·
IF 3.108
Yuanshuai Zhu,Wenzhi Li,Yijuan Lu,Tingwei Zhang,Hasan Jameel,Hou-min Chang,Longlong Ma
A resorcinol-formaldehyde resin carbon (RFC) catalyst with a well-developed, ordered, mesoporous framework was prepared using a soft template method at room temperature. The carbon was sulfonated in water using sulfanilic acid under mild atmospheric conditions. The sulfonated RFC (S-RFC) was characterized by N2 adsorption–desorption, elemental analysis, TEM, XPS, and FT-IR. It was determined that S-RFC is an efficient solid acid catalyst for furfural production from xylose and corn stover in γ-valerolactone (GVL). The effects of reaction time, reaction temperature, catalyst loading, substrate dosage and water concentration were investigated. 80% furfural yield and 100% xylose conversion were obtained from xylose at 170 °C in 15 min with 0.5 g catalyst. Comparatively, 68.6% furfural yield was achieved from corn stover at 200 °C in 100 min when using 0.6 g catalyst. Since there was no discernable decrease in furfural yield after multiple conversions utilizing the same catalyst, the recyclability of the catalyst is considered good.
研究领域:
生物化学
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可再生能源
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高影响因子
APPLIED CATALYSIS A-GENERAL
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2018
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IF 4.521
Zhenzhen Lin,Mengting Luo,Yindi Zhang,Xiaoxue Wu,Yanghe Fu,Fumin Zhang,Weidong Zhu
Heterogeneous catalytic conversion of biomass-derived methyl levulinate (ML) to γ-valerolactone (GVL) is highly attractive as a sustainable route to mitigating the dependence on nonrenewable fossil resources. However, this route is limited by its low selectivity toward GVL and severe reaction conditions. Here, we present a synergistic catalytic process that offers exclusive GVL selectivity with complete ML conversion under mild conditions (80 °C, 0.5 MPa of H 2 pressure). This is achieved over a dual-functionalized catalyst of Ru nanoparticles (Ru-NPs) and Brønsted acid SO 3 H groups in a Cr-based metal-organic framework (MIL-101). The Ru-NPs served as metal sites for the hydrogenation of ML to methyl-3-hydroxyvalerate (MHV) and the acidic SO 3 H moieties promoted the cyclization of MHV to generate GVL via lactonization. In contrast, GVL production was significantly suppressed over the physically mixed congener (2.0 wt% Ru/MIL-101 + MIL-101-SO 3 H). This result demonstrates an unrivalled advantage of the dual integration of metal/acid sites in a single MOF crystal, and the relative amount of sulfonic acid groups in the catalyst can exert significant influence on the overall catalytic performances. The activation energies for the hydrogenation and lactonization steps with the developed catalyst were 29.5 and 42.1 kJ/mol, respectively, which are much lower than those observed with the traditional 5.0 wt% Ru/AC catalyst.
研究领域:
化学工程
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催化科学
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高影响因子
FUEL PROCESSING TECHNOLOGY
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2018
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IF 3.956
Feng Huang,Wenzhi Li,Qingchuan Liu,Tingwei Zhang,Shengxin An,Dawei Li,Xifeng Zhu
A carbon solid acid was made by grafting benzenesulfonic acid groups on the tobacco stem-derived porous carbon, which was prepared from waste tobacco stem by simple carbonization . The catalyst was characterized by scanning electron microscope (SEM), N 2 adsorption-desorption, Fourier transform infrared spectroscopy (FT-IR), elemental analysis (EA), pyridine FT-IR spectroscopy and X-ray photoelectron spectroscopy (XPS). The catalyst exhibited excellent catalytic activity for 5-hydroxymethylfurfural (HMF) production from fructose and glucose in γ-valerolactone/water solvent, and high yields of HMF reached 93.7 and 43.8%, respectively. In addition, the high yields of total furans derived from fructose and glucose reached 96.8 and 54.1%, respectively. The benzenesulfonic acid group grafted onto the surface of inner pores of carbon allowed reusing the catalyst for at least five runs without obvious activity reduction. The good performance of the tobacco stem-derived carbon solid acid was determined by the unique surface active sites, such as high density of Brønsted acid, Lewis acid sites, oxygen-containing weak acidic sites and protonated nitrogen-containing functional groups. This study offered a promising approach for efficient carbohydrate conversion.
研究领域:
化学工程
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可再生资源转化
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高影响因子
Molecular Catalysis
·
2023
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IF 4.6
Bo Li,Haijun Guo,Zhen Xiong,Lian Xiong,Shimiao Yao,Mengkun Wang,Hairong Zhang,Xinde Chen
γ-valerolactone (GVL) is a sustainable chemical, which can be obtained by hydrogenation of levulinic acid (LA) and levulinate. Herein, we reported a solvent-free hydrogenation of butyl levulinate (BL) to GVL and 1,4-pentanediol (1,4-PDO) over a skeletal Cu-Al-Zn catalyst. The skeletal Cu-Al-Zn catalyst was prepared from Devarda's alloy by alkali leaching and the catalyst was characterized by different analysis methods. The aluminum in the Devarda's alloy was dissolved by sodium hydroxide in the leaching process and many active Cu atoms were generated on the catalyst surface and the skeletal Cu-Al-Zn exhibited many micrometer-scale irregular particles with rough surface. The skeletal Cu-Al-Zn catalyst showed the excellent performance in the solvent-free hydrogenation of BL to GVL under constant hydrogen pressure (5 wt% catalyst loading, 180°C, 6 MPa of H 2 , 6 h): the LA conversion was 100%, the GVL yield was 74.75% and the 1,4-PDO yield was 25.63%. Moreover, the catalyst showed stable performance and it was reusable up to 5 times without apparent loss of activity. A stable hydrogen pressure with Zn would suppressed the dehydration of 1,4-PDO.
研究领域:
催化
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绿色化学
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可持续化学
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高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2023
·
IF 22.1
Xinlei Ji,Jia Kou,Gökalp Gözaydın,Xi Chen
Chitin biorefinery offers a unique opportunity to sustainably produce highly-valued organonitrogen compounds such as the versatile pharmaceutical precursor 3-acetamido-5-acetylfuran (3A5AF), bypassing the Haber process and mitigating the consumption of fossil feedstocks. However, the reported protocols engaged large quantities of toxic organic solvents and required harsh conditions. In this work, a highly efficient catalytic system has been developed in the nontoxic, biobased γ-valerolactone (GVL) solvent under relatively mild conditions. 3A5AF was selectively obtained with an unprecedent yield of 75.3% at 140 °C for 2 h by adding NH 4 SCN and HCl. The high yielding was exclusively promoted by a dissolution-dehydration effect. Based on the UPLC-TOF-MS and NMR analyses, the presence of NH 4 SCN has induced a very rapid NAG conversion possibly by coordinating with the acetamido group and the hydroxyl groups, and the 3A5AF product was obtained in a subsequent dehydration pathway from NAG with the Chromogen I and Chromogen III as the intermediates.
研究领域:
生物化学
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可再生资源与环境科学
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高影响因子
CATALYSIS LETTERS
·
2023
·
IF 2.8
Xiang Yuchen,Zhang Huiming,Zhang Jingyi,Xu Qiong,Liu Xianxiang,Yin Dulin
Comprehensive use of available biomass, especially low-cost forestry waste to produce bioenergy, materials have great meaning for realization of green and sustainable chemical processes. In this work, forestry sawdusty waste (SD) was used to produce biochar (SDBC-P) via a H 3 PO 4 assisted hydrothermal carbonization method. And a novel zirconium-coordinated biochar catalyst Zr-SDBC-P has been prepared by self-assembly method. Characterization results revealed that hydrothermal carbonization in the presence of H 3 PO 4 promoted the formation of oxygen-containing functional groups (–COOH, Ar–OH) which were used as ligand to obtain high contents of Lewis acid − base sites (Zr 4+ –O 2− ). Zr-SDBC-P-4 showed satisfactory catalytic activity in synthesis of bioderived γ-valerolactone (GVL) from ethyl levulinate (EL). EL conversion of 98.2% and GVL selectivity of 85.4% were obtained within 5 h at 170 °C. In addition, Zr-SDBC-P-4 displayed outstanding chemical stability. There was no obvious decrease of GVL yield after being used for six cycles. Overall, this work offered a viewpoint to design catalyst from value-added utilization of biomass waste. Graphical Abstract
研究领域:
生物质化学
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催化化学
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可持续化学
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高影响因子
JOURNAL OF SUPERCRITICAL FLUIDS
·
2024
·
IF 3.4
Dongjie Zhang,Yue Zhang,Yifei Li,Zanhong Wang,Yin Zhang,Haitao Li
This study reports a novel method for γ-valerolactone (GVL) production from ethyl levulinate (EL) utilizing non-noble metal catalysts within a supercritical isopropanol (IPA) system. Nickel-loaded nickel–aluminum oxide nanosheets (Ni X Al-R) were fabricated via hydrothermal treatment of Ni–Al layered double hydroxide precursors, followed by hydrogen reduction at 550 °C for 1.5 h. Using Ni X Al-R as the catalyst and IPA as the hydrogen donor , we achieved notable results: 82.7% EL conversion, 73.6% GVL yield, and 1.178 mol GVL g −1 h −1 reaction efficiency after 1.5 h in supercritical IPA. The catalytic activity of Ni X Al-R remained stable over five catalytic cycles. The surface of Ni X Al-R exhibits abundant oxygen vacancies and unsaturated Al species (Al x+ ), which promote the initial transfer hydrogenation of EL to form the ethyl 4-hydroxypentanoate (4-HPE) intermediate. Simultaneously, the supercritical IPA environment overcomes mass transfer limitations at the solid–liquid interface between 4-HPE and the catalyst, thereby facilitating the Al x+ -catalyzed intramolecular esterification of 4-HPE into GVL.
研究领域:
化学工程
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催化科学
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可再生化学品合成
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DOI
高影响因子
危险品化学品经营许可证（带存储）