FUEL
·
2021
·
IF 6.609
Xueying Gao,Xin Yu,Lincai Peng,Liang He,Junhua Zhang
A magnetically-recoverable multifunctional catalyst (Fe 3 O 4 /ZrO 2 @MCM-41) was tailored by the impregnation of ZrO 2 supported on mesoporous MCM-41 coated Fe 3 O 4 nanoparticles, which successfully served as a monolithic catalyst for the cascade conversion of furfural (FAL) giving high yield to γ-valerolactone (GVL), a versatile platform molecule. The ordered hexagonal framework of the parent MCM-41 well reserved after the embedding of Fe 3 O 4 and ZrO 2 . The incorporation of Fe 3 O 4 could not only impart the catalyst with a strong magnetism, but also tune its acidity to promote GVL production. An impressive yield of 85% was accomplished straight from FAL processing with iso -propanol as a hydrogen donor and solvent. The kinetic study demonstrated higher activation energy for levulinate-to-GVL step (86.9 kJ/mol) than FAL transfer hydrogenation (35.0 kJ/mol) and subsequent alcoholysis process (51.0 kJ/mol). The catalyst could be fully recovered by an external magnetic field and showed good reusability. The sustainability of this conversion represents greatly improved by the process intensification based on one-pot reaction, magnetically-recoverable multifunctional catalyst, and mild operating conditions without using gaseous hydrogen.
研究领域:
催化化学
·
纳米材料科学
·
可再生化学
✓ 已验证
DOI
高影响因子
CELLULOSE
·
2020
·Vol. 27
·期 7
·3581-3590
·
IF 4.21
Yang Xue,Song Yanliang,Ma Sen,Zhang Xu,Tan Tianwei
A method for isolating components of lignocellulose in hybrid poplar by using an organic solvent (γ-valerolactone) in combination with a solid organic acid ( p -toluenesulfonic acid) is studied here. The combined hydrolysis factor (CHF) was used to measure the severity of the pretreatment conditions and to find the optimal reaction conditions (CHF = 54.99) by judging enzymatic saccharification and characterization of lignin residual. At this pretreatment strength, 91.67% hemicellulose and 86.14% lignin in lignocellulose were effectively removed, and the enzymatic hydrolysis of cellulose residue reached 84.84%. Hemicellulose was hydrolyzed to 4.39 g L −1 of xylose, and a portion was converted to 2.95 g L −1 of furfural and 3.59 g L −1 of acetic acid. The molecular weight, polydispersities and phenolic hydroxyl groups content of the isolated lignin were 1587 g mol −1 , 1.04 and 3.64 mmol g −1 respectively, which indicated that the lignin had the potential to be a phenolic resin material and wood polyurethane foam. In summary, this method effectively separated three components of lignocellulose and obtained high purity cellulose and lignin.
研究领域:
生物化学
·
生物技术
·
材料科学
✓ 已验证
DOI
高影响因子
JOURNAL OF MOLECULAR LIQUIDS
·
2025
·
IF 5.2
Zi-Quan Wang,Ya-Peng Du,Xiao-Ping Zheng,Yu Chai,Yu-Cang Zhang,Yan-Zhen Zheng
The direct conversion of raw lignocellulosic waste into specialty chemicals such as levulinic acid (LA) has the potential to significantly enhance biorefinery profitability. Here, we demonstrated that incorporating γ-valerolactone (GVL) as a co-solvent during the SO 3 H-functionalized ionic liquid-catalyzed conversion of bagasse in water markedly enhanced reaction rates and catalytic activity, achieving a LA yield as high as 76.1 % with a 1:1 vol ratio of GVL to water. This catalytic system also effectively converted other lignocellulosic waste to LA. Reaction constants and activation energies for the bagasse dehydration process to LA were obtained. Comprehensive characterization via Fourier transform infrared spectroscopy (FTIR), scanning electron microscopy (SEM), and X-ray diffraction (XRD) elucidated significant changes in functional groups, surface morphology, and crystallinity index of solid residues over extended reaction times. Notably, hemicellulose and cellulose were converted within 4 h, with lignin remaining in the solid residues and forming by-products after prolonged reaction times. This efficient one-pot conversion method showed promise as a sustainable approach to transform agricultural waste into LA, offering new opportunities for eco-friendly resource utilization.
研究领域:
生物化学
·
可再生能源
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Mengli Zhou,Sichan Li,Haojie Tian,Xinyu Liu,Zhimin Wu,Qiying Liu,Jianchun Jiang
Levlinic acid (LA) and its derived γ-valerolactone (GVL) are the two important biomass derived platform molecules, which showed wide application in the fields of fine chemicals, drug and liquid fuel industrials. Considering the coupling of sequential steps for glucose to LA and GVL, selective production of LA and GVL via glucose one-pot conversion in water is an open challenge. Herein, we used metal chlorides as the acidic catalyst for glucose conversion to LA, obtaining the high yield of 77.8 C-mol% over SnCl 4 . Moreover, using the SnCl 4 and Ru/C as the combined catalyst, glucose or cellulose could be converted to GVL with the high yield of 60.1 or 57.9 C-mol% in the case of in situ hydrogenation by formic acid (the by-products during LA formation) decomposition. The formation of LA was responsible for the cooperative effect of BAS (Bronsted acid sites) and LAS (Lewis acid sites) of SnCl 4 for accelerating glucose isomerization, fructose dehydration followed by 5-hydroxymethyl furfural (HMF) rehydration, while the GVL production is relative to the highly efficient formic acid decomposition to H 2 followed by LA hydrogenation to GVL over Ru/C. This study provided an avenue for facile and highly efficient conversion of biomass and the derivatives to LA and GVL using commercial catalysts.
研究领域:
催化化学
·
生物质能源
·
绿色化学
·
可再生化学品
·
多相催化
✓ 已验证
产品关联
DOI
高影响因子
Journal of Cleaner Production
·
2025
·
IF 10
Hongguang Zhang,Zi Yu,Yongxin Liang,Tao Gan,Zuqiang Huang,Huayu Hu,Yanjuan Zhang
The utilization of organic molecules as in-situ hydrogen donors for producing γ-valerolactone (GVL) biofuel from biomass-derived levulinic acid (LA) represents one of the promising sustainable approaches. However, this process still faces challenges, including the difficult activation of the hydrogen source and the transport limitations of active hydrogen species. Herein, a Co-MnO/spontaneously polarized ceramic-carbon (Co-MnO/SPCE-C) composite catalyst, featuring a unique spontaneous polarization effect, was developed for catalytic transfer hydrogenation (CTH) of LA to GVL in the isopropanol/H 2 O (volume ratio = 1/19) cosolvent system. Co-MnO/SPCE-C contributed to an outstanding LA conversion of 99.9% and a favorable GVL yield of 93.5%, surpassing the performance achieved by comparative catalysts. Various characterization techniques demonstrate that SPCE with far-infrared emission and surface electric field increased the oxygen vacancies, thereby promoting hydrogen spillover and enhancing the properties of CoO x –MnO acidic sites. The 17 O NMR spectra reveal that SPCE activated water clusters by weakening the hydrogen bonding network. Moreover, D 2 O experiments show that SPCE facilitated the participation of water in the reaction. This work provides valuable insights into the development of an efficient strategy for producing GVL from LA. Before the catalyst can be considered for commercial applications, the focus in the future should be on a comprehensive computational analysis, long-term evaluation of catalyst stability, and additional industrial-scale testing.
研究领域:
化学工程
·
材料科学
·
催化反应
✓ 已验证
产品关联
DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2020
·
IF 3.573
Guangyue Xu,Chuang Li,Tianyu Deng,Chenguang Wang,Ying Zhang,Yao Fu
The conversion of levulinic acid (LA) to γ-valerolactone (GVL) is one of the most important reactions from biomass-derived platform chemicals to value-added chemicals. In this work, bimetallic PdRu/TiO2 catalyst compared to monometallic Ru/TiO2 was designed for the conversion of LA to GVL at ambient H2 pressure. The highly dispersed Pd affected the reaction by two antagonistic effects: (I) increasing the reaction rate by promoting the activation of H2; (II) decreasing the reaction rate by lowering the activation ability of carbonyl group over Ru. The kinetic analysis refined by H2 concentration showed much lower apparent activation energy over 0.2Pd1Ru/TiO2 than that over Ru/TiO2. Finally, the catalysts were evaluated by both GVL productivity and catalyst cost to show increasing benefit of Pd addition at lower H2 pressure. This study offers both theoretical foundation and application instructions for high efficiency conversion of LA to GVL under mild conditions, especially ambient H2 pressure.
研究领域:
催化化学
·
生物质能
·
绿色化学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Energy Chemistry
·
2019
·
IF 5.162
Shuqi Fang,Zhibing Cui,Yuting Zhu,Chenguang Wang,Jing Bai,Xinghua Zhang,Ying Xu,Qiying Liu,Lungang Chen,Qi Zhang,Longlong Ma
Herein, we reported in situ synthesis of biomass-derived Ni/C catalyst by self-reduction with pomelo peel. Compared with the conventional method, which includes carbonization , activation, impregnation and reduction, the entire preparation process was simplified to two steps, which was more straightforward. This synthesis method was green as Ni/C can be prepared without any additional chemical and the self-reduction process was realized in N 2 , which can avoid using H 2 thus averting some problems such as storage, transportation and safety of H 2 . Meanwhile, the size and dispersion of Ni particles can be controlled by changing carbonization temperature. The synthesis mechanism of Ni/C catalyst with self-reduction was investigated, which was mainly attributed to the carbon and reducing gas produced during the carbonization process. For the catalytic performance of GVL synthesis, a high yield (94.5%) can be obtained and it exhibited good stability up to 5 cycles without obvious loss of catalytic activity .
研究领域:
催化
·
绿色化学
·
材料科学
·
生物质转化
✓ 已验证
产品关联
DOI
高影响因子
Molecular Catalysis
·
2022
·
IF 5.089
Fukun Li,Ronghe Yang,Ziting Du,Jinhang Dai,Xingmin Wang,Ning Li,Jie Zhang,Xianming Zhang,Yunqi Liu,Haifeng Gong,Hong Yin,Zhenping Cai
γ-Valerolactone (GVL) is considered as a versatile platform chemical obtained from biomass refinery. In this study, eco-friendly group III metal (Sc, Y, La) triflates were examined as homogeneous catalysts for microwave-assisted transfer hydrogenation of ethyl levulinate (EL) to GVL under mild conditions. Experimental results revealed that the selectivity of GVL has a positive relationship with the Lewis acidity of metal ion, which is related to effective charge density of the metal center (3.23, 2.81, 2.60 for Sc 3+ , Y 3+ , La 3+ , respectively). The stronger Lewis acidity of metal ion, the higher catalytic activity of MPV reduction. Among these catalysts, Sc(OTf) 3 exhibited the best catalytic activity, achieving 98.4% EL conversion and 92.4% GVL yield at 140 °C in 3.0 h. Furthermore, Sc(OTf) 3 showed high stability and recyclability for at least ten reaction cycles. In addition, a plausible reaction pathway and mechanism were proposed.
研究领域:
化学工程
·
催化
·
可再生能源
·
绿色化学
✓ 已验证
产品关联
DOI
高影响因子
Materials Today Sustainability
·
2023
·
IF 7.8
B. Putrakumar,Prem Kumar Seelam,G.S. Rao,N. Pethan Rajan,P. Bhanuchander,G. Raveendra,P. Vijayanand,U. Lassi,E.M. Bakhsh,S.B. Khan,S. Kim
This research work introduces highly dispersed Cu nanoparticles encapsulated into a nanoporous carbon (Cu@C) structure as an efficient catalytic system in selective hydrogenation of γ-valerolactone (GVL) to 1,4-pentanediol. The nanoporous carbon support and the catalysts were synthesized by sequential novel methods and characterized extensively by using a combination of different analytical techniques to determine the phase, textural, morphology, nanoparticles size, and distribution analysis, and redox behavior. The designed Cu@C embedded catalysts show moderately high activity in GVL hydrogenation with different Cu loadings. The effect of copper loadings was found to be a significant parameter in gaining the best performance in GVL conversion. The copper nanoparticles were uniformly distributed over the nano-scaled carbon structure with active metallic Cu(111) sites with high dispersion and promote GVL hydrogenation, efficiently. Over a 5Cu@C catalyst exhibited the highest GVL conversion (∼91%) and 1,4-pentanediol selectivity (∼97%) at 200 °C for a 5 h reaction time under a 5 MPa H 2 pressure. The dispersion of the active copper phase in combination with a smaller particle size and surface acidity is directly correlated with the catalytic performance activity. The effects of reaction parameters such as the reaction time, temperature, and H 2 pressure were systematically investigated. Overall, Cu@C is a promising non-noble metal-based catalytic system for the upgradation of biomass-based platform molecules via selective hydrogenation.
研究领域:
催化化学
·
生物质转化
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2023
·Vol. 47
·期 21
·10455-10462
·
IF 3.3
Mengting Chen,Qifeng Zhong,Jiao Ma,Zhiyang Zhang,Yingxin Liu,Zuojun Wei,Shuguang Deng
Hydrogenation of levulinic acid (LA) to γ-valerolactone (GVL) is a key reaction in the conversion of biomass to renewable fuels and value-added chemicals. Developing low-cost, highly efficient and reusable non-noble metal-based heterogeneous catalysts is vital but challenging. Herein, non-noble Ni–Mn/SiO2 catalysts with a low Ni loading (2.0 wt%) were designed for the selective hydrogenation of LA to GVL. The results showed that the optimal Ni–Mn/SiO2 (Ni/Mn = 2) catalyst with well-dispersed and small-sized metal nanoparticles (2.21 nm) and moderate acid sites exhibited excellent activity and selectivity and achieved a 100% yield of GVL in a 1,4-dioxane solvent under mild reaction conditions (e.g., 0.8 mol% Ni, 140 °C and 2.0 MPa H2) for 5.5 h and a 100% GVL yield at 180 °C for 2 h with a turnover frequency (TOF) of 190.2 h−1, which is better than most non-noble metal catalysts reported. Furthermore, the catalyst exhibited excellent reusability and could be recycled at least five times with only slight activity loss. This work provides new insights for the rational design of highly efficient and stable non-noble metal catalysts for the conversion of LA to GVL.
研究领域:
催化化学
·
可再生能源
·
绿色化学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS A-GENERAL
·
2025
·
IF 4.8
Weimeng Cai,Haojie Du,Erju Wang,Yuting Qiang,Kunhong Hu,Jianhua Guo
The synthesis of value-added chemicals from renewable biomass is becoming increasingly important in the transition to a sustainable and low-carbon energy system. Herein, we demonstrate a solvent-polarity modulation strategy to engineer biomass-derived Cu-MOF using 2,5-furandicarboxylic acid (FDCA) as a renewable ligand, where tailored β/α ratios via Kamlet-Taft parameters balance nucleation-growth kinetics to optimize textural properties. Pyrolyzed Cu-MOF at 500 °C under a nitrogen atmosphere yield the Cu/C catalysts, which were subsequently employed in the selective hydrogenation of levulinic acid (LA) to γ-valerolactone (GVL). Among the various solvents used, the Cu-MOF precursor synthesized in a mixed solvent of methanol and N, N-dimethylformamide (DMF) demonstrated the highest catalytic performance, outperforming those synthesized in other solvents. This highlights the significant impact of solvent selection on the structure of Cu-MOF, which in turn affects their hydrogenation activity. Advanced characterization confirming that the uniform Cu dispersion (confirmed by HRTEM mapping) and Cu⁰/Cu⁺ electronic synergy (via Cu Auger analysis) enhanced hydrogenation performance. Additionally, the biomass-derived catalysts exhibited excellent durability. Overall, this research provides a promising approach to develop highly efficient catalysts using renewable ligands and demonstrates the potential of regulating catalyst properties through the strategic selection of solvents, as informed by Kamlet-Taft parameters.
研究领域:
催化化学
·
绿色化学
·
材料科学
·
可再生能源
·
化学合成
✓ 已验证
产品关联
DOI
高影响因子
NANOTECHNOLOGY
·
2018
·Vol. 29
·期 7
·075708
·
IF 3.404
Hengcong Tao,Jingjing Ding,Chao Xie,Yunnan Gao,Jinliang Song,Zhenyu Sun
We demonstrate a facile and versatile method to grow Ru particles uniformly on pristine few-layer graphene (FLG) in supercritical diethylamine. In particular, a large number of Ru subnanometer clusters less than 1.0 nm were observed. The particle size can be tuned by manipulating the loading content of Ru and controlling the reaction temperature. The resulting Ru/FLG showed remarkably high activity, selectivity, and reusability towards the hydrogenation of levulinic acid to γ-valerolactone. This method is flexible, and can be extended to the synthesis of a variety of other ultrafine metal particles supported on FLG.
研究领域:
材料科学
·
催化化学
·
绿色化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子