ChemCatChem
·
2022
·Vol. 14
·期 13
·e202200311
·
IF 5.497
Yuyao Zeng,Bowei Wang,Fanyong Yan,Wensheng Xu,Guoyi Bai,Yang Li,Xilong Yan,Ligong Chen
Graphical Through a convenient impregnation method, highly-distributed and stable Cu nanoparticles were dispersed on the boron doped γ-Al 2 O 3 support, which catalyzed continuous reductive amination of levulinic acid to corresponding N-substituted pyrrolidinones. The reductive amination of biomass-derived levulinic acid (LA) to value-added N-substituted pyrrolidinones with amine and molecular hydrogen over heterogeneous catalyst represents an atom-economical and scalable route. In this paper, a series of boron doped Cu/Al 2 O 3 catalysts via kneading and impregnation method are developed for the continuous reductive amination of LA. Compared with Cu/Al 2 O 3 , Cu 10 /AlB 3 O catalyst exhibits greatly improved catalytic performance for this reaction at low operation temperature. Structure-property correlation investigations were performed with diverse characterization methods, and the results revealed that the excellent catalytic performance of boron doped Cu/Al 2 O 3 catalysts was mainly attributed to the synergistic effect of its well-dispersed Cu nanoparticles, appropriate surface Cu electronic state and surface acidic sites nearby. Besides, Cu 10 /AlB 3 O shows great stability during the reaction over 200 h. This work provides a low-cost, efficient and environmentally friendly heterogeneous catalytic system for the continuous production of N-substituted pyrrolidinones.
研究领域:
催化化学
·
绿色化学
·
生物质转化
✓ 已验证
DOI
高影响因子
Catalysts
·
2025
·Vol. 15
·期 5
·416
·
IF 4
Jie Qin,Guohong Chen,Kaiqi Zheng,Jiajun Wu,Fanan Wang,Xueping Liu,Rengui Weng
2-Methyltetrahydrofuran (2-MTHF), a hydrogenated derivative of levulinic acid (LA), is a biomass-derived platform compound with diverse and significant applications as a biofuel, gasoline additive, green solvent, and pharmaceutical synthesis intermediate. This study investigates the preparation of a Cu1Ni2/Al2O3catalyst through the calcination–reduction of CuNiAl hydrotalcite as a precursor, which was subsequently utilized in the hydrogenation of LA to produce 2-MTHF. The calcination–reduction process applied to CuNiAl hydrotalcite results in a lattice confinement effect. This method not only disperses the active metal sites but also alters the bonding patterns of the active metals, thereby enhancing the activity and stability of the Cu1Ni2/Al2O3catalyst. The results indicate that complete conversion of LA and a 2-MTHF yield of 87.6% can be achieved under optimal conditions of 190 °C, 5 MPa hydrogen, and a reaction time of 5 h, demonstrating an efficient one-step conversion process. Additionally, the catalyst’s recyclability was assessed through multiple reuse tests, with a loss of activity of only 9.2% after six cycle experiments, suggesting its feasibility and reliability for industrial applications.
研究领域:
催化化学
·
生物质转化
·
绿色化学
✓ 已验证
产品关联
DOI
高影响因子
Crystals
·
2020
·Vol. 10
·期 6
·530
·
IF 2.404
Chaoqun Bian,Xiao Wang,Lan Yu,Fen Zhang,Jie Zhang,Zhengxin Fei,Jianping Qiu,Longfeng Zhu
The incorporation of metal heteroatoms into zeolites is an effective modification strategy for enhancing their catalytic performance. Herein, for the first time we report a generalized methodology for inserting metal heteroatoms (such as Sn, Fe, Zn, and Co) into the layered zeolite precursor RUB-36 via interlayer expansion by using the corresponding metal acetylacetate salt. Through this generalized methodology, Sn-JHP-1, Fe-JHP-1, Zn-JHP-1 and Co-JHP-1 zeolites could be successfully prepared by the reaction of RUB-36 and corresponding metal acetylacetate salt at 180 °C for 24 h in the presence of HCl solution. As a typical example, Sn-JHP-1 and calcined Sn-JHP-1 (Sn-JHP-2) zeolite is well characterized by the X-ray diffraction (XRD), diffuse reflectance ultraviolet-visible (UV-Vis), inductively coupled plasma (ICP), N2sorption, temperature-programmed-desorption of ammonia (NH3-TPD) and X-ray photoelectron spectroscopy (XPS) techniques, which confirm the expansion of adjacent interlayers and thus the incorporation of isolated Sn sites within the zeolite structure. Notably, the obtained Sn-JHP-2 zeolite sample shows enhanced catalytic performance in the conversion of glucose to levulinic acid (LA) reaction.
研究领域:
材料科学
·
催化化学
✓ 已验证
DOI
高影响因子
MOLECULES
·
2024
·Vol. 30
·期 1
·93
·
IF 4.2
Jingru Wang,Xianshu Dong,Yuping Fan,Yingyong Wang,Xiangyun Guo
Hydrogenation of levulinic acid (LA) represents a significant approach for producing the high-value biomass-based platform compound γ-valerolactone (GVL). In this study, an efficient RuIr alloy bimetallic catalyst supported on SiC was synthesized and applied for the aqueous hydrogenation of LA into GVL under mild conditions. The RuIr/SiC catalyst exhibited high LA conversion and GVL selectivity (both > 99%) in water at 0.2 MPa H2pressure and 25 °C. The excellent performance is attributed to the synergistic interaction between Ru and Ir nanoparticles on the semiconducting SiC support. Furthermore, the catalytic activity of the RuIr/SiC alloy remained basically unchanged after five cycles, confirming the high stability of the bimetallic alloy catalyst.
研究领域:
化学工程
·
催化材料
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Sugar Tech
·
2020
·Vol. 22
·期 5
·830-841
·
IF 1.198
Chen Shuai,Zheng Wenjing,Liu Weixi,Liu Lei,Sun Weidong
Levulinic acid (LA) is an important biomass-based chemical. The preparation of LA from bagasse is of great practical significance for the comprehensive and efficient utilization of biomass. Biomass bagasse is mainly composed of cellulose, hemicellulose, and lignin. The cellulose is mainly degraded to glucose, and hemicellulose is mainly degraded to xylose, with dilute acid treatment at high temperature. In this research, we produced the LA from bagasse with dilute acid treatment at high temperature. The influences of residence time (10–60 min), reaction temperature (170–240 °C), liquid-to-solid ratio (5:1–25:1 mL/g), and acid concentration (1–5%) on the synthesis of LA were investigated by statistical methods, achieving a maximum LA yield of 16.25%. Additionally, LA was isolated and extracted from bagasses hydrolysate by ion exchange and vacuum distillation. The adsorption capacity of different resins was determined and compared. The optimal resin to acquire better adsorption capacity was determined. The better adsorption capacity was obtained when the D301 resin was selected as the filter for ion exchange. The height-to-diameter rate, eluent flow rate, elution volume of ion exchange column were 10, 0.84 BV/h, 56.4 mL, respectively. The eluent was then distilled under vacuum, collecting the components at 130–140 °C. The total yield and purity of LA were 67.1% and 78%, respectively.
✓ 已验证
DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2025
·
IF 7.2
Xi Cheng,Qingge Feng,Dachao Ma,Yuan Qi,Lin Feng,Fanghong Qin,Xiaodie Cheng,Xu Zeng
A novel organosolv pretreatment method using solid acid CH₃-SBA-15-SO₃H as a catalyst was developed to overcome the challenges posed by lignin and hemicellulose in rice husk to cellulose conversion, thereby improving the yield of levulinic acid. Through systematic optimization of pretreatment conditions, complete removal of lignin and substantial reduction of hemicellulose from rice husk were achieved within only 40 min at 150 °C, with a minimal cellulose loss of merely 4.8 %. In the γ-valerolactone/water co-solvent system, the presence of both hemicellulose and lignin was found to reduce the yield of levulinic acid. By adopting a two-step process with rice husk as the feedstock, the yield of levulinic acid was significantly increased by 1.77 times. These findings deepen our understanding of biomass conversion and highlight the promising application prospects of solid acid catalysis in sustainable chemical synthesis.
✓ 已验证
产品关联
DOI
高影响因子
PROCESS BIOCHEMISTRY
·
2019
·
IF 2.883
Xiaohui Di,Yu Zhang,Junying Fu,Qiang Yu,Zhongming Wang,Zhenhong Yuan
High value-added utilization of biomass-based platform chemicals has attracted increasing attention in recent years. The present study addresses the upgrading of levulinic acid (LA), an important biomass-based platform chemical, to methyl levulinate via a green and efficient enzymatic approach. Various lipases were assessed, with Novozym ® 435 displaying the best results for the esterification of LA. Subsequently, the effect of reaction medium on Novozym ® 435 catalyzed esterification was also studied. Compared with other reaction media, 1-butyl-3-methylimidazolium hexafluorophosphate ([bmim][PF 6 ]) showed the greatest enhancement in yield by suppressing hydrolysis activity. The catalysts reusability was also improved by protection from [bmim][PF 6 ] with 43.2% activity remained after 5 cycles, compared to that of 19.1% in 2-Me THF. Reaction temperature exerted an unusual double-peak relationship over methyl levulinate yield because Novozym ® 435 can simultaneously catalyze the esterification of LA and hydrolysis of methyl levulinate, each of which has a different optimal reaction temperature: ca. 30 °C and ca. 40 °C, respectively. When the molar ratio of LA/methanol, and the volume ratio of methanol/[bmim][PF 6 ] were 1:5 and 1:3, respectively, methyl levulinate was obtained in 93% yield at 30 °C after 24 h with 10 mg/mL catalytic loading.
研究领域:
生物化学
·
绿色化学
✓ 已验证
DOI
高影响因子
Polymers
·
2025
·Vol. 17
·期 7
·857
·
IF 4.9
Bolun Li,Mengyan Wang,Huixiang Luo,Kaina Li,Yanlong Jia,Mingjie Fu,Chenyu Jiang,Shuangquan Yao,Yongjun Yin
As a carbon-neutral and renewable raw material, cellulose can be transformed into biomass fuels to reduce the dependence on fossil fuels and carbon dioxide emissions. In view of harsh reaction conditions, low selectivity of product, and easy deactivation of the catalyst, this study studied the use of photothermal catalytic technology to convert cellulose into bio-oil rich in levulinic acid. It was discovered that a synergistic effect between heating and photocatalysis is present in cellulose degradation. Different metals were loaded on carbon nanotubes doped with titanium dioxide to prepare different photothermal catalysts, and their catalytic effects on cellulose were compared. It was found that TiO2-CNT loaded with platinum metal exhibited the highest catalytic performance. By adopting Pt/TiO2-CNT as the catalyst, the conversion rate of bio-oil reached 99.44%, and the selectivity of LA reached 44.41% at 220 °C for 3 h. As the photothermal catalysis increased the H/C ratio and decreased the O/C ratio of the liquid product, the calorific value reached 21.01 MJ/kg. This study can promote the further industrial application of lignocellulose to prepare fuel oil and decrease the environmental pollution caused by the massive consumption of fossil fuels.
研究领域:
能源科学
·
催化化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
BIORESOURCE TECHNOLOGY
·
2015
·
IF 4.494
Yue Shen,Jian-Kui Sun,Yu-Xuan Yi,Bo Wang,Feng Xu,Run-Cang Sun
A simple and effective route for the production of levulinic acid (LA) from cellulose has been developed in SO 3 H-functionalized ionic liquids. The effects of ionic liquid structures, reaction conditions and combination of metal chlorides with ILs on the yield of LA were investigated, where the highest yield of 39.4% was obtained for 120 min in the presence of 1-(4-sulfonic acid) butyl-3-methylimidazolium hydrogen sulphate ([BSMim]HSO 4 ) with addition of H 2 O. The catalytic activities of ionic liquids depended on the anions and decreased in the order: CF 3 SO 3 − > HSO 4 − > OAc − , which was in good agreement with their acidity order. The ILs play a dual solvent-acid role for the cellulose conversion into LA and exhibited favorable catalytic activity over four repeated runs.
研究领域:
化学工程
·
可再生能源
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ChemSusChem
·
2011
·Vol. 4
·期 11
·1578-1581
·
IF 6.325
Yao-Bing Huang,Jian-Jun Dai,Xiao-Jian Deng,Yan-Chao Qu,Qing-Xiang Guo,Yao Fu
Graphical Combo deal: An aqueous solution of levulinic acid (LA) and formic acid (FA) derived from biomass-based carbohydrates can be converted efficiently to pyrrolidines via a ruthenium catalyst without need for an energy-intensive separation of LA or an external H 2 source. The ruthenium catalyst combines two processes: decomposition of FA to H 2 and reductive amination of LA with an amine.
研究领域:
化学工程
·
催化
·
绿色化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
FUEL
·
2023
·
IF 7.4
Yunfei Zhang,Xilun Wang,Yi Shen
The challenge in the electrochemical reduction of levulinic acid (LA) lies in designing highly selective, energy-efficient, and non-precious-metal electrocatalysts that minimize the competitive hydrogen evolution reaction during LA conversion. Herein, we reported a facile pulsed electrodeposition strategy to fabricate bimetallic electrocatalysts with different combinations of lead (Pb), indium (In), tin, and cadmium supported by free-standing carbon felts (CFs). The as-prepared bimetallic self-supporting electrodes were examined for the electrochemical hydrogenation (ECH) of LA. The resulting InPb/CF electrocatalysts showed superior performance among the bimetallic catalysts. In addition, it was demonstrated that the catalytic performance of bimetallic samples was better than that of the corresponding monometallic samples. Notably, the In 72.4 Pb 27.6 /CF exhibited the best performance for ECH of LA, leading to 86.1 % of LA conversion, 99.7 % of selectivity towards valeric acid and 60.8 % of Faradaic efficiency at −1.5 V vs RHE. The excellent performance is mainly attributed to the modification of the electronic structures by the ligand and strain effects. Meanwhile, the relatively high electrochemically active surface area and the low charge transfer resistance are also conducive to improving the catalytic performance.
✓ 已验证
产品关联
DOI
高影响因子
FUEL
·
2018
·
IF 4.908
Wanbing Gong,Chun Chen,Ruoyu Fan,Haimin Zhang,Guozhong Wang,Huijun Zhao
Transfer-hydrogenation (TH) has attracted great attention because it does not require the use of high pressure H 2 . In this work, we report a facile ultrasound-assisted impregnation method with the aid of carbothermal reduction property of activated carbon (AC) to synthesize AC supported copper catalyst (Cu/AC) for efficient TH of bio-derived unsaturated oxygenated compounds such as furfural (FAL) and levulinic acid (LA). In the presence of 2-propanol as the hydrogen donor, within 5 h under 200 °C, the resultant Cu/AC catalyst can convert FAL into 2-methylfuran (2-MF, a high-value fuel additive) with a superior selectivity of 91.6%. The Cu/AC catalyst can also covert LA into γ-valerolactone (GVL) with a high selectivity of 89.9% under 220 °C for 5 h. The superior TH catalytic performance of the Cu/AC catalyst could be attributed to the uniform size and well dispersed Cu nanoparticles supported on the high surface area AC with the suitable proportion of Cu 2+ , Cu 0 and Cu + . Cycling test results confirm the reusability of the Cu/AC catalyst. Additionally, the reported Cu/AC catalyst is cheap and massive producible, advantageous for large-scale conversion of bio-derived platforms to value-added chemicals and bio-fuels.
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）