Catalysts
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2025
·Vol. 15
·期 5
·416
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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
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生物质转化
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绿色化学
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产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2021
·
IF 19.503
Yaowei Lu,Yongxing Wang,Qinghu Tang,Qiue Cao,Wenhao Fang
The synergistic effect in a bimetallic oxide usually plays a vital role in determining the behavior of supported-metal catalysts. We show the unique synergy in a Sn x Mn 1 O y oxide, which can boost the hydrogenation catalysis of supported Pt nanoparticles for selective conversion of levulinic acid (LA) to γ-valerolactone (GVL). On a series of Pt/Sn x Mn 1 O y catalysts with a similar Pt loading ( ca. 0.44 wt%) and a controlled Pt size ( ca. 2.7 nm), the intrinsic TOF presents a volcano-like dependence on Pt 0 sites and Lewis acidity, which is determined by the variable synergistic effect between MnO y and SnO y . The optimal Pt/Sn 0.8 Mn 1 O y catalyst exhibits a high i TOF of 2709 h −1 and achieves 100% selectivity to GVL at 99% conversion of LA at 120 ℃ and 2 MPa of H 2 . DFT calculations demonstrate that the incorporation of Sn can provide a lower energy barrier for the crucial elementary reactions.
研究领域:
化学工程
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催化科学
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产品关联
DOI
高影响因子
ChemSusChem
·
2023
·Vol. 16
·期 21
·e202300754
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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.
研究领域:
催化化学
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绿色化学
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材料科学
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF CHEMICAL THERMODYNAMICS
·
2016
·
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.
研究领域:
化学工程
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物理化学
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产品关联
DOI
高影响因子
CHINESE JOURNAL OF CATALYSIS
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2018
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IF 3.525
Haojie Wang,Chun Chen,Haimin Zhang,Guozhong Wang,Huijun Zhao
Bimetallic nanostructures have attracted great interest as efficient catalyst to enhance activity, selectivity and stability in catalytical conversion. Herein, we report a facile one-pot carbothermal route to in-situ controllable synthesize heterogeneous bimetallic Ni 3 Fe NPs@C nanocatalyst. The X-ray diffraction, transmission electron microscopy, X-ray photoelectron spectroscopy and N 2 adsorption-description results reveal that the Ni 3 Fe alloy nanoparticles are evenly embedded in carbon matrix. The as-prepared Ni 3 Fe NPs@C catalyst shows excellent selective hydrogenation catalytic performance toward the conversion of levulinic acid (LA) to γ-valerolactone (GVL) via both direct hydrogenation (DH) and transfer hydrogenation (TH). In DH of LA, the bimetallic catalyst achieved a 93.8% LA conversion efficiency with a 95.5% GVL selectivity and 38.2 mmol g −1 h −1 GVL productivity (under 130 °C, 2MPa H 2 within 2 h), which are 6 and 40 times in comparison with monometallic Ni NPs@C and Fe NPs@C catalysts, respectively. In addition, the identical catalyst displayed a full conversion of LA with almost 100% GVL selectivity and 167.1 mmol g −1 h −1 GVL productivity at 180 °C within 0.5 h in TH of LA. Under optimal reaction conditions, the DH and TH catalytic performance of 500-Ni 3 Fe NPs@C(3:1) catalyst for converting LA to GVL is comparable to the state-of-the-art noble-based catalysts. The demonstrated capability of bimetallic catalyst design approach to introduce dual-catalytic functionality for DH and TH reactions could be adoptable for other catalysis processes.
研究领域:
催化化学
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材料科学
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能源化学
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产品关联
DOI
高影响因子
GREEN CHEMISTRY
·
2019
·Vol. 21
·期 16
·4499-4511
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IF 9.405
Yuewen Shao,Kai Sun,Qingyin Li,Qianhe Liu,Shu Zhang,Qing Liu,Guangzhi Hu,Xun Hu
γ-Valerolactone (GVL) and 1,4-pentanediol (1,4-PDO) are value-added chemicals that can be produced from levulinic acid/ester via hydrogenation coupled with acid/base-catalyzed reactions. In this study, we demonstrate that the Cu-based catalysts produced via the hydrotalcite precursors with tunable distribution of acidic and basic sites could, according to the requirement of the target products, effectively tune the production of GVL or to 1,4-PDO from levulinic acid/ester. The abundant Brønsted acid sites over the CuAl catalyst suppressed the opening of the ring of GVL, achieving a higher GVL selectivity while inhibiting 1,4-PDO formation. The introduction of Mg species to the catalyst significantly increased the abundance of the basic sites on the surface of the catalyst, which was essential for the selective conversion of GVL to 1,4-PDO via the opening of the ring structure of GVL, the rate-determining step in the conversion from levulinic acid/ester to 1,4-PDO. In addition, the CuMgAl catalyst showed a much superior catalytic stability to the CuMg or CuAl catalyst due to the more stable crystal structure, the more developed porous structure, the higher dispersion of the Cu species and the higher capability to suppress the growth of metallic Cu species under hydrothermal conditions.
研究领域:
化学工程
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催化科学
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产品关联
DOI
高影响因子
Crystals
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2020
·Vol. 10
·期 6
·530
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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
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催化化学
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DOI
高影响因子
CATALYSIS LETTERS
·
2020
·Vol. 150
·期 12
·3553-3560
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IF 2.482
Tian Yi,Zhang Ruoqi,Zhao Wenguang,Wen Sha,Xiang Yanping,Liu Xianxiang
Abstract Alkyl levulinates are important biobased chemicals with great fuel-blending properties and good reactivity. In this work, a new functionalized nitrogen-containing organic polymer bearing sulfonic acid groups (PDVTA-SO 3 H) was successfully prepared and studied for the esterification of levulinic acid with alcohols to produce alkyl levulinates. The results showed that this sulfonic acid-functionalized organic polymer possessed high catalytic activity, and the yield of n -butyl levulinate reached 97.4% under the mild conditions. PDVTA-SO 3 H exhibited strong acidic sites and high stability, and would be well expected to be a potential candidate better than some commercial sulfonic solid catalysts for alkyl levulinates production. The catalyst had been reused without any treatment for five times and the results proved its potential for industrial applications. Graphic Abstract
A new sulfonic acid-functionalized organic polymer showed high activity in the conversion of biomass derived levulinic acid into alkyl levulinates.
研究领域:
化学工程
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生物质能
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催化化学
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产品关联
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
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催化材料
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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.
研究领域:
生物化学
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可再生资源工程
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DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2025
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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.
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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
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DOI
高影响因子
危险品化学品经营许可证（带存储）