MICROPOROUS AND MESOPOROUS MATERIALS
·
2026
·
IF 4.5
Yongtai Li,Yuanting Du,Yushan Jia,Ruixi Yang,Weijun Shan,Zhenning Lou,Haibiao Yu,Ying Xiong
Hollow coral-like MCM-41-C was successfully prepared by adjust ethanol dosage. • Hollow coral-like 7wt%Al-MCM-41-C with rich weak acid site was prepared by impregnation. • Butene yield was 92.26% for 7wt%Al-MCM-41-C catalyst (300 °C, 90 min). • Due to hollow coral-like structure, 7wt%Al-MCM-41-C exhibits high catalytic stability. In this paper, the hollow coral-like ordered mesoporous MCM-41-C zeolites were synthesized by hydrothermal method, and their synthesis conditions were thoroughly investigated. Then, x wt%Al-MCM-41-C catalysts feature with hollow coral-like morphology were prepared by impregnation method, and used for the catalytic conversion of γ-valerolactone (GVL) to butene. The results showed that the introduction of Al species not only did not destroy the original special microscopic morphological structure of the MCM-41-C, but also co-existed on the surface and skeleton of the catalyst, resulting in a large number of weak acid sites. The optimal 7wt%Al-MCM-41-C catalyst has a specific surface area of 708.56 m 2 g −1 . The content of weak acid was 0.7262 mmol g −1 . At 300 °C, the GVL conversion and butene yield over the catalyst can reach 99.10% and 92.26%, respectively, within just 90 min of reaction. Meanwhile, the 7 wt%Al-MCM-41-C catalysts also demonstrated excellent catalytic cycle stability, and the butene yield remained above 90% after the 4th cycle. Download: Download high-res image (330KB) Download: Download full-size image
✓ 已验证
产品关联
DOI
高影响因子
RENEWABLE ENERGY
·
2025
·
IF 9.1
Yingfu Tian,Tianliang Lu,Hongjin Qu,Xiaomei Yang,Lipeng Zhou
Efficient conversion of ethyl levulinate (EL) in high concentration to γ-valerolactone (GVL) at moderate temperature via catalytic transfer hydrogenation strategy is highly desirable. In this work, hydrothermally synthesized Sn-β zeolite with high Sn content was employed as a catalyst to realize this aim. Fully crystallized Sn-β zeolite with high Sn content ( n Si / n Sn = 60) was successfully synthesized within 12 days using MgCl 2 as a promoter. The synthesized zeolites were characterized by XRD, SEM, UV-vis spectroscopy, FT-IR spectroscopy and XPS. The L acid density of Mg-Sn-β-60-12d increased to 90 μmol g −1 compared to Mg-Sn-β-100-7d (56 μmol g −1 ). 92% yield of GVL was achieved on Mg-Sn-β-60-12d using high concentration of EL (1.2 mol L –1 ) as reactant at 130 o C for 8 h. The performance of Mg-Sn-β is better than that of Sn-β with same n Si / n Sn . The reaction mechanism over Mg-Sn-β was discussed. In addition, Mg-Sn-β-60-12d showed excellent stability and reusability during five runs.
研究领域:
化学工程
·
催化材料科学
✓ 已验证
产品关联
DOI
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
·
催化科学
·
可再生化学品合成
✓ 已验证
产品关联
DOI
高影响因子
Catalysts
·
2024
·Vol. 14
·期 12
·924
·
IF 3.8
Yu Yue,Guozhi Zhu,Min Liu,Yue Zhu,Weilong Ji,Xiaoqin Si,Tianliang Lu
As an important biomass resource, γ-valerolactone (GVL) shows considerable potential for applications in biofuel production, organic synthesis, polymer, and food industries. Herein, an effective method was presented for synthesizing GVL through the catalytic transfer hydrogenation (CTH) of ethyl levulinate (EL) under mild conditions. Using isopropanol as a hydrogen donor, a 100% conversion of ethyl levulinate and an 88.7% yield of GVL were achieved over 2%Zr-Beta-7d catalyst at 110 °C for 8 h. The acidic sites of synthesized Zr-Beta via hydrothermal methods easily adjusted and offered high catalytic activity and selectivity. The Lewis (L) acid sites on the zeolite serve as the active centers for the conversion of EL. Characterization results indicate that the amounts of L acid sites on Zr-Beta increased with the Zr content and crystallization time rose, thus enhancing the selectivity for GVL. Additionally, the influences of catalyst dosage, reaction temperature, and time on catalytic performance are studied, as well as calculations of kinetic parameters such as reaction rate constants and activation energies. The 2%Zr-Beta-7d catalyst retains its high performance after five cycles. The current research may present an efficient approach for the conversion of EL to GVL under mild conditions.
研究领域:
生物质化学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2021
·
IF 5.909
Xi Cheng,Qingge Feng,Dachao Ma,Hongcheng Chen,Xu Zeng,Feifan Xing,Jiayang Teng
To eco-friendly catalyze glucose to levulinic acid, recyclable acid catalyst has been researched. The synthesis process of propyl sulfonic acid functionalized SBA-15 was improved and the hydrophobic treatment was performed. The structure and functional groups of materials were characterized by X-ray diffraction, transmission electron microscopy , N 2 adsorption–desorption isotherms, elemental analysis, Fourier transform infrared spectroscopy , X-ray photoelectron spectroscopy and simultaneous thermal analysis. The catalytic activity , recyclability and hydrothermal stability of CH 3 -SBA-15-SO 3 H material were researched. The highest yield of levulinic acid at 61.56% was obtained at 180 ℃ for 2.5 h in γ-GVL-water solvent system, and the yield of levulinic acid was only decreased by 2% after 4 times reuse. The high degree of silicon polycondension and hydrophobic surface of CH 3 -SBA-15-SO 3 H were the key to maintain the hydrothermal stability. The CH 3 -SBA-15-SO 3 H solid acid had great potential in development and utilization of biomass resources .
研究领域:
化学工程
·
生物质资源开发
✓ 已验证
产品关联
DOI
高影响因子
Reaction Kinetics Mechanisms and Catalysis
·
2018
·Vol. 125
·期 1
·71-84
·
IF 1.515
Xie Yongdi,Wang Haijun,Liu Xiang,Xia Yongmei
Hydrogenation of levulinic acid and its esters to produce γ-valerolactone (GVL) is an important reaction in the process of biomass valorization. Herein, a series of novel and porous acid–base bifunctional Zirconium tripolyphosphate were successfully synthesized and utilized to catalyze the hydrogenation of ethyl levulinate (EL) to GVL. It was found that Zr-TPPA-3 with a large number of Lewis acid–base sites and a high specific area displayed the highest catalytic activity, a satisfied GVL yield of 93.1% with 99.5% EL conversion was obtained under the optimal reaction conditions. In addition, poisoning experiments revealed that the acid–base sites play a synergistic effect in the hydrogenation of EL to GVL, and finally proposed a plausible reaction mechanism.
研究领域:
化学工程
·
催化科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF THE CHINESE CHEMICAL SOCIETY
·
2018
·Vol. 65
·期 11
·1370-1378
·
IF 0.862
Jianjia Wang,Ruiying Wang,Huimin Zi,Haijun Wang,Yongmei Xia,Xiang Liu
Catalytic transfer hydrogenation (CTH) of ethyl levulinate (EL) to γ-valerolactone (GVL) is an alluring reaction in the field of biomass catalytic conversion, but it normally depends on the consumption of H 2 . In this study, we report a porous Zr-containing inorganic pyrophosphate catalyst (ZrOPP), which was used as a catalyst for CTH of EL to GVL in the presence of isopropanol and characterized using FT-IR, py-FTIR, TGA, XRD, BET, XPS, ICP-AES, SEM, TEM, NH 3 -TPD, and CO 2 -TPD. We achieved a high yield of 94% GVL at 433 K for 11 hr. Furthermore, the ZrOPP has the trait of easy separation and could be reused more than five times without distinct decrease in activity and selectivity. In addition, this catalyst could also be applied to other catalytic hydrogenation reactions, such as those of cyclohexanone, acetophenone, 2-heptanone etc. Its outstanding performance was mainly ascribed to the acid sites from the Zr element and basic sites from phosphate groups interspersing on the surface of the catalyst.
研究领域:
化学工程
·
生物质能转化
·
催化科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
·
2021
·
IF 6.064
Yafei Li,Xiaocheng Lan,Boyang Liu,Tiefeng Wang
A stable and highly efficient supported Cu-Ni catalysts for the conversion of ethyl levulinate (EL) to γ-valerolactone (GVL) was developed. The catalysts were characterized by XRD, TEM, TPD, TPR, and XPS. The support effect of metal oxides (Al 2 O 3 , SiO 2 , ZrO 2 , and TiO 2 ) revealed that Cu-Ni supported on Al 2 O 3 showed the highest activity for EL hydrogenation to ethyl 4-hydroxypentanoate (EHP) and the subsequent intramolecular esterification of EHP to GVL. EHP intramolecular esterification to GVL in the ethanol solution was a reversible reaction with an equilibrium constant of 24 at 453 K. A simplified reaction kinetic network was established. The solvent had a significant influence on the reaction equilibrium and the catalyst stability. Cu-Ni/Al 2 O 3 in n-hexane solvent gave a higher GVL yield than that in ethanol solvent, and showed better recyclability than that in toluene solvent. With optimizing the conditions, Cu-Ni/Al 2 O 3 gave 99.9% conversion and 98% selectivity to GVL with a space–time yield of 1.13 g GVL g cat -1 h −1 in n-hexane solvent with good recyclability.
研究领域:
化学工程
·
催化材料科学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Xiaoyan Yin,Tingting Cai,Chao Liu,Chen Huang,Jia Wang,Jun Hu,Neng Li,Jianchun Jiang,Kui Wang
Efficient depolymerization of lignocellulosic biomass into platform chemicals is of great importance to bring the comprehensive bio-refinery concept into industrial reality. Herein, we reported an environmentally benign pretreatment process for full components utilization of moso bamboo in co-solvent of γ-valerolactone (GVL) and aqueous solution of p -toluenesulfonic acid (TsOH aq). Notably, over 98 wt% of lignin and hemicelluloses could be simultaneously degraded into oligomeric phenols and pentose under the mild condition of 130 °C for 60 min with GVL/TsOH aq volume ratio of 4/1, following with 91.5 wt% of cellulose retained which was then enzymatic hydrolyzed into 773.2 mg/g glucose. All of the obtained platform chemicals could be easily separated and purified, which significantly facilitate the excellent retrieve of the co– solvent. Moreover, the synergistic effect between GVL and TsOH on efficiency and specificity was proposed by control group experiment and verified by molecular dynamics simulation and quantum chemical calculation. This study provides a facile pretreatment and direct conversion strategy for biorefinery process of lignocellulosic biomass in novel GVL/TsOH aq co-solvent.
研究领域:
生物化学
·
可再生能源
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
FUEL
·
2021
·
IF 6.609
Rulu Huang,Yao Liu,Junhua Zhang,Junnan Wei,Lincai Peng,Xing Tang
Both value-added utilization of agricultural waste to prepare catalytic materials and selective conversion of biomass-based carbonyl compounds are hot topics. Herein, sugarcane bagasse ( SB ), a main by-product of cane sugar manufacturing industry, was directly assembled with HfCl 4 and methanesulfonic acid (MSA) via a one-step hydrothermal method for scalable preparation of Hf-containing coordination complex (Hf@ SB -MSA). Characterization results revealed that the coordination between Hf 4+ and phenolic hydroxyl, alcohol hydroxyl, carboxyl groups in SB resulting in the formation of Lewis acid (LA) and Lewis base (LB) sites, while sulfonic group in MSA providing Brønsted acid (BA) sites. The cooperative role of LA, BA and LB in Hf@ SB -MSA delivered prominent catalytic performance for catalytic transfer hydrogenation (CTH) of levulinic acid (LvA) to γ-valerolactone (GVL) with isopropanol as solvent and H-donor at mild reaction conditions (GVL yield was up to 99.1%). Heterogeneity and recycling experiments further revealed the good recyclability of Hf@ SB -MSA, which can be easily separated from the reaction mixture by filtration and repetitively used at least five reaction runs without an obvious loss of activity. More gratifyingly, Hf@ SB -MSA also displayed superior universality for the CTH of various carbonyl compounds to their corresponding alcohols with yields up to 90%.
研究领域:
催化化学
·
生物质能
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2022
·Vol. 46
·期 27
·13047-13053
·
IF 3.925
Feng Xu,Chao Liu,Jia-Xin Li,Cai-Zhen Zhan,Qi-Ning Xun,Wen-Shen Zhang,Wen-Fang Xing,Gang-Gang Chang
γ-Valerolactone (GVL) is an important lignocellulosic platform molecule with huge potential for various industrial and chemical applications, which is usually produced using levulinic acid (LA) or its esters as raw materials. However, a two-step reaction process in which hydrogenation of the carbonyl groups on metal sites and subsequent lactonization catalyzed by acidic sites over multiple catalysts has generally been needed to realize this synthesis. In this work, a hierarchically multifunctional single catalyst of Ru/phosphotungstic acid/hierarchically porous UiO-66 (Ru/HPW/HP-UiO-66), simultaneously integrated with acidic and metal sites, has been fabricated via a simple strategy and successfully applied in the one-pot synthesis of GVL using methyl levulinate (ML) as the raw material. The hierarchically porous and nanosized (∼15 nm) HP-UiO-66 can not only provide sufficient space for the mass transfer of substrates but also favors the loading of bulk HPW molecules, which can effectively mediate the catalytic activities and stability of Ru NPs using the confined pore effect of UiO-66 and the strong interaction between HPW and Ru. When applied in the one-pot synthesis of GVL, the hierarchical Ru/HPW/HP-UiO-66 catalyst showed excellent catalytic activity (>97% yield) and stability (maintained after 7 successive cycles) for GVL. More importantly, the hierarchical catalyst also exhibited an extraordinary performance in the hydrogenation of different unsaturated hydrocarbons in aqueous solution. It is expected that our study offers a novel route to biomass upgrades involving metal/acid bifunctional synergistic catalysts.
研究领域:
催化化学
·
材料科学
·
能源化学
✓ 已验证
DOI
高影响因子
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
危险品化学品经营许可证（带存储）