JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
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2016
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IF 4.179
Jian He,Hu Li,Yanxiu Liu,Wenfeng Zhao,Tingting Yang,Wei Xue,Song Yang
A series of mesoporous acid–base bifunctional Zr/B mixed oxides with different molar ratios were prepared by a sol–gel method, and developed for conversion of ethyl levulinate (EL) to γ -valerolactone (GVL) by using alcohol as hydrogen source. The morphological structures and physico-chemical characteristics of the synthesized materials were identified by various techniques. A high GVL yield of 88.5% was achieved from EL in 2-propanol when Zr 1 B 1 was used. And acid–base sites played a synergic role in synthesizing GVL from EL as evident by poisoning experiments. Furthermore, the catalyst could be reused several times without significant loss of its catalytic activity.
研究领域:
化学工程
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催化材料科学
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产品关联
DOI
高影响因子
RSC Advances
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2016
·Vol. 6
·期 93
·90232-90238
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IF 3.289
Xiao-Fang Liu,Hu Li,Heng Zhang,Hu Pan,Shan Huang,Kai-Li Yang,Song Yang
Catalytic ethanolysis of furfuryl alcohol (FA) to ethyl levulinate (EL) with MIL-101(Cr)–SO3H, prepared by simple one-pot hydrothermal treatment, is presented for the first time. The as-prepared catalyst with high surface area, hydrothermal and chemical stability, good dispersion, and feasible accessibility of –SO3H Brønsted acid sites was found to show superior performance to other sulfonic acid-functionalized solid catalysts. Besides the special textural properties, the obtained good catalytic activity of 79.2% EL yield and 100% FA conversion were also dependent on the density and strength of the Brønsted acid and the reaction parameters. A slight loss of catalytic activity after five consecutive recycles and the hot filtration experiment confirmed the good stability of MIL-101(Cr)–SO3H. Two coexisting reaction paths for the ethanolysis of FA to EL catalyzed by MIL-101(Cr)–SO3H were proposed, wherein 2-ethoxymethylfuran (2-EMF) was observed to be the dominant intermediate.
研究领域:
化学工程
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催化科学
✓ 已验证
产品关联
DOI
高影响因子
Catalysts
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2016
·Vol. 6
·期 9
·143
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IF 2.964
Lincai Peng,Ruili Tao,Yu Wu
Levulinate ester has been identified as a promising renewable fuel additive and platform chemical. Here, the use of a wide range of common metal salts as acid catalysts for catalytic upgrading of biomass-derived furfuryl alcohol to butyl levulinate was explored by conventional heating. Both alkali and alkaline earth metal chlorides did not lead effectively to the conversion of furfuryl alcohol, while several transition metal chlorides (CrCl3, FeCl3, and CuCl2) and AlCl3exhibited catalytic activity for the synthesis of butyl levulinate. For their sulfates (Cr(III), Fe(III), Cu(II), and Al(III)), the catalytic activity was low. The reaction performance was correlated with the Brønsted acidity of the reaction system derived from the hydrolysis/alcoholysis of cations, but was more dependent on the Lewis acidity from the metal salts. Among these investigated metal salts, CuCl2was found to be uniquely effective, leading to the conversion of furfuryl alcohol to butyl levulinate with an optimized yield of 95%. Moreover, CuCl2could be recovered efficiently from the resulting reaction mixture and remained with almost unchanged catalytic activity in multiple recycling runs.Keywords:biofuel;furfuryl alcohol;catalytic upgrading;metal salt;levulinate ester
研究领域:
化学工程
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可再生能源
✓ 已验证
产品关联
DOI
高影响因子
Journal of Energy Chemistry
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2016
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IF 2.322
Ran An,Guizhuan Xu,Chun Chang,Jing Bai,Shuqi Fang
Butyl levulinate (BL) is a promising new candidate as diesel fuel and fuel additive. In this study, an efficient process for a one-pot synthesis of BL from biomass-derived carbohydrates in butanol medium with the catalysis of metal sulfates was developed. The catalytic activity of a series of metal sulfates for the synthesis of BL from fructose was investigated. Among various metal sulfates, ferric sulfate Fe 2 (SO 4 ) 3 was found to be the most efficient catalyst, which gave a remarkably high BL yield of 62.8 mol% under the conditions of 463 K, 3 h, a catalyst dosage of 5.0 g/L, and fructose concentration of 25 g/L. Different carbohydrates including glucose, cellulose , inulin and sucrose were also used for one-pot synthesis of BL with the catalysis of Fe 2 (SO 4 ) 3 , showing the yields of 39.6, 30.5, 56.6 and 50.1 mol%, respectively. In addition, the recycling and reuse of Fe 2 (SO 4 ) 3 was studied by characterizing them using powder X-ray diffraction (XRD), scanning electron microscope (SEM), X-ray photoelectron spectroscopy (XPS). A plausible reaction pathway for the one-pot synthesis of BL from fructose was proposed. This study provides a facile and feasible way for the synthesis of BL from biomass.
研究领域:
生物化学
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能源科学
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产品关联
DOI
高影响因子
Molecular Catalysis
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2017
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IF 0
Yongdi Xie,Fan Li,Jianjia Wang,Ruiying Wang,Haijun Wang,Xiang Liu,Yongmei Xia
The synthesis of γ-valerolactone (GVL) from catalytic transfer hydrogenation (CTH) of levulinic acid (LA) and its esters is attracting more and more attention due to its wide application in additive, solvent, and precursor. Herein, a novel Zirconium trimetaphosphate (Zr-TMPA) was successfully synthesized and characterized by Fourier transform infrared, N 2 adsorption-desorption, powder X-ray diffraction, scanning electron microscopy, transmission electron microscopy, and NH 3 /CO 2 -TPD. The as-synthesized Zr-TMPA was used to catalyze the CTH reaction of EL to GVL using isopropanol as the hydrogen donor and solvent. Experimental results shown that Zr-TMPA could catalyze the CTH reaction and 96.2% GVL yield could be achieved at 160 °C for 8 h. Key to this success was attributed to the acid sites and basic sites of the prepared catalyst (Zr-TMPA). Finally, a possible reaction mechanism was proposed.
研究领域:
化学工程
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催化材料科学
✓ 已验证
产品关联
DOI
Nanomaterials
·
2022
·Vol. 12
·期 21
·3870
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IF 5.719
Shuolin Zhou,Lu Wu,Junzhuo Bai,Min Lei,Min Long,Keying Huang
Levulinic esters, synthesized by the esterification of biomass-derived levulinic acid with various alcohols, is an important chemical that plays an essential role in the fields of biomass fuel additives, organic synthesis, and high value-added products. In the present work, the catalytic esterification of levulinic acid with n-butyl alcohol was selected as a typical model reaction to investigate the catalytic performance of an inexpensive commercial catalyst, titanium oxide nanoparticles. The influences of reaction time, reaction temperature, and catalyst loading on the conversion of levulinic acid to n-butyl levulinate were systematically examined through single-factor experiments. Additionally, the optimization of the reaction conditions was further investigated by a Box–Behnken design in response to the surface methodology. The desired product, n-butyl levulinate, with a good yield (77.6%) was achieved under the optimal conditions (reaction time of 8 h, reaction temperature of 120 °C, and catalyst dosage of 8.6 wt.%) when using titanium oxide nanoparticles as catalysts. Furthermore, it was found that addition of water to the catalytic system facilitated the reaction process, to some extent. This study reveals that the nanosized TiO2material,as an efficient solid acid catalyst, had good catalytic performance and stability for the esterification of levulinic acid after six consecutive uses.Keywords:TiO2nanoparticles;solid acid catalyst;n-butyl levulinate;esterification;response surface methodology
研究领域:
化学工程
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催化科学
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生物燃料合成
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产品关联
DOI
PubMed
高影响因子
CHEMICAL PAPERS
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2022
·Vol. 76
·期 12
·7535-7544
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IF 2.146
Hu Aiyun,Wang Haijun,Ding Jian
In this study, a functionalized, heterogeneous, and insoluble acid catalyst of yeast-sulfonic acid was prepared by simple steps using spent yeast and sulfonic acid as raw materials. Its unique internal microstructure and abundant sulfonic acid groups on the surface endow it with the properties of Brønsted acid and high-performance activity. The catalyst was characterized by Fourier transform infrared spectroscopy, powder X-ray diffraction, scanning electron microscopy, transmission electron microscopy, Barrett–Emmett–Teller N 2 adsorption–desorption analysis, X-ray photoelectron spectroscopy, and thermogravimetric analysis. The catalyzed synthesis of ethyl levulinate (EL) from furfuryl alcohol (FA) was carried out at a temperature of 120 °C for 2 h. The conversion rate and yield percentages for the catalyzed reaction of FA to produce EL were 98.2 and 94.7%, respectively. The results show that the amount of catalyst used and reaction conditions significantly impacted the EL yield and FA conversion rate. Overall, the possible reaction mechanism for the conversion of FA to EL was proposed. It was found that the main reason for the high catalytic activity of the catalyst was the effect of Brønsted acid sites.
研究领域:
催化
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化学工程
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有机化学
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可持续化学
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产品关联
DOI
高影响因子
BIOMASS & BIOENERGY
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2023
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IF 6
Xiaoqi Lin,Kaisen Jiang,Xuebin Liu,Hongyan Bi,Tianya Li,Dezhi Han,Qinqin Zhang
The chemical transformation of lignocellulosic biomass into platform chemicals is one of the most efficient utilization methods for agricultural wastes . In this work, a one-pot strategy for the conversion of corn stalk to ethyl levulinate and further extraction of valorizable lignin catalyzed by ILs was proposed. With the optimized catalyst of [C 3 H 6 SO 3 Hmim]HSO 4 , corn stalk of 92.45% was transformed into ethyl levulinate with a favorable yield of 24.72% at 200 °C for 90 min. Furthermore, the lignin extraction was substantially influenced by co-solution system. A high lignin yield of 79.94% was achieved with ethanol content of 75% (v/v) in the ethanol-water system. The analysis on morphology, thermal stability and functional group showed that condensation of lignin occurred during the liquefaction process, the two-dimensional heteronuclear single quantum correlation (2D-HSQC) investigation demonstrated that the stable structure of lignin provides a favorable foundation for its valorization. Overall, this work proposed a feasible biorefinery strategy for effective conversion and utilization of lignocellulosic biomass.
研究领域:
生物化学
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可再生资源利用
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING SCIENCE
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2024
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IF 4.1
Ying Gao,Yong Liu,Lingling Gao,Jinxing Long
An effective strategy is proposed here for transfer hydrogenation of alkyl levulinate to γ-valerolactone (GVL) using a UiO-66 framework modified with phosphotungstate ionic liquid (UiO-66@IL(HPW)). Due to the intensive influence of ionic liquid fragment, the modification significantly enhances the catalytic activity of UiO-66@IL(HPW), leading to a complete conversion of ethyl levulinate with over 93.1% selectivity for GVL. Characterizations techniques, including XRD, N 2 absorption/desorption, SEM, FT-IR, pyridine FT-IR, NH 3 -TPD and CO 2 -TPD, confirm that while the basic structure of UiO-66-NH 2 is insignificantly changed, the introduction of the ionic liquid greatly improves the acidic/base properties of the catalyst. XAFS and XPS results reveal an intensive interaction between the N and W species in UiO-66@IL(HPW), and the formed W-N/O moiety is responsible for the enhanced catalytic activity. In addition, a plausible catalytic mechanism is proposed based upon in situ DRIFTS and density functional theory (DFT) calculations, highlighting the crucial role of ionic liquid fraction within the UiO-66 ligand. Therefore, this work would contribute to the valorization of biochemicals.
研究领域:
化学工程
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材料科学
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产品关联
DOI
高影响因子
APPLIED CATALYSIS A-GENERAL
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2015
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IF 3.942
Jian He,Hu Li,Ye-Min Lu,Yan-Xiu Liu,Zhi-Bing Wu,De-Yu Hu,Song Yang
A series of Al–Zr mixed oxides with different molar ratios were prepared by co-precipitation method and utilized to catalyze conversion of ethyl levulinate (EL) to γ -valerolactone (GVL). Those as-prepared catalysts were characterized by XRD, SEM, N 2 adsorption–desorption, XPS, TG, NH 3 -TPD, CO 2 -TPD and pyridine-IR. The introduction of Al into ZrO 2 was demonstrated to enlarge surface areas, as well as increase the number of acid and base sites that were catalytically active for transfer hydrogenation. Effects of Al–Zr molar ratio, calcination temperature, reaction temperature and time, catalyst dosage, and alcohols used as hydrogen donors on the catalytic performance were investigated. A high GVL yield of 83.2% at EL conversion of 95.5% could be achieved at 220 °C in 4 h over Al 7 Zr 3 -300 using 2-propanol as hydrogen donor and solvent. Poisoning experiments verified that acid–base sites played a synergic role in producing GVL from EL. Moreover, the Al–Zr mixed oxide catalyst was able to be reused for several times with a slight loss in its catalytic activity.
研究领域:
催化化学
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可再生化学
✓ 已验证
DOI
高影响因子
Journal of Biobased Materials and Bioenergy
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2017
·Vol. 11
·期 6
·543-552
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IF 0.975
Dong Kaijun,Zhang Jun,Luo Weimin,Su Lin,Huang Zhilin
A series of zirconium based catalysts were synthesized to study the transfer hydrogenation of biomass derived ethyl levulinate into γ-valerolactone (GVL) using lower alcohols as hydrogen donors. The essential textural and chemical characteristics of prepared samples were
identified by various techniques including SEM, XRD, NH3-TPD, TGA, CO2-TPD and nitrogen physisorption. Parameters such as hydrogen donor, catalyst type, temperature, stirring rate, and catalyst dosage were found to play a critical role in GVL production. A promising GVL
yield of 98.3 mol% with a highest GVL formation rate at 5239.4 μmol g–1
cat h–1 was obtained in isopropanol at 433 K over zirconium oxide derived from zirconyl nitrate. The recycling experiments revealed that the zirconium oxide catalyst
derived from zirconyl nitrate presented relatively satisfied performance and stability.
研究领域:
化学工程
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催化材料科学
✓ 已验证
DOI
高影响因子
BIORESOURCE TECHNOLOGY
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2021
·
IF 9.642
Wenran Gao,Gang Wu,Xun Zhu,Muhammad Asif Akhtar,Guiying Lin,Xun Hu,Yong Huang,Shu Zhang,Hong Zhang
The conversion of cellulose to platform chemicals has attracted much attention because of its renewability. This work proposed an earth-abundant cobalt disulfide as a heterogeneous catalyst for methyl levulinate production from cellulose. The highest yield of methyl levulinate reached 61 mol% under the tested conditions of 200 °C, 2 MPa initial pressure, 0.45 catalyst/cellulose mass ratio, and 3 h reaction time. The XRD and TEM analyses demonstrated the crystal facet (111) of cobalt disulfide as a robust active site, which was in good agreement with the highest acidity of the crystal facet (111) calculated by the work functions. The XPS characterization showed that the main chemical valence of cobalt disulfide responsible for the methyl levulinate production was the surface Co 2+ species. This study is valuable for the development of a recoverable catalyst for the cellulose to methyl levulinate process.
研究领域:
化学工程
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催化
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可再生能源
✓ 已验证
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）