FUEL
·
2017
·
IF 4.601
Chuang Li,Guangyue Xu,Yongxiang Zhai,Xiaohao Liu,Yanfu Ma,Ying Zhang
Gamma-valerolactone (GVL) has been identified as a sustainable high-value platform molecular for the production of fuels and carbon-based chemicals. In this work, a series of activated carbon supported low-cost bimetallic Ni-Fe catalysts (Ni-Fe/AC) with different molar content of Fe species were prepared by using co-precipitation method for the liquid phase hydrogenation of ethyl levulinate (EL) to produce γ-valerolactone. The Ni-Fe 0.5 /AC exhibited the highest activity among the bimetallic or monometallic catalysts under mild reaction conditions (100 °C, 4 MPa H 2 , 6 h) and achieved 99.3% conversion of EL and 99.0% yield of GVL. Under more mild conditions (60 °C, 2 MPa H 2 ) and prolonging the reaction time to 24 h, EL could be converted completely and the obtained GVL yield was more than 98%. The catalysts were characterized by various techniques including XRD, TEM, HRTEM, EDX, XPS, H 2 -TPR and NH 3 -TPD. Based on the structure and activity relationship study, the formation of highly dispersed Ni-Fe alloy structure and the co-presented FeO x nanoparticles could be responsible for the high catalytic hydrogenation activity.
研究领域:
催化化学
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可再生资源化学
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DOI
高影响因子
JOURNAL OF CHEMICAL TECHNOLOGY AND BIOTECHNOLOGY
·
2018
·Vol. 94
·期 1
·167-177
·
IF 2.587
Xuejuan Cao,Junnan Wei,Huai Liu,Xinyue Lv,Xing Tang,Xianhai Zeng,Yong Sun,Tingzhou Lei,Shijie Liu,Lu Lin
BACKGROUND γ-Valerolactone (GVL) is a versatile biomass-derived platform molecule that could serve as a building block to produce chemicals, materials and fuels, but the production of GVL from biomass via a cost-competitive method is challenging. In this contribution, a robust Cu─Mg oxide was prepared as an efficient bifunctional catalyst for both H 2 production by MeOH reforming and hydrogenation of methyl levulinate (ML) to GVL in MeOH medium. RESULTS Cu 0.87 Mg 0.13 O x prepared by a urea hydrolysis method offered a GVL yield up to 90.6% at 220°C in 4 h without external hydrogen. This catalyst could be reused for at least seven consecutive cycles without loss of its activity. Notably, Cu 0.87 Mg 0.13 O x also provided nearly 70% GVL yield in methanolysis products of cellulose in the presence of humins. Characterization of the catalyst indicates that the incorporation of MgO greatly facilitates the stabilization of Cu + species that possess a better catalytic performance in ML hydrogenation compared with metallic Cu. CONCLUSION This robust Cu 0.87 Mg 0.13 O x could greatly contribute to develop a highly facile and desirable two-step strategy for GVL production from cellulose, through the integration of ML production by methanolysis of cellulose, H 2 formation by MeOH reforming and ML hydrogenation in MeOH medium. © 2018 Society of Chemical Industry
研究领域:
化学工程
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可再生资源化学
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DOI
高影响因子
CATALYSIS LETTERS
·
2020
·Vol. 150
·期 9
·2709-2715
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IF 2.482
Mao Fei-Feng,Zhao Wenguang,Tao Duan-Jian,Liu Xianxiang
Abstract A new solid acid catalyst Fe 3 O 4 @TNTs-SO 3 H was successfully prepared, characterized, and applied for efficient conversion of renewable levulinic acid to n -butyl levulinate, serving as a promising liquid fuel additive. This catalyst was demonstrated to show high catalytic activity and afford n -butyl levulinate with a yield of 94.6% under optimum conditions. Graphic Abstract
研究领域:
化学工程
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催化材料
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能源化学
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DOI
高影响因子
CATALYSIS LETTERS
·
2020
·Vol. 151
·期 2
·538-547
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IF 2.482
Chen Han,Xu Qiong,Li Hui,Liu Jian,Liu Xianxiang,Huang Geng,Yin Dulin
Nickel supported on equilibrium fluid-catalytic-cracking catalysts (Ni/E-cats) were prepared by a simple grinding-pyrolysis method and employed for the transfer hydrogenation of ethyl levulinate (EL) to γ-valerolactone (GVL). 96.2% selectivity of GVL and 90.3% conversion of EL were obtained at 180 °C for 6 h over 30-Ni/E-cat. Through XRD, N 2 adsorption–desorption, NH 3 -TPD and SEM analysis, the high activity of the 30-Ni/E-cat catalyst was attributed to its dispersed Ni metal active centers and available acidic sites. Catalytic probe test revealed that metal and acid sites of Ni/E-cat played a synergistic catalytic role in the synthesis of GVL in 2-propanol, where Ni metal sites contribute to the hydrogenation of ketone group in EL, and acid sites of E-cat promoted the lactonization of intermediate ethyl- or isopropyl 4-hydroxyvalerate. Two reaction pathways and synergistic mechanism were proposed in this catalytic system. Moreover, Ni/E-cat catalyst exhibited good stability up to four cycles without obvious loss of catalytic activity. Graphic Abstract
研究领域:
化学工程
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催化科学
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DOI
高影响因子
Molecular Catalysis
·
2021
·
IF 5.062
Haijun Guo,Shuai Ding,Hairong Zhang,Can Wang,Fen Peng,Lian Xiong,Xinde Chen,Xinping Ouyang
The acid-activated Palygorskite (H + -PAL) was applied to support Cu(M)NiCoB amorphous alloy catalysts with high-activity and self-regeneration ability for selective hydrogenation of butyl levulinate (BL) to γ-valerolactone (GVL). The catalysts were characterized by ICP-OES, nitrogen physisorption, XRD, FE-SEM, TEM, XPS, H 2 -TPD, NH 3 -TPD and FTIR-pyridine adsorption techniques. Compared to the unsupported Cu 0.5 Ni 1 Co 1 B catalyst, the Cu 0.5 Ni 1 Co 1 B/H + -PAL catalyst showed the highest GVL yield of 96.3 % with BL conversion of 99.7 % at 200 °C. When Mo was doped into the Cu 0.5 Ni 1 Co 1 B/H + -PAL catalyst, the GVL yield showed gradually increase to 95.7 % with BL conversion of 100 % after five times run. The high activity and self-regeneration ability was attributed to the Mo doping effect and the synthetic effect between Cu hydrogenation active species and H + -PAL support. Various characterization results indicated that Mo acted as both structural promoter to improve the dispersion of metallic Cu and CuMoNiCoB amorphous alloy and electronic promoter to enhance the formation and increase the fraction of Cu + species. In addition, the incorporation of Mo provided more Lewis acid sites to promote BL conversion to GVL and GVL conversion to 1,4-PDO and n-PeOH. On the basis of characterization and catalytic performance testing results, the synergistic effect between CuMoNiCoB amorphous alloy and Cu 2 O/Cu hydrogenation sites and Lewis/Brønsted acid site of H + -PAL support is considered to be the key to produce GVL.
研究领域:
化学工程
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催化
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材料科学
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DOI
高影响因子
JOURNAL OF AGRICULTURAL AND FOOD CHEMISTRY
·
2023
·
IF 6.1
Dingkai Wang,Mingyu Cui,Yanjun Li,Wei Zhao,Shangshang Ma,Zhijie Jiang,Xutang Liu,Chong Liang,Rujuan Li,Long Ma,Yanmin Song,Xian-Yong Wei
The facile, green, and efficient strategy for the separation of lignin from straw and subsequent production of value-added chemicals is crucial to the current utilization of straw. Herein, up to 23.72% of lignin was isolated from wheat stalk over cheap and green 1-(3-sulfobutyl) triethylammonium hydrogen sulfate ([BSTEA]HSO4) in aqueous ethanol (Vethanol: Vwater = 4:1). The acquired lignin was verified as a p-hydroxyphenyl-guaiacyl-syringyl type, which had a narrower molecular weight distribution, better thermal stability, and higher purity compared with those of the lignin obtained using 1-methyl-3-(4-sulfobutyl)-imidazolium hydrogen sulfate and 1-(3-sulfobutyl) pyridinium hydrogen sulfate. Moreover, a carbohydrate-rich liquid containing [BSTEA]HSO4 was obtained by water removal from the waste liquid after lignin separation and further converted to ethyl levulinate (EL) by a one-pot process in the presence of inexpensive and stable USY zeolite. The yield of EL reached 30.23% at 200 °C for 60 min over the presence of 40% [BSTEA]HSO4 and 60% USY zeolite. Under optimal conditions, the yields of lignin and EL can respectively reach 83.89 and 72.28% of those catalyzed by a fresh catalyst after five cycles. In short, the above-mentioned methods present a green, economic, and efficient route for the extraction of lignin and further treatment of the liquid waste generated during the extraction process.
研究领域:
生物质能
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绿色化学
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产品关联
DOI
PubMed
高影响因子
FUEL
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2023
·
IF 7.4
Honghui Gong,Juan Zhang,Qi Li,Longxing Wei,Ya Hu,Yifan Rui,Xian-Lei Shi
A series of sulfonic acid functionalized coffee biochar (SFCB-x) with high acid density and strength were prepared by using sulfuric acid as the sulfating agent. The obtained catalysts could be directly used for esterification of levulinic acid (LA) and alcoholysis of furfural alcohol (FA) affording ethyl levulinate (EL). Further activity tests and characterization confirmed the linear correlation between the catalytic activity and -SO 3 H density of the catalyst, SFCB-4 holds the highest -SO 3 H density and thus exhibits the highest catalytic activity towards the production of EL. Under mild conditions, about 97.6% and 81.7% yield of EL could be obtained for LA esterification and alcoholysis of FA, respectively. The catalyst also shows high stability during consecutive catalytic recycles. Furthermore, hot filtration testing suggested that the leaching of the active species was not observed during catalytic recycles, which could be attributed to the covalently linked -SO 3 H groups on SFCB-4 skeleton. The rational design and construction of SFCB-4 will drive the development of solid acid catalyst derived from natural biomass for the production of bio-based chemicals.
研究领域:
化学工程
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生物质能
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催化科学
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产品关联
DOI
高影响因子
Molecular Catalysis
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2023
·
IF 4.6
Yi Tian,Kangyu Zhao,Shuolin Zhou,Qiong Xu,Dulin Yin,Xianxiang Liu
Furfuryl alcohol (FOL), as a cheap green biomass derivative, has high potential application value in the production of various biomass chemicals. In this work, a sulfonic acid functional porous organic polymer-coated carbon nanotubes catalyst (CNTs@PDVTA-SO 3 H) was successfully prepared. The structure of as-prepared catalysts was confirmed by TG/DTG, Raman spectra, TEM, FT-IR, N 2 adsorption-desorption, and XPS measurements. The catalytic properties of CNTs@PDVTA-SO 3 H were evaluated for the synthesis of n -butyl levulinate (BL) via the alcoholysis of FOL. It was found that the 99.1 % yield of BL was achieved under optimal conditions. The apparent activation energy of FOL to 2-bufurdoxy methyl-furan (BMF) and BMF to BL was 58.08 kJ/mol and 35.38 kJ/mol, respectively. This work provides a new avenue for the preparation of alkyl levulinates using FOL as raw material.
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产品关联
DOI
高影响因子
RSC Advances
·
2013
·Vol. 3
·期 26
·10277-10284
·
IF 2.562
Xing Tang,Lei Hu,Yong Sun,Geng Zhao,Weiwei Hao,Lu Lin
A green and efficient process was developed for the conversion of biomass-derived ethyl levulinate (EL) into γ-valerolactone (GVL) using supercritical ethanol as the hydrogen donor and the reaction medium over low-cost and eco-friendly ZrO2 catalysts, which were prepared by the precipitation method and characterized by BET, SEM, XRD, FT-IR, TGA-DTA, TPD-NH3 and TPD-CO2. The results indicated that amorphous ZrO2 with a high specific surface area and a large number of acid–base sites exhibited the highest catalytic activity, an excellent GVL yield of 81.5% with 95.5% EL conversion was achieved at 523 K over 3 h. In addition, combined with the results of poisoning experiments, a plausible mechanism of catalytic transfer hydrogenation (CTH) via a six-membered ring transition state was also presented.
研究领域:
生物质化学
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催化反应工程
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DOI
高影响因子
Sustainable Chemistry and Pharmacy
·
2026
·
IF 6.7
Deyang Zhao,Xinyu Zhao,Qikai Si,Kongde Li,Huawei Yang,Christophe Len
γ-valerolactone (GVL) is a renewable and sustainable platform chemical derived from biomass, with broad applications in chemical synthesis and energy-related fields. Consequently, the development of efficient strategies for GVL production has attracted significant attentions. In this study, the hydrogenation of ethyl levulinate (EL) to GVL was investigated using copper-cobalt basic carbonate, (CoCu) 2 (OH) 2 CO 3 , as a catalyst. The influence of different substrates—including esters and acids such as EL, GVL, ethyl acetate (EA), and levulinate acid (LA)-on catalyst recyclability and performance was systematically evaluated. Among the substrates tested, EL exhibited the most favorable behavior, delivering a GVL yield of up to 96% in the second recycling cycle under optimized conditions. This superior performance is attributed to the synergistic interaction between the basic sites of the catalyst and the ability of metallic Cu to activate hydrogen, as well as the formation of larger metal particle clusters when EL is used as the substrate. Notably, the catalytic activity remained largely preserved even after the third recycling cycle. In contrast, when GVL was sued as the substrate, moderate yields were obtained, accompanied by the formation of surface coatings on the catalyst particles. Furthermore, both EA and LA induced varying degrees of catalyst etching, resulting in a drastic loss of activity, with negligible catalytic performance observed in the second cycle. These findings indicate that catalyst deactivation due to etching has a more pronounced impact on catalytic performance than structural changes associated with bimetallic cluster formation. This observation indirectly highlights the critical role of basic sites in maintaining catalytic activity during the hydrogenation process.
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DOI
高影响因子
RENEWABLE ENERGY
·
2015
·
IF 3.476
Guizhuan Xu,Chun Chang,Shuqi Fang,Xiaojian Ma
Cellulose reactivity in ethanol at elevated temperature (170–210 °C) was investigated in this study. Water and acid catalyst can improve the solubilization and the conversion of cellulose in ethanol. In ethanol/water medium, more humic solids will be formed, but the amounts of diethyl ether decreased greatly. In ethanol medium, the ethanolysis reaction of cellulose played a dominant role, with ethyl levulinate (EL) as the main liquid product. In addition, organic esters and furan derivatives were the main small molecules in the liquid, and diethoxymethane and diethyl sulfate were considered as the main liquid by-products. On the basis, the kinetics of one-pot preparation of EL from cellulose was further investigated at a temperature range of 170–210 °C and an acid concentration range of 0.5–2.0 wt%. Artificial Neural Network (ANN) was employed to develop an approach for the evaluation of the process. A good agreement of the ANN model results and the experimental data was obtained, and the optimum reaction conditions for one-pot preparation of EL were temperature 188 °C, reaction time 30 min, acid concentration 1.2 wt%. Under the conditions, higher EL yield can be obtained, which was close to the ANN model result.
研究领域:
化学工程
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生物化学
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DOI
高影响因子
CHEMICAL PAPERS
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2013
·Vol. 67
·期 11
·1355-1363
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IF 0.879
Gui-Zhuan Xu,Chun Chang,Wei-Na Zhu,Bo Li,Xiao-Jian Ma,Feng-Guang Du
Direct production of ethyl levulinate (EL) from glucose catalysed by a liquid acid catalyst (sulfuric acid) and a solid acid zeolite catalyst USY NKF-7 (USY) in ethanol media was investigated in this study. Effects of the initial glucose concentration (C
G0), reaction temperature (T), amount of acid catalyst, and water addition on the yields of EL were compared, respectively. The results show that higher yield of EL can be obtained at lower C
G0. Higher temperature and acid concentration can accelerate the reaction rate, but the formation rate of the by-products increases more quickly than that of EL. Water addition also can result in the decrease of the yield of EL. Although sulfuric acid is efficient in the production of EL, the USY is more efficient in converting glucose to 5-ethoxymethyl-2-furaldehyde. Moreover, the use of USY can limit the diethyl ether production, and it can be reused for multiple times.
研究领域:
生物化学
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催化化学
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DOI
高影响因子
危险品化学品经营许可证（带存储）