Asia-Pacific Journal of Chemical Engineering
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2024
·Vol. 19
·期 4
·e3076
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IF 1.4
Haoran Zhao,Yu Jia,Yihang Chen,Xuanyu Liang,Jinbo Hao,Binglin Chen,Chao He,Liang Liu,Chun Chang,Guizhuan Xu
Ethyl levulinate (EL) production from steam-exploded corn straw (SCS) in a cascade of reaction using a Brønsted (B) acid and a Lewis (L) acid in ethanol was studied. The entangled structure of corn straw could be obviously damaged through steam explosion when the pressure was 1.5 MPa holding 10 min. The content of cellulose can be increased from 35.9% to 46.8%, and the contents of hemicellulose and lignin were changed from 16.7% to 8.8% and 22.6% to 27.5%, respectively. EL yield was significantly increased from 10.7 to 24.6 wt% under optimal reaction conditions (L/B = 1/20 [mol/mol], 205°C, 90 min, 1.8 g of SCS, 60 mL of ethanol). According to kinetic models, the activation energies for the main and side reactions were 56.8 and 110.5 kJ mol −1 , respectively. It suggested that SCS was more easily to be converted to EL rather than other by-products. The highest occupied molecular orbital (HOMO)–lowest unoccupied molecular orbital (LUMO) energy gaps (HOMO-LUMO gaps) of cellobiose over the mixed acids in ethanol were significantly reduced with frontier molecular orbital (FMO) theory. This work provides an effective strategy for EL production from agricultural waste straws.
研究领域:
生物化学
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可再生资源与环境科学
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DOI
高影响因子
APPLIED ENERGY
·
2015
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IF 5.613
Junfeng Feng,Jianchun Jiang,Junming Xu,Zhongzhi Yang,Kui Wang,Qian Guan,Shuigen Chen
One-step preparation of methyl levulinate from biomass was investigated. The process used was direct liquefaction under pressure in methanol using a 1 L autoclave. Bamboo, a lignocellulosic biomass , was liquefied using sulfuric acid in subcritical methanol. When sulfuric acid was used as the catalyst, a 30.75 wt% methyl levulinate yield could be obtained from bamboo at 200 °C after a reaction time of 120 min when the catalyst loading was 2.5 wt% per 60 g bamboo. In addition, microcrystalline cellulose , corn starch , methyl glucoside and glucose were selected as model compounds for the liquefaction reaction so that the biomass to methyl levulinate reaction pathway could be investigated. The results suggested that lignocellulosic biomass is a renewable material that can be used to produce a high value-added fuel additive (methyl levulinate) by the direct liquefaction under pressure reaction process.
研究领域:
生物化学
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可再生能源
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DOI
高影响因子
CELLULOSE
·
2017
·Vol. 24
·期 12
·5403-5415
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IF 3.417
Deng Lin,Chang Chun,An Ran,Qi Xiaoge,Xu Guizhuan
Direct production of butyl levulinate (BL) by butanolysis of cellulose was carried out using single or combined metal sulfates catalysts. The synergetic enhancement of the ferric sulfate and aluminum sulfate can improve the conversion of cellulose to BL. Moreover, the butanolysis of cellulose was optimized by using response surface methodology. Under the optimum conditions of 194 °C, catalyst concentration 10.0 g/L and reaction time 3 h, the average cellulose conversion of 100% and BL yield of 40.3% were obtained. In addition, the analysis of liquid products and the characterization of catalyst were performed, and the reusability experiments showed that the metal sulfates can be easily recycled and be reused more than five times with high activity in the butanolysis process. This study provided an economical and feasible method for bio-based BL production from cellulose.
研究领域:
生物化学
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可再生资源与环境工程
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DOI
高影响因子
Journal of Bioresources and Bioproducts
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2023
·
IF 0
Yan Ma,Hongxiao Wang,Ziyang Wu,Weihong Tan,Guodong Feng,Jianchun Jiang
Ethyl levulinate (EL) is a key biomass-derived compounds due to its socio-economic benefits for the synthesis of commodity chemicals. Herein, we proposed an efficient one-step bamboo conversion to EL in ethanol, and a novel stepwise fractionation to purify EL and lignocellulose degradation products. A proton acid, due to its high catalytic efficiency, yielded 26.65% EL in 120 min at 200 °C. The productions of ethyl glucoside and 5-ethoxymethylfurfural were analyzed in terms of by-products formation. To the best of our knowledge, there is no single report on catalyst for one step synthesis of EL directly from bamboo, as well as a stepwise fractionation to purify EL. Due to similar physiochemical properties in each fraction, the platform molecules could broaden a new paradigm of bamboo biomass utilization for renewable energy and value-added biochemicals. In addition, glucose, ethyl glucoside, corn starch, and microcrystalline cellulose were also investigated as substrates, so that the reaction intermediates of this one-pot procedure were identified and a possible reaction mechanism was proposed.
研究领域:
生物化学
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可再生资源与环境
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DOI
TURKISH JOURNAL OF CHEMISTRY
·
2022
·Vol. 45
·期 4
·1133-1145
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IF 1.151
WANG DING-KAI,ZHAO WEI,CUI MING-YU,GUO TIAN-TIAN,FU SHUI-YUAN,LI WEI-GANG
A series of Zr(SO4)2/SiO2 solid acid catalysts with different Zr(SO4)2 loadings were prepared by water-soluble-impregnation method at room temperature. Then, the prepared catalysts were characterized by Fourier transform infrared spectroscopy, transmission electron microscopy and energy-dispersive X-ray spectrum, X-ray diffraction, adsorption/desorption of N2, and temperature-programmed desorption of NH3. The results showed that the active component Zr(SO4)2 was successfully adhered to the mesoporous SiO2, and the acid amount of Zr(SO4)2/SiO2 increased with the increasing of the Zr(SO4)2 loadings. Finally, the wheat stalk was used as raw material and depolymerized over Zr(SO4)2/SiO2 to produce ethyl levulinate (EL). The reaction mixture was separated and purified by filtration and vacuum distillation. The kinetic characteristics and the reaction pathway were also studied. A comparative study showed that 20 wt.% Zr(SO4)2/SiO2 exhibited higher catalytic activity. When reaction temperature, time, catalyst dosage and Zr(SO4)2 loadings were 190 °C, 50 min, 20 wt.% and 30 wt.%, the EL yield reached a maximum of 17.14%. The relative content of EL exceeded 90% after three steps of distillation.
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DOI
高影响因子
INDUSTRIAL CROPS AND PRODUCTS
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2018
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IF 3.849
Qian Guan,Tingzhou Lei,Zhiwei Wang,Haiyan Xu,Lu Lin,Gaofeng Chen,Xueqin Li,Zijie Li
Wheat straw, a typical lignocellulosic biomass, is difficult to be liquefied because of its complex structure, which limits its further conversion to valuable products. Ionic liquid can dissolve the cellulose, which can destroy the connection of biomass components. Ionic liquids, [BMIM][HSO 4 ], [BMIM][Cl], and [HSO 3 -BMIM][HSO 4 ], were used in the liquefaction of wheat straw to produce ethyl levulinate (EL) in a one-pot reaction under mild conditions in ethanol, which served as both solvent and reactant. The highest conversion rate, 85.50%, was obtained following reaction at 200 °C for 60 min using the acidic ionic liquid 1-methyl-3-(4-sulfobutyl) imidazole bisulphate as the catalyst. Under optimal conditions, ethyl levulinate was obtained with a yield of 16.23% and its content in the liquid products was 28.11%. Without the acidic ionic liquid catalyst, the conversion rate of wheat straw and the yield of ethyl levulinate were only 22.33% and 6.23%, respectively. Of the catalysts evaluated, [HSO 3 -BMIM][HSO 4 ] was the most effective, and its recovery rate was 64.71%. This study provides a theoretical basis for the development and utilisation of low-corrosion and environment-friendly catalysts for liquefaction processes for the preparation of high-grade chemicals.
研究领域:
生物化学
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可再生能源
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DOI
高影响因子
Journal of Energy Chemistry
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2016
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IF 2.322
Bingfeng Chen,Fengbo Li,Zhijun Huang,Guoqing Yuan
Furfural is directly converted to levulinate esters (isopropyl levulinate and furan-2-ylmethyl-levulinate) as potential biofuel feedstocks , through a combined catalytic strategy. Nb 2 O 5 -ZrO 2 mixed oxide microspheres are used as bifunctional catalysts for hydrogen-transfer hydrogenation and acid-catalyzed alcoholysis in isopropanol. Bifunctional catalysts improve sustainability of furfural conversion through process intensification. Hydrogen transfer hydrogenation from isopropanol avoids dangerous hydrogen gas , and abates process and environmental costs. Isopropyl levulinate and furan-2-ylmethyl-levulinate are the main products that can be applied as blending components in biodiesel or hydrocarbon fuels.
研究领域:
化学工程
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可再生能源
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DOI
高影响因子
JOURNAL OF CHEMICAL TECHNOLOGY AND BIOTECHNOLOGY
·
2021
·Vol. 97
·期 1
·240-253
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IF 3.174
Zhihang Huang,Songyuan Hao,Hong Yuan
BACKGROUND A novel double acid site solid catalyst (Al-OCS-0.1) having an ordered mesoporous structure was synthesized by grafting sulfonic acid groups on an oxidized ordered mesoporous carbon (OOMC) support and loading 10% Al 2 (SO 4 ) 3 . RESULT Assessments using Field emission scanning electron microscopy, Transmission electron microscopy and X-ray diffraction showed that the OMC structure remained unchanged after the chemical modification and Al 2 (SO 4 ) 3 loading. The Brunauer–Emmett–Teller surface area and average pore size of Al-OCS-0.1 decreased to 181 m 2 g −1 and 7.1 nm after loading Al 2 (SO 4 ) 3 , respectively. Ammonia temperature-programmed desorption (NH 3 -TPD) and Pyridine adsorption infrared spectroscopy (Py-IR) demonstrated that Al-OCS-0.1 had abundant Brønsted and Lewis acid sites. The ammonia desorption of Al-OCS-0.1 increased from 2.0 to 7.2 mmol g −1 after loading Al 2 (SO 4 ) 3 . CONCLUSION The Al-OCS-0.1 was used to catalyze the synthesis of ethyl levulinate from cellulose in ethanol and gave an extremely high yield of 50.8 mol% after 5 h at 200 °C. © 2021 Society of Chemical Industry (SCI).
研究领域:
化学工程
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催化材料科学
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DOI
高影响因子
ACS Catalysis
·
2022
·
IF 13.7
Anon Bunrit,Teera Butburee,Meijiang Liu,Zhipeng Huang,Keerati Meeporn,Chaiyasit Phawa,Jian Zhang,Sanchai Kuboon,Huifang Liu,Kajornsak Faungnawakij,Feng Wang
Herein, we developed photo–thermo-dual catalytic strategies for the production of γ-valerolactone (GVL) from levulinic acid (LA) and its ester using platinum-loaded TiO2 as a dual-functional catalyst. Both catalytic systems were evaluated under mild reaction conditions. In the photocatalysis system, a base plays crucial roles in the conversion of LA and EL to GVL. The control experiments reveal that plausible mechanistic pathways of both systems proceed via the hydrogenation of the ketone group of LA to the corresponding alcohol as a major intermediate followed by a subsequent cyclization step to GVL. This dual-functional catalyst provides alternative strategies for the conversion of LA and its ester into GVL, which could pave the way for biomass utilization in a more effective and practical manner.
研究领域:
催化
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生物质转化
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化学工程
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可持续化学
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DOI
高影响因子
BIORESOURCE TECHNOLOGY
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2025
·
IF 9
Zhen Ma,Jingyang Zhang,Yucheng Lin,Xiuli Han,Haoran Wu,Chunbao Xu,Chun Chang
Achieving the efficient biomass alcoholysis to methyl levulinate (ML) under high solid content conditions and establishing its kinetic model are crucial, but remain challenging. Here, the alcoholysis of microcrystalline cellulose (MC) and xylose residue (XR) to ML under high solid content conditions using CuSO 4 as a catalyst was reported. High yield (34.96 wt%) and concentration (41.48 g/L) of ML from MC alcoholysis are achieved under the optimal conditions. Meanwhile, the yield and concentration of ML from XR alcoholysis can reach 26.73 wt% and 31.72 g/L, respectively. The alcoholysis pathways of MC and XR are proposed. A mixed model consisting of a shrinking core model and a pseudo-first-order kinetic model was established to elucidate the alcoholysis behavior of biomass. The generation of glucose is the rate-limiting step of the alcoholysis process, and there is no significant dependence between the activation energies of main reactions and the solid content of biomass.
研究领域:
生物化学
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可再生资源工程
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产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Huai Liu,Yanping Kong,Weipeng Song,Rui Zhang,Junhua Zhang,Yong Sun,Lincai Peng
The inhibition effect of impurities in the raw lignocellulosic biomass greatly impedes its direct acid-catalyzed alcoholysis process to produce downstream chemicals. Previous literatures widely investigated the inhibition problems of lignin content and cellulose crystallite in the raw biomass for the production of alkyl levulinate (AL), while the effect of inorganic matters on this process only received cursory attention. In this contribution, the vital importance of ash removal in raw material for efficient catalytic alcoholysis of cellulose fraction been highlighted. Moreover, it has been found that the facile pretreatment of Napier grass stem greatly facilitates the acid-catalyzed alcoholysis of its cellulose fraction towards ethyl levulinate (EL), a versatile commodity chemical. EL yield as high as 72.1 % can be accomplished from the NaOH-pretreated Napier grass stem in ethanol/γ-valerolactone co-solvent medium over Al(OTf) 3 at 170 ℃ for 150 min, which is almost ten times that from the pristine one in ethanol medium. It is also interesting to note that a facile and green water prewashing treatment can efficiently remove the inorganic component of the raw biomass, which thus largely promotes the conversion of Napier grass stem to EL. The activation energies of cellulose degradation and glucopyranoside alcoholysis after pretreatment decreased to 62.4 kJ/mol and 68.6 kJ/mol, respectively. This work presents a highly-reliable strategy for valorizing grass lignocellulosic feedstock to produce bio-based ester compounds.
研究领域:
生物化学
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可再生资源与环境科学
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产品关联
DOI
高影响因子
APPLIED CATALYSIS A-GENERAL
·
2026
·
IF 4.8
Ying Gao,Jinxing Long
Conversion of ethyl levulinate to GVL was proposed using Pd 4 /UiO-66-NH 2 . • Pd 4 /UiO-66-NH 2 was constructed via a post-synthetic modification strategy. • Synergistic effects between Pd species and acidic sites drive superior performance. • GVL yield of 90% with 98.9% selectivity was achieved under 170 ℃ and 1.0 MPa H 2 . • The catalyst shows good recyclability, and can be reused for at least five runs. An efficient strategy is proposed for direct hydrogenation of ethyl levulinate (EL) to γ-valerolactone (GVL) using a highly dispersed palladium nanoparticles supported on the UiO-66-NH 2 framework (Pd/UiO-66-NH 2 ), which was prepared via a facile post-synthetic modification by anchoring palladium (Pd) nanoparticles on the framework's native -NH 2 groups. Under optimized conditions (170 °C, 1.0 MPa H 2 ), 90% yield and 98.9% selectivity of GVL were shown when the reaction was catalyzed by Pd 4 /UiO-66-NH 2 in cyclohexane. Catalyst characterization using XRD, N 2 adsorption-desorption, FT-IR, TEM, TGA, XPS and H 2 -TPR, confirmed that an intensive synergistic effect existed between the Pd and the acidic sites, which is responsible for the superior performance of Pd@UiO-66-NH 2 . The solvent effect and the feedstock adaptability were also investigated. Furthermore, the catalyst of Pd 4 /UiO-66-NH 2 demonstrated good stability and reusability, where no significant activity loss was shown even after five consecutive cycles. Therefore, this study provides new insights for efficient upgrading biochemical. Download: Download high-res image (188KB) Download: Download full-size image
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高影响因子
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