RENEWABLE ENERGY
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2021
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IF 8.001
Ruoqing Wang,Feng Shen,Yiwei Tang,Haixin Guo,Richard Lee Smith,Xinhua Qi
Levulinic acid in high yields (90%) was produced from hemicellulose-derived furfuryl alcohol catalyzed by a uniform, dandelion-like, SO 3 H-modified silica nanoflower solid acid (SiNF–SO 3 H). The SiNF–SO 3 H catalyst was prepared by soft template method in microemulsion system, followed by grafting of –SH and oxidation of –SH to –SO 3 H at room temperature to avoid use of corrosive sulfonating agents such as concentrated H 2 SO 4 . Dandelion-like porous structures of the SiNF–SO 3 H catalyst provided accessible and abundant catalytic sites ensuring high activity for furfuryl alcohol conversion (100%). Mixed-solvent γ -valerolactone-water (GVL-H 2 O) inhibited undesirable furfuryl alcohol polymerization reactions ensuring highly selective conversion of furfuryl alcohol to levulinic acid. Combination of catalyst and solvent system allowed achievement of the highest levulinic acid yields that have been reported to date. Both the catalyst synthesis protocol and reaction solvent (GVL-H 2 O) are green and sustainable. The SiNF–SO 3 H/(GVL-H 2 O) catalytic system has application to many acid catalyzed schemes for lignocellulosic biomass conversion.
研究领域:
化学工程
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催化
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绿色化学
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生物质转化
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产品关联
DOI
高影响因子
JOURNAL OF APPLIED POLYMER SCIENCE
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2020
·Vol. 137
·期 36
·49066
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IF 2.52
Yigane Wang,Xiaoan Nie,Guigan Fang,Laihui Xiao
Epoxy bisphenol acid isooctyl ester (EBAIE) was synthesized and characterized by FTIR and H-NMR. EBAIE was used as poly(vinyl chloride) (PVC) plasticizer for the first time, and its addition amount was 30 wt% of PVC. The mechanical properties, thermal stability, compatibility, and decomposition activation energy of PVC blends were systematically studied. Compared to the commercial plasticizer-dioctyl phthalate (DOP), the tensile strength had been significantly increased from 30.64 to 45.07 MPa, while the elongation at break had little difference. The thermal stability analysis showed that the static stability time at 180°C had been extended from 40 to 300 min. The decomposition activation energy indicated that the EBAIE plasticized PVC was with a higher thermal stability. The extraction and volatility resistance of the novel plasticizer were superior to those of DOP.
研究领域:
材料科学
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化学工程
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产品关联
DOI
高影响因子
CELLULOSE
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2019
·Vol. 26
·期 15
·8313-8323
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IF 3.917
Wang Chao,Yang Guihua,Zhang Xueming,Shao Lupeng,Lyu Gaojin,Mao Jianzhen,Liu Shijie,Xu Feng
Levulinic acid (LA) production from corncob acid hydrolysis residues (CAHR) using FeCl 3 as Lewis acid catalyst in green solutions of salt was investigated. The reaction kinetic relationships were determined in the temperature range of 160–180 °C, with FeCl 3 concentrations of 0.12–0.36 M, and a reaction time of 0–60 min. The maximum LA concentration of 59.0 mol% (24.5 g/L) was achieved at 170 °C in a 30% NaCl solution containing 0.24 M FeCl 3 . A pseudo first-order kinetic model was proposed to describe the cellulose deconstruction to LA. The model agreed perfectly with the evolution in the concentrations of the major compounds such as glucose, 5-hydroxymethylfurfural and LA during the CAHR hydrolysis. The kinetic model developed for CAHR was in good agreement with that previously developed for other lignocellulosic systems. Based on our kinetic model and reaction system, the LA yield is increased at the lower end of the temperature range with the higher acid concentrations. The results indicated that the concentrated seawater after desalination could be a green solvent in the biorefinery.
研究领域:
化学工程
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生物技术
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可再生能源
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产品关联
DOI
高影响因子
Molecular Catalysis
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2018
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IF 0
Zhongzhe Wei,Xuefeng Li,Jiang Deng,Jing Wang,Haoran Li,Yong Wang
The catalytic transformation from levulinic acid (LA) into γ-valerolactone (GVL) is of great interest as it is an impressive strategy to convert lignocellulosic platform chemical into high value-added compounds. Herein, a novel heterogeneous catalyst made of Ru nanoparticles (NPs) supported on N-doped hierarchically porous carbon from biomass, Ru/NHPC, was shown to be highly active, selective and stable in this transformation. The reaction can proceed smoothly under mild conditions in aqueous media even at room temperature. The catalyst Ru/NHPC could be recycled for 13 consecutive runs exhibiting no obvious activity decay, much better than that of Ru NPs supported on activated carbon. The process offers an efficient, environmentally responsible, and safe approach to high production of GVL.
研究领域:
化学工程
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可再生能源
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环境科学
✓ 已验证
产品关联
DOI
Waste and Biomass Valorization
·
2017
·Vol. 10
·期 5
·1141-1150
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IF 1.337
Fang Chengjiang,Liu Yanxiu,Wu Weibo,Li Hu,Wang Zhongwei,Zhao Wenfeng,Yang Tingting,Yang Song
Liquid-phase catalytic hydrogenation of furfural, followed by hydration to levulinic acid has been considered as one of efficient approaches for upgrading pentose sugars. However, a two-step process is generally employed, which involves the separation and purification of the key intermediate furfuryl alcohol from the reaction mixture. To simplify this catalytic process with improved efficiency, Cu-doped niobium phosphate ( x Cu/NbP; x = 0.1–5.0 wt%, denoted as Cu loading) catalysts with different Cu loadings were prepared by impregnation and reduction, which could catalyze furfural conversion to levulinic acid through a one pot single-step process. The as-prepared x Cu/NbP catalysts were characterized by H 2 -TPR, XRD, NH 3 -TPD, XPS, the pore size and pore volume and pyridine-adsorption FT-IR. In this study, the effect of Cu loading, formic acid amount, support type, reaction temperature/time and catalyst reusability on the reaction were investigated. It was found that 1.5 wt% Cu/NbP loading exhibited predominant catalytic activity in the cascade conversion of furfural, producing levulinic acid with a high yield of up to 67.0 mmol% using ten equivalent of formic acid at 160 °C for 3 h. Moreover, the possible mechanism was further elucidated. Also, the catalyst could be easily separated from the mixture, and reused with no remarkable loss of reactivity.
研究领域:
生物质化学
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催化科学
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产品关联
DOI
高影响因子
FUEL
·
2022
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IF 8.035
Yao Liu,Feiyi Chen,Junhua Zhang,Liang He,Lincai Peng
Acid treatment is the key to improve the physicochemical properties of metal-lignocellulosic hybrid, thus contributing to the catalytic performance for catalytic transfer hydrogenation (CTH) of carbonyl compounds to their corresponding alcohols. Herein, a series of organic acids were introduced to assist the design of Zr- Pennisetum sinese hybrid. Comprehensive studies demonstrated the dramatic changes of specific surface and acid/base sites of the prepared hybrid. Remarkably, formic acid-assisted Zr@ PS -FA possessed the largest surface area and enhanced interaction effects between acids (Lewis acid and Brønsted acid) and Lewis base sites, which exhibited excellent catalytic activity for CTH of levulinic acid to γ-valerolactone with a high yield of 95.6% in isopropanol under moderate reaction conditions (180 °C and 1.5 h). Zr@ PS -FA also showed remarkable cycle stability, and it could be consecutively used at least six runs without a significant loss in catalytic activity. More gratifyingly, Zr@ PS -FA displayed a superior universality for CTH of various carbonyl compounds to their corresponding alcohols, demonstrating great potential for upgrading biomass-derived aldehydes/ketones.
研究领域:
化学工程
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生物质能
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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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2022
·Vol. 12
·期 11
·1361
·
IF 4.501
Wenli Feng,Xuebin Lu,Jian Xiong,Zhihao Yu,Yilin Wang,Jianguo Cui,Rui Zhang,Rengui Weng
Three common solid wastes (waste incineration fly ash, sewage sludge, and polluted soil) were the raw materials used in the synthesis of a geopolymer–type zeolite–like product, which was then used as a catalyst carrier to prepare a nickel hydrogenation catalyst for the catalytic hydrogenation of levulinic acid to γ–valerolactone. Under optimum synthesis conditions, the synthesized geopolymer zeolite has excellent structure and performance. The characterization results show that the composites have a three–dimensional network structure, and the pore structure is homogeneous mesoporous or microporous. In this work, the results of catalytic hydrogenation show that the yield of γ–valerolactone can achieve up to 94% using the synthesized catalyst, which is comparable to that of commercial catalysts and the concentrations of typical polluting heavy metals of Cu, Zn, Pb, and Cd in the reaction solution were all below the emission concentration limit (Class I standard) after five cycles of reaction. In summary, this geopolymer–type zeolite–like catalyst is cheap and has excellent performance; it is, therefore, expected to be widely used in catalysis instead of commercial carriers.Keywords:geopolymer–type zeolite–like catalyst;levulinic acid;hydrogenation
研究领域:
催化材料科学
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环境工程
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化学工程
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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2022
·
IF 16.744
Yanlin Liu,Zhen Yu,Guangming Lu,Wanding Chen,Zixian Ye,Yueran He,Zhaobin Tang,Jin Zhu
Bio-based dynamic covalent thermosets have attracted extensive attention as they are expected to break conventional thermosets' reliance on fossil resources and address the recycling issue after disposal. However, there has always been a contradiction between using bio-based feedstocks and possessing high properties, as well as a conflict between high performance and rapid recycling (reprocessing and degradation). In this work, a simple approach was developed to prepare bio-based thermosets with high performance, rapid reprocessing, high flame retardancy, and antibacterial properties enabled by in-situ generated dynamic covalent imine (Schiff base) bonds and multiple hydrogen bonds. The levulinic acid epoxy (ELA) was successfully synthesized and cured with 2-(4-aminophenyl)-1H-benzimidazol-5-amine (BIA) containing benzimidazole structures. The high concentration of Schiff bases and multiple hydrogen bonds of ELA-BIA endowed it with high glass transition temperature and mechanical properties, as well as satisfactory catalyst-free malleability, rapid reprocessing and repairing. Furthermore, due to the combined effect of the in-situ Schiff base and benzimidazole structure, ELA-BIA exhibited excellent condensed phase char formation ability, resulting in intrinsic flame retardancy with a limiting oxygen index of 33.8 % and a UL-94 V-0 rating, both of which were significantly higher than 4, 4′-diaminodiphenyl methane (DDM) cured ELA or DDM cured bisphenol A epoxy. Moreover, the Schiff bases bonded in the networks provided 100 % of the intrinsic antibacterial rates. This work provides a feasible and simple strategy for the preparation of high-performance and versatile bio-based dynamic covalent thermosets.
研究领域:
材料科学
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绿色化学
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产品关联
DOI
高影响因子
ChemCatChem
·
2023
·Vol. 15
·期 5
·e202201274
·
IF 4.5
Shengbin Shi,Wenting Wu,Panli Liu,Guomin Xiao
Graphical Polymeric ionic liquids for conversion of cellulose into levulinic acid : A high levulinic acid yield of 79.4 % was achieved when used cellulose as substrates and sulphonic acid-functionalized polymeric ionic liquids as catalyst. Sulphonic acid-functionalized polymeric ionic liquids (PILs) were synthesized and applied into catalytic conversion of cellulose into levulinic acid (LA). The structure, thermal stability, and Hammett acidity function (H 0 ) of PILs were characterized and all were more thermostable than those of small-molecular ionic liquids (IL). At the optimum reaction conditions, the LA yield was maximized to 79.4 % by catalyst [Pim]CH 3 SO 3 . More importantly, catalyst [Pim]CH 3 SO 3 performed well in other biomass conversion, such as cellobiose, starch and rice husk. The product LA can be easily extracted by methyl isobutyl ketone from the reaction mixture. The PILs with high catalytic activity were easily recycled with an LA yield up to 68.9 % even after five cycles. These sufficient PILs will offer new approaches for transforming biomass to platform chemicals.
研究领域:
化学工程
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材料科学
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绿色化学
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生物质利用
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产品关联
DOI
高影响因子
RENEWABLE ENERGY
·
2022
·
IF 8.634
Rulu Huang,Huai Liu,Junhua Zhang,Yuan Cheng,Liang He,Lincai Peng
Design catalytic materials with high Lewis acid/base sites for catalytic transfer hydrogenation (CTH) of levulinic acid (LvA) to γ-valerolactone (GVL) is highly demanded but challenging. Herein, we report a concept of metal ion-polymer hybridization to design a tea polyphenol (TP) and HfCl 4 co-doped polyacrylonitrile (PAN) nanofiber (Hf@PAN-TP) via electrospinning technique . Comprehensive characterization revealed the well coordination between hafnium ions and phenolic hydroxyl groups of TP on PAN fiber, which promoted the formation of Lewis acid and Lewis base sites. As expected, a satisfactory GVL yield of 99.1% with 100% of LvA conversion was obtained using isopropanol as a hydrogen donor at 170 °C in 5 h, and the catalytic activity remained unchanged for five cycles. The kinetic study revealed the lower activation energy for CTH of LvA to GVL (33.5 kJ/mol), demonstrating the outstanding GVL formation rate of 3383.9 μmol/g . h. Based on the systematical combine of catalyst characterization and catalytic behavior, the structure-function relationship and reaction mechanism were proposed. More gratifyingly, Hf@PAN-TP was applicable for catalytic reduction of various carbonyl compounds, demonstrating a great potential for upgrading biomass-derived aldehydes/ketones.
研究领域:
材料科学
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催化化学
✓ 已验证
DOI
高影响因子
ACS Sustainable Chemistry & Engineering
·
2025
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IF 7.3
Wenjing An,Weiping Yang,Liqing Shi,Kejiang Qian,Huichao Suo,Peipei Ma,Tingzhao Xin,Jinhao Liu,Shuangxi Liu,Lan-Lan Lou,Kai Yu
Catalytic conversion of levulinic acid (LA) to γ-valerolactone (GVL) is one of the key reactions of biomass utilization, but the relatively high reaction temperature and H2 pressure always introduce safety and energy consumption issues. In this work, a photocatalytic transfer hydrogenation method was applied to achieve the hydroconversion reaction from LA to GVL under green and mild conditions using non-noble metal Bi2S3 materials as the catalyst. Up to 74.8% GVL yield and 76.3% selectivity can be achieved after 36 h of irradiation using the spherical Bi2S3 as the catalyst and isopropanol as the hydrogen source, which is significantly higher than any reported results on non-noble metal photocatalysts. The structural characterization and density functional theory calculation results indicated that the appropriate band position and lower adsorption energy toward LA rendered the spherical Bi2S3 catalyst highly reactive. Based on the results of electron paramagnetic resonance and density functional theory calculations, a reasonable photocatalytic transfer hydrogenation reaction pathway of LA to GVL was proposed. Bi2S3-photocatalyzed dehydrogenation of isopropanol generates H radicals, which react with LA adsorbed on the surface of Bi2S3 to form GVL through a hydrogenation-esterification process. The presence of Bi2S3 greatly promotes the adsorption of LA and reduces the energy barrier for LA hydrogenation.
研究领域:
化学工程
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可再生能源
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催化科学
✓ 已验证
产品关联
DOI
高影响因子
CARBON
·
2024
·
IF 10.5
Hao Wen,Fubin Ma,Haoyang Li,Yi Yue,Jiacheng Luo,Ruiyang Qu,Hepeng Zhang,Yueling Cao
Fabrication of metal/porous carbon catalysts with high catalytic activity and stability is highly desirable but challenging because the metal nanoparticles in these catalysts cannot have both high exposure and strong interaction with carbon support. Here, for the first time, a facile CO 2 -assisted one-pot pyrolysis (CAOP) strategy was developed to in situ liberate the inaccessible Ru sites without obviously affecting the size of Ru nanoparticles . The Ru@CN-700-80 prepared with the assistance of CO 2 exhibits a remarkable improvement in catalytic activity for levulinic acid hydrogenation compared with that without CO 2 during pyrolysis, giving a TOF of 28449 h −1 under mild conditions, which is superior to the reported Ru-based catalysts. Additionally, the Ru@CN-700-80 also demonstrates an excellent stability without activity loss after 10 cycles. We anticipate that this CAOP strategy addresses a crucial issue that currently plagues the design of metal/porous carbon catalyst with high catalytic performance applied in energy and environmental fields.
研究领域:
催化
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化学工程
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材料科学
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）