Frontiers in Chemistry
·
2022
·
IF 5.545
Zhou Shuolin,Lei Min,Bai Junzhuo,Liu Xianxiang,Wu Lu,Long Min,Huang Keying,Yin Dulin
The titania nanotubes-bonded sulfamic acid (TNTs-NHSO3H) catalyst was designed and successfully fabricated by the post-synthesis modification method. The as-prepared catalyst was characterized by a variety of characterization techniques, including Fourier transform infrared (FT-IR) spectroscopy, X-ray photoelectron spectroscopy (XPS), transmission electron microscopy (TEM), scanning electron microscopy (SEM), X-ray diffraction (XRD) analysis, and thermogravimetry-differential thermal gravimetry (TG-DTG). The crystal structure of the TNTs still maintained during the modification process. Although the BET surface area was decreased, the amount of Brønsted acid sites can be efficiently fabricated on the TNTs. The catalytic activity of TNTs-NHSO3H was examined for the synthesis of n-butyl levulinate (BL) from levulinic acid (LA) and furfuryl alcohol (FA). A relatively high selectivity (99.6%) at 99.3% LA conversion was achieved for esterification of levulinic acid owing to the strong Brønsted acidity sites. And also, the TNTs-NHSO3H catalyst exhibited a higher reactivity for alcoholysis of FA and the yield of BL reached 90.4% with 100% FA conversion was obtained under the mild conditions.
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
PubMed
高影响因子
FUEL
·
2022
·
IF 8.035
Huifa Zhang,Shaolin Wang,Huixian Zhang,Lingrui Cui,Fahai Cao
Ethyl levulinate (EL), as a potential fuel additive and versatile biomass-based platform molecule, has been the focus in the field of sustainable chemistry. In this contribution, a series of economic and environmental friendly biomass-derived P doped carbon catalysts were developed in this study for synthesis of EL from renewable furfural alcohol (FAL) in a hot ethanol medium. The carbon catalyst, P-C-800, synthesized via carbonizing the phytic acid at 800 °C, exhibited a good catalytic activity in alcoholysis of FAL to EL. The highest yield of EL could be 79.7% with a complete conversion of FAL at 140 °C in 6 h. Moreover, P-C-800 could be recovered efficiently and reused multiple times with sustained catalytic activity. It was revealed further by the detailed catalyst characterization and systematic evaluation of catalytic performance that both the acid content and surface area of the P-C-800 were crucial for the alcoholysis of FAL to EL.
研究领域:
催化
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可持续化学
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生物质转化
✓ 已验证
产品关联
DOI
高影响因子
CATALYSIS TODAY
·
2022
·
IF 6.562
Ying Ji,Huifang Liu,Feng Wang,Xinwen Guo
It is a green and environment-friendly strategy to use biomass to assist the synthesis of catalysts and use the prepared catalysts for biomass utilization. In this study, aluminum-rich silicon-phosphorus-aluminum nanosheet (Al-SPAN) was synthesized with biomass amino acids as additives for catalytic transfer hydrogenation of ethyl levulinate to γ-valerolactone. Compared with commercial Al 2 O 3 , Al-SPAN showed greatly improved catalytic performance for the reaction. The conversion of ethyl levulinate was increased by 47 % and the yield of γ-valerolactone was increased by 52 %. The effects of different alcohol on the reaction properties were investigated, with isopropanol used as a safe and efficient hydrogen source. The catalyst has good stability with little change in reaction performance after five cycles.
研究领域:
化学工程
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Cleaner Production
·
2021
·
IF 9.297
Fengjiao Lai,Feng Yan,Yingqing Wang,Chunyan Li,Jianjun Cai,Zuotai Zhang
Biomass-derived carbohydrates exploited toward the synthesis of alkyl levulinates is very promising, but still limited by the applicable catalyst. In this study, novel metal/Si-pillared montmorillonite supported phosphotungstic acid catalysts (SG-HPW-XSiMt-y, where X = La 3+ , Ce 3+ , Er 3+ , Cu 2+ , Al 3+ , Ti 4+ , Zr 4+ ) were synthesized by sol-gel method. The catalytic performance of SG-HPW-XSiMt-y were comprehensively studied for glucose methanolysis to methyl levulinate (ML), focusing on the effects of metal acidity, HPW contents and reaction conditions. The appropriate Lewis acidity of metal ions effectively facilitated the isomerization of glucose/methyl-glucoside to fructose/methyl-fructoside; the strong Brønsted acidity of incorporated HPW was capable of suppressing the side reactions; and the large specific surface area and hierarchical pores of the mesoporous structure allow the reaction to take place both on surface and inside the porous framework. Among these as-synthesized catalysts, the SG-HPW-ZrSiMt-20 showed the most superior activity and achieved 65.8% yield of ML from glucose at 170 °C for 4 h. Alternative biomass-derived carbohydrates, including fructose, sucrose and cellobiose, also gave excellent ML yields under such catalytic system . The SG-HPW-ZrSiMt-20 had impressively stable reusability with merely loss of catalytic activity after eight cycles, owing to the uniform dispersion and stable bonding of HPW with ZrSiMt support. Generally, this catalyst system realizes an efficient and sustainable conversion of biomass-derived carbohydrates to ML production.
研究领域:
化学工程
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生物质能转化
✓ 已验证
产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2023
·
IF 8.2
Ran Liu,Yuanlong Guo,Min Pei,Yumei Chen,Lihua Zhang,Long Li,Qin Chen,Yaozhu Tian,Haibo Xie
Facile modification of cellulose or cellulosic derivatives is one of the important strategies to prepare materials with targeted properties, multifunctionality, thus extending their applications in various fields. Cellulose levulinate ester (CLE) has the structural advantage of acetyl propyl ketone moiety pendant, on which fully biobased cellulose levulinate ester derivatives (CLEDs) have been successfully designed and prepared via aldol condensation reaction of CLE with lignin-derived phenolic aldehydes catalyzed by DL-proline. The structure of CLEDs are featured by a phenolic α,β-unsaturated ketone structure, thus endowing them with good UV absorption properties, excellent antioxidant activity , fluorescence properties and satisfactory biocompatibility. The utility of this aldol reaction strategy, together with the facile tunable substitution degree of cellulose levulinate ester and the diversity of aldehydes, can provide potentially a large spectrum of structurally diverse functionalized cellulosic polymers and create new avenues to advanced polymeric architectures.
研究领域:
材料科学
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有机化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
FUEL
·
2023
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IF 7.4
Qiang Lu,Yuefang Chen,Weipeng Song,Chaonan Tao,Junhua Zhang,Yong Sun,Lincai Peng,Huai Liu
Direct utilization of cellulosic material to produce specialty chemicals such as levulinate ester could greatly increase biorefinery profitability, but low-level efficiency due to its structural nature limits the strategy for industrial deployment. We report herein that adding γ-valerolactone (GVL) co-solvent during the acid-catalyzed conversion of cellulose in ethanol leads to a high reaction rate and improved catalytic activity towards ethyl levulinate (EL) production. With GVL as the co-solvent (the volume ratio of GVL to ethanol in 1:4), the yield of EL highly enhanced from 31% to 56% under mild operating conditions (170 °C for 2 h) over a low loading Al(OTf) 3 of 0.005 mol/L. The mechanistic role of GVL co-solvent to accelerate EL formation from cellulose has been fully elucidated via the combination of experimental and theoretical approaches. It demonstrates that GVL intervention not only favored the dissolution and depolymerization of cellulose, but also enabled the formation of Al species with higher acidity and catalytic activity by modulating the solvation environment, both of which are in charge of promoting cellulose conversion to EL. The activation energy barriers for cellulose depolymerization and glucoside alcoholysis have decreased by 30.8 kJ/mol and 24.8 kJ/mol, respectively. The understanding of this solvation effect can be employed to optimize the rate and yield for production of the versatile bio-based ester compound straight from cellulose valorization.
研究领域:
化学工程
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可再生资源与环境科学
✓ 已验证
产品关联
DOI
高影响因子
CATALYSIS LETTERS
·
2024
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IF 2.3
He Xiangyan,Liu Huai,Wang Yue,Peng Lincai,Zhang Junhua
Effective structural design can make the catalyst have higher specific surface area and dispersed active sites, thus endowing the catalyst higher catalytic efficiency. In this work, magnetic nitrogen-doped carbon nanotube (CNT) was introduced as the support to immobilize the zirconium-based biomass-derived hybrid (Zr-FDCA) through solvothermal method, in which specific surface area had significantly increased to improve the dispersibility of zirconium, thus improving the adsorption over the catalyst to ethyl levulinate (EL). In addition, the introduced nitrogen served as the basic sites to boost the proton transfer in catalytic transfer hydrogenation (CTH) reaction. As a result, the prepared Zr-FDCA@CNT exhibited an ideal catalytic performance in CTH of EL into γ-valerolactone. Gratifyingly, Zr-FDCA@CNT also showed magnetism and good reusability, which could be easily separated from the reaction mixture and no significant loss in the activity after reuse for four runs. Graphical Abstract
Schematic for CTH of EL over Zr-FDCA@CNT
研究领域:
材料科学
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催化化学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Jun Zhang,Zihao Li,Huiyu Liu,Rui Shan,Haoran Yuan,Yong Chen
The present research firstly developed the waste lithium-ion batteries as heterogenous catalysts for catalytic upgrading of bio-based ethyl levulinate (EL) into γ-valerolactone (GVL) using 2-propanol as both the hydrogen source and solvent. The existing acid and basic sites in waste lithium-ion batteries significantly favored the MPV reduction of bio-based EL, wherein 87.4 % GVL yield and low activation energy of 35.2 kJ/mol were achieved. Furthermore, the waste lithium-ion batteries contributed to H-transfer upgrading of a variety of building blocks containing unsaturated groups, such as aldehydes and esters. More gratifyingly, the economic assessment demonstrated that EL-to-GVL transformation via H-transfer manner was preferred as compared with the traditional hydrogenation, in which the total cost for converting 1 kg EL declined by 10.58 $ and overall profit increased by 12.35 $. In addition, the plausible mechanism for H-transfer upgrading of EL into GVL over waste lithium-ion batteries was proposed.
研究领域:
化学工程
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催化科学
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可再生能源
✓ 已验证
产品关联
DOI
高影响因子
Energy Sources Part A-Recovery Utilization and Environmental Effects
·
2021
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IF 3.447
Yan Li,Weibo Wu,Hu Li,Wenfeng Zhao,Song Yang
γ-Valerolactone (GVL) is a versatile biomass-derived molecule for both value-added chemicals and biofuels, which is typically prepared from levulinates over metal particles or oxides in the presence of hydrogen, formic acid or alcohol. Herein, we reported a rapid and mild approach for cascade hydrogenation-cyclization of ethyl levulinate (EL) to GVL in the presence of readily available ionic liquid tetrabutylammonium fluoride ([TBA]F) and polymethylhydrosiloxane (PMHS) as catalyst and hydrogen source, respectively. After reacting at room temperature for 30 min, a high GVL yield of 85% with TOF value of 52 h−1 could be obtained over 3 mol% [TBA]F. In addition to optimizing reaction parameters, the catalytic mechanism was also elucidated for the one-pot sequential transformation of EL to GVL.
✓ 已验证
DOI
高影响因子
JOURNAL OF CHEMICAL TECHNOLOGY AND BIOTECHNOLOGY
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2017
·Vol. 93
·期 2
·557-568
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IF 3.135
Fengjiao Lai,Jia Luo,Dan Jiang,Tongchao Su,Fan Zhang
BACKGROUND Because of the decline in conventional sources of energy and the increasing pollution, the fossil fuel based energy structures is being replaced by renewable energy based structures such as biomass energy. Among current biodiesel sources, methyl levulinate (ML) obtained from catalytic conversion of renewable carbohydrate with methanol has received a great deal of attention. Silica-pillared montmorillonites (MMTSi) functionalized by iron-modified tungstophosphoric acid (HPWFe) were prepared, and their physicochemical properties and catalytic effects on ML production studied. RESULTS Catalysts characterization demonstrated the high dispersion and Keggin structure of HPWFe in the framework of MMTSi. Effects of various reaction parameters and catalyst recycling on the reaction performance were studied to optimize fructose conversion. With 4-HPWFe-MMTSi as the catalyst, an optimized ML yield of around 74 mol% was obtained at 180°C for 1 h, and the recovered catalyst after calcination was found to retain high activity after being reused five times. CONCLUSION The prepared HPWFe-MMTSi catalysts showed high porosity, perfect Br nsted-Lewis acidity and high thermal stability, which made their catalytic activity for fructose conversion and catalyst reusability values higher than others reported in the literature. © 2017 Society of Chemical Industry
研究领域:
化学工程
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可再生能源
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催化化学
✓ 已验证
DOI
高影响因子
ENERGY & FUELS
·
2021
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IF 3.605
Lincai Peng,Xueying Gao,Yao Liu,Junhua Zhang,Liang He
Alkyl levulinate as one kind of fuel additive and versatile biomass-based platform molecule has attracted significant interests in the field of sustainable chemistry, which can be harvested straight from furfural (FAL), an important industrial chemical derived from agricultural residues. The development of a high-efficiency and low-cost catalytic system is highly desirable toward this challenging valorization process. In this contribution, bifunctional zirconia-zeolite-supported heteropoly acid catalysts with adjustable Lewis and Brønsted acid sites were successfully designed via an in situ synthetic method and attempted to couple transfer hydrogenation and alcoholysis for one-pot conversion of FAL to alkyl levulinate. The catalyst characterization and catalytic behavior were systematically combined for insight into the structure–function relationship and reaction mechanism. Selectivity toward alkyl levulinate was found to be strongly dependent upon the distribution of acid sites. As-prepared HPMo(20)/Zr-MCM-41 with a Si/Zr molar ratio of 60 and H3[P(Mo3O10)4] (HPMo) impregnation concentration of 20 g/L was uniquely effective using isopropanol as a hydrogen donor and reaction medium, leading to a high isopropyl levulinate yield of 79.6%. This monolithic catalyst exhibited good stability and could be reused at least 5 times without any substantial change in the product yield after plain thermal regeneration.
研究领域:
催化化学
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可持续化学
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生物质转化
✓ 已验证
产品关联
DOI
高影响因子
FUEL
·
2022
·
IF 8.035
Chao Li,Jian Zhao,Huixin Tong,Xiaodong Fan,Xinjie Fang,Yuli Sha,Zhizhong Sun,Wenyi Chu
Ethyl levulinate (EL) is a key platform compound for the catalytic conversion of biomass. Ionic liquids (ILs) have attracted much attention due to their unique tunable structures and wide range of applications, a series of SO 3 H-functionalized imidazole based acidic ILs were designed and synthesized. These SO 3 H-functionalized ILs were used as the catalyst to be applied to the conversion of the wheat straw to EL. Among them, SimIL-6 exhibited good catalytic performance for the conversion of wheat straw to EL in ethanol. When the concentration of SimIL-6 was 30 mmol/L, the yield of EL could reach 20.1 wt% at 180 ℃ for 2 h. Furthermore, SimIL-6 as the catalyst was reused at least six times without significant reduction in catalytic efficiency. This work shed light on a new approach towards the full utilization of biomass and efficient degradation of biomass to EL.
研究领域:
化学工程
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生物质能
✓ 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）