CHEMISTRY-A EUROPEAN JOURNAL
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2023
·Vol. 29
·期 52
·e202300950
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IF 4.3
Fukun Li,Ronghe Yang,Zheng Tian,Ziting Du,Jinhang Dai,Xingmin Wang,Ning Li,Jie Zhang
Graphical Microwave-assisted one pot cascade transformation of furfural to γ-valerolactone catalyzed by Sc(OTf) 3 . γ-Valerolactone (GVL) is considered as a star biochemical which can be used as a green solvent, fuel additive and versatile organic intermediate. In this study, metal triflate (M(OTf) n ) was utilized as the catalyst for one-pot transformation of furfural (FF) to GVL in alcohol media under microwave irradiation. Alcohol plays multiple functions including solvent, hydrogen donor and alcoholysis reagent in this cascade reaction process. And process efficiency of GVL production from FF upgrading is strongly related to the effective charge density of selected catalyst and the reduction potential of selected alcohol. Complex (OTf) n -M−O(H)R, presenting both Brønsted acid and Lewis acid, is the real catalytic active species in this cascade reaction process. Among various catalysts, Sc(OTf) 3 exhibited the best catalytic activity for GVL production. Various reaction parameters including the Sc(OTf) 3 amount, reaction temperature and time were optimized by the response surface methodology with the central composite design (RSM-CCD). Up to 81.2 % GVL yield and 100 % FF conversion were achieved at 143.9 °C after 8.1 h in the presence of 0.16 mmol catalyst. This catalyst exhibits high reusability and can be regenerated by oxidative degradation of humins. In addition, a plausible cascade reaction network was proposed based on the distribution of product.
研究领域:
化学工程
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生物化工
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产品关联
DOI
PubMed
高影响因子
EUROPEAN POLYMER JOURNAL
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2022
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IF 5.546
Xianqiang Zeng,Liguo Wang,Yan Cao,Chen Liu,Ziqiang Han,Peng He,Huiquan Li
Aliphatic polyethers are synthesized byring-opening polymerization (ROP) of the most common epoxide monomers, such as ethylene oxide (EO) and propylene oxide (PO). 1,2-Butylene oxide (BO) and tetrahydrofuran (THF) are potentially extended ROP monomers, which can give polyether unique properties. In this work, a series of poly(1,2-butylene oxide- stat -tetrahydrofuran)s (PBO- stat -PTHFs) with M n of 900–3700 g·mol −1 were synthesized by cationic ring-opening polymerization (CROP) of BO with THF using strong Lewis acid Rare Earth triflates (RE(OTf) 3 ) as catalysts and diols as an initiator at room temperature. PBO- stat -PTHFs product with yield up to 90 %, narrow polydispersity of Đ <1.30, and molar ratio of PBO to PTHF 1:1 were obtained. The copolymerization process was studied by in-situ IR and 1 H NMR spectroscopy analysis, and the results showed that PBO- stat -PTHF is a statistical copolymer. The early stage of the polymerization reaction was dominated by the activated chain end mechanism (ACEM), which incorporates a large amount of THF into the polymer chains. However, the late stage of the polymerization reaction was dominated by the activated monomer mechanism (AMM), which incorporates a large amount of BO into the polymer chains. Most PBO- stat -PTHFs have a suitable M n range, super high viscosity index (≥198) and low pour point (≤-53 °C), which can be used as a lubricant base oil and additives. In addition, PBO- stat -PTHFs have excellent miscibility with polyalphaolefin (PAO), which could significantly improve the PAO viscosity index. This study provides a mild route to construct high-performance copolyether materials through cationic ring-opening controllable polymerization.
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
Molecular Catalysis
·
2022
·
IF 5.089
Fukun Li,Ronghe Yang,Ziting Du,Jinhang Dai,Xingmin Wang,Ning Li,Jie Zhang,Xianming Zhang,Yunqi Liu,Haifeng Gong,Hong Yin,Zhenping Cai
γ-Valerolactone (GVL) is considered as a versatile platform chemical obtained from biomass refinery. In this study, eco-friendly group III metal (Sc, Y, La) triflates were examined as homogeneous catalysts for microwave-assisted transfer hydrogenation of ethyl levulinate (EL) to GVL under mild conditions. Experimental results revealed that the selectivity of GVL has a positive relationship with the Lewis acidity of metal ion, which is related to effective charge density of the metal center (3.23, 2.81, 2.60 for Sc 3+ , Y 3+ , La 3+ , respectively). The stronger Lewis acidity of metal ion, the higher catalytic activity of MPV reduction. Among these catalysts, Sc(OTf) 3 exhibited the best catalytic activity, achieving 98.4% EL conversion and 92.4% GVL yield at 140 °C in 3.0 h. Furthermore, Sc(OTf) 3 showed high stability and recyclability for at least ten reaction cycles. In addition, a plausible reaction pathway and mechanism were proposed.
研究领域:
化学工程
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催化
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可再生能源
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绿色化学
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产品关联
DOI
高影响因子
Materials Today Energy
·
2021
·
IF 7.311
Shufeng Song,Weiling Gao,Guanming Yang,Yanfang Zhai,Jianyao Yao,Liyang Lin,Weiping Tang,Ning Hu,Li Lu
Building safe and high-energy-density lithium metal batteries (LMBs) is currently being pursued to sustain our modern lifestyles. However, new electrolyte engineering is rigorously required that is capable of simultaneously providing good protection on lithium metal anode and sustaining high oxidative stability at the cathode, besides sufficient bulk conductivity and low interfacial resistance. Here, we report a novel hybrid poly-ether/carbonate ester quasi-solid-state electrolyte with high oxidative stability formed by a simple and efficient in situ polymerization of strategy, in which ring-opening polymerization of ether-based 1,3-dioxolane (DOL) and ester-based ethylene carbonate (EC)-ethylmethyl carbonate (EMC) is initiated by rare-earth triflate catalyst Sc(OTf) 3 at room temperature. Such electrolyte engineering not only achieves a sufficiently high ionic conductivity of 5 × 10 −4 S cm −1 but enables a high anodic voltage limit of 5 V while maintaining feasible battery manufacture technology. The hybrid poly-DOL/EC/EMC quasi-solid-state electrolyte is capable of producing a stable solid electrolyte interphase (SEI) featuring Li plating/stripping over 500 h at 0.5 mA cm −2 and decreased charge transfer resistance. The derived Li||LiFePO 4 quasi-solid-state LMB, benefited from the enhanced oxidative stability of electrolyte, exhibits a notable capacity of 169 mAh g −1 at 1C with no capacity decay after 300 cycles.
研究领域:
材料科学
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电化学
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能源存储
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电池技术
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产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）