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Synergistic catalysis of sulfate ionic liquids and FeCl3 for the dehydration of 1,4-butanediol to tetrahydrofuran

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Fuel 2024年 363卷

作者： Wang, Ziyi Luo, Cong Wang, Binshen Lai, Tong Hong, Yang Gao, Guohua State Key Laboratory of Molecular & Process Engineering Shanghai Key Laboratory of Green Chemistry and Chemical Processes School of Chemistry and Molecular Engineering East China Normal University 3663 North Zhongshan Road Shanghai200062 China Institute of Eco-Chongming 20 Cuiniao Road Shanghai202162 China Institute of New Energy and Low-Carbon Technology Sichuan University Sichuan Chengdu610207 China

Tetrahydrofuran is a widely used bulk chemical in both laboratory and industry. In this study, a homogeneous catalytic system composed of sulfate ionic liquids and FeCl3 was applied for the synthesis of tetrahydrofuran by the dehydration of 1,4-butanediol with a high yield of 89.2%. Kinetic studies showed that the reaction rate constant (k) of the dehydration of 1,4-butanediol catalyzed by the combination of 1-ethyl-3-methylimidazolium ethyl sulfate ionic liquid ([EMIm][EtSO4]) and FeCl3 was significantly higher than that of [EMIm][EtSO4] or FeCl3 as catalyst alone. Besides, the activation energy (Ea) of this reaction over [EMIm][EtSO4] and FeCl3 was lower than either of them as catalyst. Higher reaction rate constant and lower Ea indicated that [EMIm][EtSO4] and FeCl3 had a synergistic catalytic effect. Mechanism studies showed that 1-ethyl-3-methylimidazolium hydroxybutyl sulfate ionic liquid [EMIm][HO-BuSO4], generated by the transesterification of [EMIm][EtSO4] with 1,4-butanediol over FeCl3, acted as an active species to synergistically catalyze the dehydration reaction of 1,4-butanediol with FeCl3. Density functional theory (DFT) calculations demonstrated the synergistic catalytic mechanism of [EMIm][HO-BuSO4] and FeCl3, and revealed that the intramolecular nucleophilic attack was the rate-determining step of the dehydration reaction. Continuous reactive distillation of 1,4-butanediol showed [EMIm][EtSO4] and FeCl3 could be used continuously for 54 h with the TON of 182 without any loss in activity. The catalysts also exhibited good substrate generality in the dehydration of various diols to cyclic ethers. © 2024 Elsevier Ltd

关键词： Ionic liquids

Unraveling the Effect of Sorbitol on Cu-Based Catalysts for the Continuous Hydrogenation of Co2-Derived Ethylene Carbonate to Methanol and Ethylene Glycol

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SSRN 2025年

作者： Song, Tong-Yang Zhang, Ji-Zheng Chen, Xian-Lang Huang, Xin-Yuan Jia, Ai-Ping Li, Xiaohong Li, Rong-Rong Lu, Ji-Qing Key Laboratory of the Ministry of Education for Advanced Catalysis Materials Zhejiang Key Laboratory for Reactive Chemistry on Solid Surfaces Institute of Physical Chemistry Zhejiang Normal University Jinhua321004 China Engineering Research Center of Recycling & Comprehensive Utilization of Pharmaceutical and Chemical Waste of Zhejiang Province School of Pharmaceutical and Chemical Engineering Taizhou University Zhejiang Taizhou318000 China State Key Laboratory of Petroleum Molecular & Process Engineering Shanghai Key Laboratory of Green Chemistry and Chemical Processes ECNU Engineering Center for Sustainable Carbon School of Chemistry and Molecular Engineering East China Normal University Shanghai200062 China Zhejiang Normal University China

The hydrogenation of ethylene carbonate (EC) is a crucial step in the indirect transformation of CO2 into methanol (MeOH) and ethylene glycol (EG) over Cu-based catalysts. In this work, a series of sorbitol-modified Cu/SiO2 catalyst were prepared and tested for continuous hydrogenation of EC. As a result, the MeOH selectivity displayed a volcano-like trend with the sorbitol/Cu molar ratios. The optimized Cu@0.04Cs/SiO2 catalyst exhibited excellent MeOH selectivity (91.4%) and EG selectivity (99.6%) at an EC conversion of 99.9%. The results showed that copper-sorbitol complexes were preferentially formed, which could restrict the formation of copper phyllosilicate. However, a strong electronic interaction between copper and carbon, as confirmed by multiple characterizations, which may lead to possible formation of Cu-O-C bond located on the periphery of copper and carbon interface. This interfacial effect not only reduces the activation energy but also effectively enhances the Cu+/(Cu0 + Cu+) ratios, and thus improves the selectivity to MeOH. Furthermore, according to DFT calculation and kinetic study results, the interface between copper and carbon serves as active sites to facilitate the adsorption of H2 and EC, resulting in reduced activation energy. © 2025, The Authors. All rights reserved.

关键词： Activation energy

Based on Peg Composite Phase Change Material for Efficient Solar Sustainable Seawater Desalination

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SSRN 2024年

作者： Dong, Weixiong Cao, Xulei Wang, Yaoyao Tao, Haiyan Jia, Shuping Meng, Guihua Xinjiang Key Laboratory of Novel Functional Materials Chemistry College of Chemistry and Environmental Sciences Kashi University Kashi844000 China College of Chemistry and Chemical Engineering Shihezi University State Key Laboratory of Green Process of Chemical Industry Shihezi Xinjiang832003 China Shihezi University China

To solve the problem that current solar thermal conversion materials cannot run continuously under intermittent solar radiation. The phase-change energy storage material polyethene glycol (PEG) is cleverly introduced into the interfacial evaporation material, polyacrylic acid (PAA) hydrogel is used as the leakproof support material to stabilize the PEG form, graphene oxide (GO) and nano silver (Ag NPs) are used as the solar thermal conversion medium. A novel interface evaporation three-dimensional network gel (PEG/PAA/GO-Ag) composite phase change material (PCM) was constructed by sol-gel-in-situ reduction methods. In the full spectrum range, 95.4% light absorption is achieved and matched well with the solar spectrum. Under 1 kW·m-2 sunlight, the evaporation rate of 2.14 kg·m-2·h-1 and the solar thermal conversion efficiency of 91.2% were obtained. In the absence of sunlight, the solar energy stored in PEG/PAA/GO-Ag released through the phase transition process continues to evaporate the clean water, obtaining an evaporation rate of 0.73 kg·m-2·h-1 and a solar thermal conversion efficiency of 35.0%. In addition, the material shows excellent performance stability in 10 consecutive heating and cooling cycle evaporation tests, which not only possess good cyclic stability but also can be used for saltwater desalination and dye wastewater purification. © 2024, The Authors. All rights reserved.

关键词： Conversion efficiency

Inclusion Complexation of Catechins by Hyperbranched Cyclodextrin: Preparation, Characterization, Stability, Antioxidant Properties, and Antimicrobial Properties

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SSRN 2024年

作者： Zhao, Qingsheng Chena, Fengyang Tang, Xia Sheng, Qinghai Zhu, Yuan Li, Hang Yang, Baoru State Key Laboratory of Biochemical Engineering China College of Bioscience and Engineering Hebei University of Economics and Business Shijiazhuang050061 China College of Food Science and Technology Hebei Agriculture University Baoding071001 China Key Laboratory of Biopharmaceutical Preparation and Delivery Engineering Institute of Process Engineering Chinese Academy of Sciences Beijing100190 China Department of Life Technologies Faculty of Technology University of Turku FI-20014 Finland

Catechin (C) is a flavonoid natural polyphenol with a variety of biological activities;however, it has a poor solubility, stability and oral bioavailability, which greatly limits its application in food and medical fields. Hyperbranched cyclodextrin (CDP) has the advantages of hyperbranched polymer network structure and cyclodextrin macrocyclic basic backbone, which can provide a strong contact between the two components to effectively improve the properties of catechin molecule. In this study, catechin/hyperbranched cyclodextrin inclusion complex (Catechin/CDP IC) and catechin/β-cyclodextrin inclusion complex (Catechin/β-CD IC) were prepared by freeze-drying method at a molar ratio of 1:1. The embedding efficiency (CE) of the two inclusion complexes were 83. 85%, and 64. 85% . The structural characterization was carried out via FT-IR, DSC and 1H NMR analyses. Furthermore, the results of solubility, thermal stability, storage stability, sustained-release characteristics, antioxidant capacity and antibacterial ability of catechin complexed with CDP were better than that complexed with β-CD. © 2024, The Authors. All rights reserved.

关键词： Solubility

Unraveling the Effect of Sorbitol on Cu-Based Catalysts for the Continuous Hydrogenation of Co2-Derived Ethylene Carbonate to Methanol and Ethylene Glycol

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SSRN 2025年

关键词： Activation energy

Enhancing antibiotic removal of mixed matrix membranes through electrostatic surface segregation of MIL-101(Fe) catalysts

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Chemical engineering Journal 2025年 505卷

作者： Zheng, Xia Yang, Zhaomei Zeng, Guangyong Lin, Qingquan Chen, Xi Xiang, Yuan Chiao, Yu-Hsuan Gonzales, Ralph Rolly Low, Ze-Xian Luo, Jianquan State Key Laboratory of Geohazard Prevention and Geoenvironment Protection Chengdu University of Technology Sichuan Chengdu610059 China College of Materials and Chemistry & Chemical Engineering Chengdu University of Technology Sichuan Chengdu610059 China Department of Mathematical & Physical Sciences Chengdu University of Technology Sichuan Chengdu610059 China Research Center for Membrane and Film Technology Kobe University Kobe6578501 Japan Scion Private Bag 3020 Rotorua3046 New Zealand State Key Laboratory of Materials-Oriented Chemical Engineering National Engineering Research Center for Special Separation Membrane Nanjing Tech University Nanjing210009 China State Key Laboratory of Biochemical Engineering Institute of Process Engineering University of Chinese Academy of Sciences Chinese Academy of Sciences Beijing100190 China

Introducing Fenton-like catalysts into mixed matrix membranes offers two significant advantages— it addresses challenges related to catalyst recovery and reuse while integrating membrane technology with catalytic processes for enhanced pollutant removal. However, achieving a uniform distribution of catalysts within the membrane and maintaining catalytic activity post-blending remains challenging. In this study, positively charged chitosan (CS)-modified MIL-101(Fe) photo-Fenton-like catalysts were incorporated into the casting solution, while negatively charged polyacrylic acid (PAA) was dissolved in the coagulation bath. During the non-solvent induced phase separation (NIPS) of the membrane, the combined effects of hydrophilicity and electrostatic interactions facilitated the migration of MIL-101(Fe) towards the membrane surface, boosting the peroxymonosulfate (PMS) catalytic activity of MIL-101(Fe) for antibiotic degradation. The developed CS@MIL-101(Fe)-PAA/PVDF/PMS/Vis system achieved high removal ratio against tetracycline hydrochloride (TCH) (>99 %), broad working pH range (1–9), and excellent long-term operational stability. Density functional theory (DFT) calculations revealed that PMS exhibited a higher affinity toward the ternary structure, and the activation reaction was thermodynamically favorable and spontaneous. This study offers a novel strategy for the rational design of nanomaterial-based catalytic membranes, bridging the gap between photocatalysis and heterogeneous catalysis, and providing new insights for aquatic environment remediation. © 2025 Elsevier B.V.

关键词： Surface segregation

在TiO_(2)@C/Fe_(2)O_(3)纳米片阵列上电还原硝酸根制氨:揭示水热碳的影响

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Science China Materials 2023年第11期66卷 4367-4376页

作者：吴璇马爱静刘丹李雪倩周颖康 Alex T.Kuvarega Bhekie B.Mamba 李虎桂建舟 State Key Laboratory of Separation Membranes and Membrane Processes School of Material Science and TechnologyTiangong UniversityTianjin 300387China Tianjin Key Laboratory of Green Chemical Technology and Process Engineering School of Chemical Engineering and TechnologyTiangong UniversityTianjin 300387China School of Chemistry Tiangong UniversityTianjin 300387China Institute for Nanotechnology and Water Sustainability College of ScienceEngineering and TechnologyUniversity of South AfricaFlorida 1709JohannesburgSouth Africa Ningxia Coal Industry Co. Ltd.CHN ENERGYYinchuan 750011China

电化学硝酸根还原制氨(NRA)可以同时实现硝酸盐废水处理和氨合成,是一种很有前途的环保节能策略.目前构建高效的电催化剂是人们关注的焦点.本文构建了TiO_(2)@C/Fe_(2)O_(3)纳米片阵列作为高效催化剂,采用多种表征手段系统研究了水热碳... 详细信息

电化学硝酸根还原制氨(NRA)可以同时实现硝酸盐废水处理和氨合成,是一种很有前途的环保节能策略.目前构建高效的电催化剂是人们关注的焦点.本文构建了TiO_(2)@C/Fe_(2)O_(3)纳米片阵列作为高效催化剂,采用多种表征手段系统研究了水热碳的引入对NRA性能的影响.我们发现水热碳既可作为良导体实现电荷的快速传递,又可作为还原剂引入更多的氧空位,实现了“一石二鸟”催化剂构建策略.与TiO_(2)/Fe_(2)O_(3)相比,TiO_(2)@C/Fe_(2)O_(3)具有更高的NRA性能,硝酸盐转化率为88.6%、氨选择性为83.4%、法拉第效率为85.3%、氨收率为0.2176 mmol h^(-1)cm^(-2).此外,在9次循环实验后,TiO_(2)@C/Fe_(2)O_(3)的高活性仍得以保持,证实了TiO_(2)@C/Fe_(2)O_(3)出色的稳定性.此外,我们利用电化学准原位电子自旋共振实验、电化学原位衰减全反射傅立叶变换红外测量和在线差分电化学质谱法推导了可能的NRA反应途径.这种引入水热碳中间层的策略可为开发新型NRA电催化剂开辟新的途径.

关键词： ammonia electrocatalysis nitrate TiO_(2) hydro-thermal carbon

Co-Pyrolysis Mechanism of Pp and Pet Under Steam Atmosphere

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SSRN 2023年

作者： Song, Kuntong Li, Yi Wang, Nan Hou, Wenxia Zhang, Ruiqi Liu, Junhong Zhou, Qing Lu, Xingmei Beijing Key Laboratory of Ionic Liquids Clean Process CAS Key Laboratory of Green Process and Engineering State Key Laboratory of Multiphase Complex Systems Institute of Process Engineering Chinese Academy of Sciences Beijing100190 China Sino Danish College University of Chinese Academy of Sciences Beijing100049 China School of Chemical Engineering University of Chinese Academy of Sciences Beijing100049 China Henan Institute of Advanced Technology Zhengzhou University Zhengzhou450001 China

The pyrolysis of polyethylene terephthalate (PET) under steam atmosphere is an effective method for reducing impurities and improving the yield of terephthalic acid (TPA). However, the yield is still low compared to the theoretical maximum. Here, further improvements were achieved through the steam-assisted co-pyrolysis of PET and polypropylene (PP). The results showed that the presence of PP inhibits the excessive cracking of PET and promotes the complete cracking of PP to gaseous products. The optimal reaction temperature was found to be 450 °C, with a maximum yield of TPA of 85.0 wt%, representing an increase compared to the pyrolysis of pure PET. Further, a large amount of olefin monomer was obtained, and the proportion of carbon dioxide in the gaseous products was reduced to 47.7 vol%, which not only improves the efficiency of resource recovery but also reduces carbon emissions. The reaction mechanism of the co-pyrolysis was also explored through analysis of the products in the co-pyrolysis process and by comparing the measured data with theoretical predictions. It was noticed that TPA has a promoting effect on the pyrolysis of PP. This is mainly because TPA is a highly thermally stable Bronsted acid, which can still provide the acidic catalytic site when PP was thermally decomposed during the co-pyrolysis process. Further, a new hydrogen transfer reaction pathway between PP and PET was discovered via isotope tracing experiments, with density functional theory simulations by Material Studio indicating that this pathway occurs between the active hydrogen on the methyl group of PP and the hydrogen on the benzene ring of PET. This study demonstrates that the monomer yield can be improved through the co-pyrolysis of mixed plastics under steam atmosphere, which has important implications for industrial waste plastic recycling applications. © 2023, The Authors. All rights reserved.

关键词： Pyrolysis

Silver modified Cu/SiO2 catalyst for the hydrogenation of methyl acetate to ethanol

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Chinese Journal of Chemical engineering 2020年第6期28卷 1612-1622页

作者： Zhiheng Ren Muhammad Naeem Younis Hui Zhao Chunshan Li Xiangui Yang Erqiang Wang Gongying Wang Chengdu Institute of Organic Chemistry Chinese Academy of SciencesChengdu 610041China National Engineering Laboratory for VOCs Pollution Control Material&Technology University of Chinese Academy of SciencesBeijing 101408China CAS Key Laboratory of Green Process and Engineering State Key Laboratory of Multiphase Complex SystemsThe National Key Laboratory of Clean and Efficient Coking TechnologyBeijing Key Laboratory of Ionic Liquids Clean ProcessInstitute of Process EngineeringChinese Academy of SciencesBeijing 100190China Zhongke Langfang Institute of Process Engineering Langfang 065000China Zhongke Langfang Institute of Process Engineering Zhengzhou 450000China School of Chemical Science University of Chinese Academy of SciencesBeijing 100049China

A series of silver modified Cu/SiO2 catalysts were synthesized with ammonia-evaporation method and applied in vapor-phase hydrogenation of methyl acetate to *** influence of additive‘Ag’on the structural evolution of catalyst was systematically studied by several characterization techniques,such as N2 adsorption–desorption,N2O titration,PXRD,FTIR,in-situ FTIR,H2-TPR,H2-TPD,XPS and *** showed that incorporation of a small amount of Ag could enhance the structural stability,and the strong interaction between Cu and Ag species was conducive to increase the dispersion of copper species and create a suitable Cu+/(Cu0+Cu+)ratio,which was proposed to be responsible for the improved catalytic *** maximum conversion of MA(94.1%)and selectivity of ethanol(91.3%)over optimized Cu-0.5 Ag/SiO2 and 120 h on stream without deactivation under optimal conditions demonstrates its excellent stability.

关键词： Copper Silver Hydrogenation Methyl acetate Ethanol Kinetic