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Construction of multifunctional lanthanum manganese mixed nanoparticles mediated by ionic liquids for selective aerobic oxidation of cyclohexane

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Rare Metals 2024年第5期43卷 2205-2221页

作者： Hao Li Rui-Rui Zhang Ke-Xin Li Shuang Wei Yu-Mei Liu Rui-Xia Liu Beijing Key Laboratory of ionic liquids Clean Process CAS Key Laboratory of Green Process and EngineeringState Key Laboratory of Multiphase Complex SystemsInstitute of Process EngineeringChinese Academy of SciencesBeijing 100190China University of Chinese Academy of Sciences Beijing 100049China

Selective oxidation of alkanes to produce highvalue chemicals is an essential strategy and means to realize efficient utilization of *** this work,a strategy of lanthanum manganese mixed metal oxides(LMMO)regulated via a facile ionic liquid(IL)-assisted hydrothermal method was proposed to construct the multifunctional catalysts,which exhibited excellent catalytic performance in the selective aerobic oxidation of *** 8.9%cyclohexane conversion with 90%KA oi(cyclohexanol and cyclohexanone)selectivity was achieved over the optimal LMMO catalyst under mild *** effects of anion type,carbon chain length and concentration of ILs on the structure and properties of catalysts were investigated through various characterizations,indicating the structure-directing and template effect of ILs on the multifunctional *** formation of self-assembled spherical nanoparticles followed the"dissolution-nucleation-proliferation"mechanism with the introduction of 1-butyl-3-methylimidazolium hydrogen sulfate,ascribing the synergistic effect between the microenvironment of ILs and the hydrothermal ***,the high reactive oxygen concentration redox capacity,and suitable basic sites of LMMO catalysts mediated by ILs enhance the activation of C-H bonds and molecular oxygen,simultaneously influencing the adsorption and desorption of the substrate.A comprehensive understanding of the high KA oil selectivity and radical reaction mechanism was elucidated based on in situ diffuse reflectance infrared Fourier transform spectroscopy(DRIFTS)and radical trapping *** recycling and regeneration experiments further illuminated that the removal of adsorbed cyclohexanone acting on the LMMO catalyst was the key to achieve high KA oil selectivity.

关键词： ionic liquids Nanoparticle Multifunctional catalyst Cyclohexane oxidation

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Solvent effects on Diels-Alder reaction in ionic liquids:A reaction density functional study

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Chinese Journal of Chemical Engineering 2024年第2期66卷 180-188页

作者： Zijiang Dou Weiqiang Tang Peng Xie Shuangliang Zhao Guangxi Key Laboratory of Petrochemical Resource Processing and Process Intensification Technology and School of Chemistry and Chemical Engineering Guangxi UniversityNanning 530004China State Key Laboratory of Chemical Engineering and School of Chemical Engineering East China University of Science and TechnologyShanghai 200237China

Extensive experimental studies have been performed on the Diels-Alder(DA)reactions in ionic liquids(ILs),which demonstrate that the IL environment can significantly influence the reaction rates and ***,the underlying microscopic mechanism remains *** this work,the multiscale reaction density functional theory is applied to explore the effect of 1-butyl-3-methylimidazolium hexafluorophosphate([BMIM][PF_(6)])solvent on the reaction of cyclopentadiene(CP)with acrolein,methyl acrylate,or *** analyzing the free energy landscape during the reaction,it is found that the polarization effect has a relatively small influence,while the solvation effect makes both the activation free energy and reaction free energy *** addition,the rearrangement of local solvent structure shows that the cation spatial distribution responds more evidently to the reaction than the anion,and this indicates that the cation plays a dominant role in the solvation effect and so as to affect the reaction rates and selectivity of the DA reactions.

关键词： Solvent effect ionic liquids Diels-Alder reaction Reaction density functional theory

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Application status and prospect of ionic liquids in oilfield chemistry

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Petroleum 2024年第1期10卷 11-18页

作者： Jinsheng Sun Zhuoyang Xiu Li Li Kaihe Lv Xianfa Zhang Zonglun Wang Zhiwen Dai Zhe Xu Ning Huang Jingping Liu School of Petroleum Engineering China University of Petroleum (East China) CNPC Engineering Technology R&D Company Limited Oil & Gas Technology Research Institute of Changqing Oilfield Company

The ionic liquid, as a new treatment agent, has been increasingly applied in oil fields due to its strong temperature resistance, good solubility and high surface activity. In this paper, we systematically discuss the action mechanism and application effect of ionic liquids in oilfield chemistry. ionic liquids can inhibit shale hydration expansion and reduce fluid loss through adsorption and intercalation, inhibit the formation of natural gas hydrate through imidazole five-membered ring structure as a space barrier, reduce viscosity of heavy oil by breaking chemical bonds of heavy oil macromolecules and charge transfer,improve oil displacement efficiency by forming ions pairs with carboxyl groups in crude oil, demulsify by forming channels between dispersed water droplets, acidify the formation by reacting with water to produce acid, interacts with organic material through weak hydrogen bonds and extracts it from oilfield wastewater, desulphurize by inserting sulfide molecules into the “stack” structure and form liquid inclusion complex, inhibit corrosion by forming a protective film on the metal surface. Based on the above aspects, the development direction of ionic liquids is proposed. The application of ionic liquids in oilfield chemistry is still in its infancy. It is urgent to fully explore the application performance of ionic liquids in oilfield chemistry, which also provides theoretical and technical supports for efficient reservoir development.

关键词： ionic liquids Oilfield chemistry Shale inhibitor Drilling fluid

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Intelligent solubility estimation of gaseous hydrocarbons in ionic liquids

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Petroleum 2024年第1期10卷 109-123页

作者： Behnaz Basirat Fariborz Shaahmadi Seyed Sorosh Mirfasihi Abolfazl Jomekian Bahamin Bazooyar Ahvaz Faculty of Petroleum Engineering Petroleum University of Technology (PUT) School of Engineering & Physical Sciences Heriot Watt University Department of Fluids & Environment The University of Manchester Department of Engineering Chemical Engineering Group Esfarayen University of Technology Mechanical and Aerospace Engineering Brunel University London

The research focuses on evaluating how well new solvents attract light hydrocarbons, such as propane,methane, and ethane, in natural gas sweetening units. It is important to accurately determine the solubility of hydrocarbons in these solvents to effectively manage the sweetening process. To address this challenge, the study proposes using advanced empirical models based on artificial intelligence techniques like Multi-Layer Artificial Neural Network(ML-ANN), Support Vector Machines(SVM), and Least Square Support Vector Machine(LSSVM). The parameters for the SVM and LSSVM models are estimated using optimization methods like Genetic Algorithm(GA), Particle Swarm Optimization(PSO), and Shuffled Complex Evolution(SCE). Data on the solubility of propane, methane, and ethane in various ionic liquids are collected from reliable literature sources to create a comprehensive database. The proposed artificial intelligence models show great accuracy in predicting hydrocarbon solubility in ionic liquids. Among these, the hybrid SVM models perform exceptionally well, with the PSO-SVM hybrid model being particularly efficient computationally. To ensure a comprehensive analysis, different examples of hydrocarbons and their order are included. Additionally, a comparative analysis is conducted to compare the AI models with the thermodynamic COSMO-RS model for solubility analysis. The results demonstrate the superiority of the AI models, as they outperform traditional thermodynamic models across a wide range of data. In conclusion, this study introduces advanced artificial intelligence algorithms such as ML-ANN, SVM, and LSSVM in accurately estimating the solubility of hydrocarbons in ionic liquids. The incorporation of optimization techniques and variations in hydrocarbon examples improves the accuracy, precision, and reliability of these intelligent models. These findings highlight the significant potential of AI-based approaches in solubility analysis and emphasize their superiori

关键词： Solubility Gaseous hydrocarbon Intelligent models ionic liquids

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A systematic COSMO-RS study on mutual solubility of ionic liquids and C6-hydrocarbons

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Green Chemical Engineering 2024年第1期5卷 97-107页

作者： Chuxin Qi Zhen Song Hongye Cheng Lifang Chen Zhiwen Qi State Key Laboratory of Chemical Engineering School of Chemical EngineeringEast China University of Science and Technology130 Meilong RoadShanghai200237China

When considering the usage of ionic liquids(ILs)for reactions and separations involving non-polar or weak-polar hydrocarbons,the knowledge of the mutual solubility behaviors of ILs and hydrocarbons is of the utmost *** this work,taking four typical C6-hydrocarbons namely benzene,cyclohexene,cyclohexane,and hexane as representatives,the mutual solubility of ILs and non-polar or weak-polar hydrocarbons are systematically studied based on the COSMO-RS *** reliability of COSMO-RS for these systems is first evaluated by comparing experimental and predicted hydrocarbon-in-IL activity coefficient at infinite dilution and binary/ternary liquid-liquid equilibria of related ***,the mutual solubility of the four hydrocarbons and13,650 ILs(composed by 210 cations and 65 anions)are *** effect of different IL structural characteristics including alkyl chain length,cation family/symmetry/functional group,and anion on the IL-hydrocarbon mutual solubility behaviors are further analyzed by the analyses of interaction energy and screen charge *** mutual solubility databases and the structural effects identified thereon could provide useful guidance for IL selection in related applications.

关键词： C6-hydrocarbons ionic liquids Mutual solubility COSMO-RS Structural effect analysis

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ionic liquids as boundary additives in water-based and PAO lubricants

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Friction 2022年第9期10卷 1405-1423页

作者： Wahyu WIJANARKO Hamid KHANMOHAMMADI Nuria ESPALLARGAS Norwegian Tribology Center Department of Mechanical and Industrial EngineeringNorwegian University of Science and Technology(NTNU)Trondheim 7491Norway Department of Mechanical Engineering Sepuluh Nopember Institute of Technology(ITS)Surabaya 6011Indonesia

ionic liquids have been widely discussed as potential lubricants,however,their properties make them also very good potential candidates as lubricant additives(e.g.,friction modifiers and anti-wear).In this work,the tribological study of two ionic liquids(tributylmethylphosphonium dimethylphosphate(PP),and 1-butyl-1-methylpyrrolidinium tris(pentafluoroethyl)trifluorophosphate(BMP))as lubricant additives has been performed on stainless steel(AISI 316L)exposed to polar(water-glycol)and non-polar(polyalphaolefin)based lubricants under boundary lubricating *** performance of these ionic liquids as lubricant additives has been compared to a classical organic friction modifier(dodecanoic acid(C12)).The water–glycol lubricant formulated with the two ionic liquids showed friction values higher than the same base lubricant formulated with dodecanoic acid,however,opposite results were observed for polyalphaolefin(PAO).A detailed surface chemical analysis using X-ray photoelectron spectroscopy(XPS)revealed differences in the passive/tribofilm thickness and chemical composition of the stainless steel surface tested in all *** the case of the polar lubricant additivated with ionic liquids,the tribochemical reaction accompanied by a tribocorrosion process led to the formation of an unstable passive/tribofilm resulting in high friction and ***,in the absence of tribocorrosion process(polyalphaolefin base lubricant),the tribochemical reaction led to the formation of a stable passive/tribofilm resulting in low friction and wear.A detailed surface and subsurface investigation of the microstructure using scanning electron microscopy equipped with a focused ion beam(SEM-FIB)showed that high wear rates resulted in thicker recrystallization region under the wear track *** all lubricant additives tested in this work,BMP in non-polar lubricant media showed the best tribological performance.

关键词： water lubricant polyalphaolefin(PAO) ionic liquids tribochemistry tribocorrosion tribofilm

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ionic liquids in transdermal drug delivery system: Current applications and future perspectives

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Chinese Chemical Letters 2023年第3期34卷 113-121页

作者： Yang Zhang Chao Liu Jiaqi Wang Shoujun Ren Yilin Song Peng Quan Liang Fang Department of Pharmaceutical Sciences Shenyang Pharmaceutical UniversityShenyang 110016China

The transdermal drug delivery(TDD) shows considerable advantages over other administration ***, conventional enhancing permeation methods face a series of challenges owing to barrier function provided by the skin, of which enhancing abilities either are so strong that it results in toxicity and irritation, or too weak to achieve desirable therapeutical effects. To address these issues, it is an urgent need to develop a novel method to overcome the limitations of current measures. Fortunately, in the preceding decades, ionic liquids(ILs) have been extensively studied and increasingly applied in pharmaceutical drug delivery due to their unique physicochemical and biological properties. What is more, tunability of structure resolves the challenges in processing active pharmaceutical ingredient(API) formulation, such as polymorphism and poor solubility of drugs. Thus, the presence of ILs provides an ample design space for the transdermal drug delivery system(TDDS). This review discusses the shortcomings of conventional enhancing permeation methods and introduces the application of ILs in transdermal delivery from three aspects: i) ILs are applied as enhancers to weaken the barrier function of the stratum corneum(SC). ii) As counterions, ILs are combined with API to modify the physicochemical properties of drugs. iii) ILs assist in the design of transdermal preparation for perfecting formulation. This review comprehensively introduces the major breakthroughs made in the applications of ILs, which can serve as guidance to provide novel ideas for formulation scientists who hit the bottleneck in the development of TDD.

关键词： TDD ionic liquids Skin Permeation enhancers Physicochemical properties

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A simple hydroxypyridine ionic liquids for conversion of CO_(2)into quinazoline-2,4(1H,3H)-diones under atmospheric conditions

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Chinese Journal of Chemical Engineering 2023年第10期62卷 217-224页

作者： Bowen Jiang Meiling Weng Jigang An Yuewei Fan Jia Liu Ying Liu Ting Yu Leizhi zheng Guoqiang Yang Zhibing Zhang School of Chemistry and Chemical Engineering Nanjing UniversityNanjing 210093China School of Materials Science and Engineering Suzhou University of Science and TechnologySuzhou 215009China

The transformation of CO_(2)into high value-added product is a promising pathway for utilizing CO_(2).However,the process tends to require harsh reaction conditions owing to CO_(2)chemical *** a high efficiency catalytic system with environmentally benign characteristic are important *** this work,protic ionic liquids[TMG][2-OPy]were prepared via one-step neutralization between 1,1,3,3-tetramethylguanidine and 2-hydroxypyridine,applying to the domain of synthesizing quinzoline-2,4(1 H,3H)-diones from CO_(2)and 2-aminobenzontiles without any solvent or metal,achieving the yield of 97%at 90℃for 8 h under atmospheric.A series of substrates with good to acceptable yield were detected,revealing the generality and universality of the ***,the system could be facilely reused for at least six runs,retaining the yield of 94%.A preliminary kinetic equation is calculated with the activation energy of 68 kJ·mol^(-1),and a plausible reaction mechanism was put *** study highlights that the[TMG][2-OPy]enables to activate CO_(2)carboxylation efficiently.

关键词： CO_(2)conversion Homogeneous catalyst ionic liquids Reaction kinetic

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Separation of isopropyl alcohol+isopropyl acetate azeotropic mixture:Selection of ionic liquids as entrainers and vapor-liquid equilibrium validation

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Chinese Journal of Chemical Engineering 2022年第10期50卷 326-334页

作者： Lianzheng Zhang Jie Wang Lin Yang Dongmei Xu Yixin Ma Jun Gao Yinglong Wang College of Chemical and Biological Engineering Shandong University of Science and TechnologyQingdao 266590China College of Chemical Engineering Qingdao University of Science and TechnologyQingdao 266042China

Based on the COSMO-SAC model,1-ethyl-3-methylimidazolium acetate and 1-ethyl-3-methylimidazolium p-toluenesulfonate were selected from 30 ILs as entrainers to investigate the separation of the isopropyl alcohol+isopropyl acetate *** screening indicators,σ-profile and infinite dilution selectivity(S^(∞)),were adopted as the *** iso baric vapor-liquid equilibrium experiments for isopropyl alcohol+isopropyl acetate binary system and isopropyl alcohol+isopropyl acetate+confirmed ILs ternary systems were performed at the pressure of atmospheric *** experimental measurement demonstrated that the adopt ILs enhanced the relative volatility of the above alcohol-ester azeotrope,leading to the elimination of the azeotropic point with a certain amount ***,the thermodynamic correlation for two systems containing ILs was explored with the NRTL model,which also reflects the extensive applicability of that by comparing the deviation between experimental and calculated *** its binary interaction parameters were regressed,which can provide a basis for its simulation process.

关键词： Vapor-liquid equilibrium ionic liquids NRTL Alcohol-ester azeotrope COSMO-SAC model

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Engineering of hollow polymeric nanosphere-supported imidazolium-based ionic liquids with enhanced antimicrobial activities

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Nano Research 2022年第6期15卷 5556-5568页

作者： Yu Zhang Shuwei Li Yixin Xu Xinyun Shi Mingxin Zhang Yingning Huang Ying Liang Yaqiong Chen Wanli Ji Jung Rae Kim Wenliang Song Deng-Guang Yu Il Kim School of Pharmacy Shanghai University of Medicine&Health SciencesShanghai 201318China School of Materials Science&Engineering University of Shanghai for Science and TechnologyShanghai 200093China Department of Polymer Science and Engineering Pusan National UniversityBusan 46241Republic of Korea School of Chemical and Biomolecular Engineering Pusan National UniversityBusan 46241Republic of Korea

The design of stable,efficient and processable bactericidal materials represents a significant challenge for combating multidrugresistant bacteria in a variety of engineering ***,we report a facile strategy for the preparation of hollow polymeric nanosphere(HPN)-supported imidazolium-based ionic liquids(denoted as HPN-ILs)with superior antimicrobial *** were tailored by moderate Friedel−Crafts polymerization followed by the sequential covalent bonding of imidazole and *** resultant HPN-ILs have uniform hollow spherical morphology,an adequate surface area,and excellent physicochemical ***,they are highly active against both Gram-positive and Gram-negative bacteria and exhibit typical time/dosage-dependent antibacterial *** rational combination of porous HPNs and antibacterial ILs to generate an all-in-one entity may open new avenues for the design and fabrication of efficient bacteriostatic ***,HPN-ILs have good biocompatibility and can also be loaded onto diverse matrices,and thus could extend their practical bactericidal application in the potential biomedical-active field.

关键词： antibacterial materials bioactive materials hollow nanospheres ionic liquids porous polymers

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