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Regulating sulfur removal efficiency of fuels by Lewis acidity of ionic liquids

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Science China Chemistry 2016年第5期59卷 526-531页

作者： Yi Nie Yuxiao Dong Hongshuai Gao xiangping zhang Suojiang zhang 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 College of Chemistry and Chemical Engineering Qufu Normal UniversityQufu 273165China

It is urgent to develop a new deep desulfurization process of fuels as the environmental pollution increases seriously. In this work, a series of Lewis acidic ionic liquids （ILs） [C43MPy]Cl/nZnCl2 （n=1, 1.5, 2, 3） were synthesized and used in extraction and catalytic oxidative desulfurization （ECOD） of the fuels. The effects of the Lewis acidity of ILs, the molar ratio of H2O2/sulfur, temperatures, and different substrates including dibenzothiophene （DBT）, benzothiophene （BT） and thiophene （TS）, on sulfur removal were investigated. The results indicated that [C43MPy]Cl/3ZnCl2 presented near 100% DBT removal of model oil under conditions of 323 K, H2O2/DBT molar ratio 6：1. Kinetics for the removal of DBT, BT and TS by the [C43MPy]Cl/3ZnCl2-H2O2 system at 323 K is first-order with the apparent rate constants of 1.1348, 0.2226 and 0.0609 h-1, and the calculated apparent activation energies for DBT, BT and TS were 61.13, 60.66, and 68.14 kJ/mol from 298 to 308 K, re- spectively. After six cycles of the regenerated [C43MPy]Cl/3ZnCl2, the sulfur removal had a slight decrease. [C43MPy]Cl/ 3ZnCl2 showed a good desulfurization performance under optimal conditions.

关键词： desulfurization Lewis acidity ionic liquids extractant catalyst

Rare-earth separation based on the differences of ionic magnetic moment via quasi-liquid strategy

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Frontiers of Chemical Science and Engineering 2022年第11期16卷 1584-1594页

作者： Na Wang Fujian Li Bangyu Fan Suojiang zhang Lu Bai xiangping zhang College of Chemical and Engineering Zhengzhou UniversityZhengzhou 450001China CAS Key Laboratory of Green Process and Engineering State Key Laboratory of Multiphase Complex SystemsBeijing Key Laboratory of Ionic Liquids Clean ProcessInstitute of Process Engineering and Innovation Academy for Green ManufactureChinese Academy of SciencesBeijing 100190China Ganjiang Innovation Academy Chinese Academy of SciencesGanzhou 341000China College of Chemistry Nanchang UniversityNanchang 330031China

The separation of rare earth elements is particularly difficult due to their similar physicochemical *** on the tiny differences of ionic radius,solvent extraction has been developed as the“mass method”in industry with hundreds of stages,extremely intensive chemical consumption and large capital *** differences of the ionic magnetic moment among rare earths are greater than that of ionic ***,a novel method based on the large ionic magnetic moment differences of rare earth elements was proposed to promote the separation *** earths were firstly dissolved in the ionic liquid,then the ordering degree of them was improved with the Z-bond effect,and finally the magnetic moment differences between paramagnetic and diamagnetic rare earths in quasi-liquid system were *** the separation of Er/Y,Ho/Y and Er/Ho as examples,the results showed that Er(Ⅲ)and Ho(Ⅲ)containing ionic liquids had obvious magnetic response,while ionic liquids containing Y(Ⅲ)had no *** separation factors of Er/Y and Ho/Y were achieved at 9.0 and 28.82,*** separation via quasi-liquid system strategy provides a possibility of the novel,green,and efficient method for rare earth separation.

关键词： rare earth element different magnetic moment magnetic separation ionic liquid

Modification to solution-diffusion model for performance prediction of nanofiltration of long-alkyl-chain ionic liquids aqueous solutions based on ion cluster

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Green Energy & Environment 2020年第1期5卷 105-113页

作者： Jianguo Qian Ruiyi Yan Xiaomin Liu Chunshan Li xiangping zhang Key Laboratory of Green Process and Engineering Beijing Key Laboratory of Ionic Liquids Clean ProcessState Key Laboratory of Multiphase Complex SystemsInstitute of Process EngineeringChinese Academy of SciencesBeijing 100190China College of Chemistry and Chemical Engineering University of Chinese Academy of SciencesBeijing100049China

Mathematical modeling for nanofiltration of ionic liquids(ILs) solutions could assist to understand transfer mechanism and predict experimental values. In this work, modeling by solution-diffusion model for nanofiltration of long-alkyl-chain ILs aqueous solutions was proposed. Molecular simulations were performed to validate the existence of ion cluster in long-alkyl-chain ILs aqueous solution. Based on the results of simulations, parameters used in the solution-diffusion model were modified, such as concentration of ILs and diameter of ion *** modeling process was developed for three long-alkyl-chain ILs aqueous solutions with different concentrations(1-alkyl-3-methylimidazolium chloride: [C6 mim]Cl, [C8 mim]Cl, [C10 mim]Cl). The calculated values obtained from modified solution-diffusion model could well match the experimental values.

关键词： Solution-diffusion model Nanofiltration Long-alkyl-chain ionic liquid Molecular dynamic simulation Ion cluster

Ionic liquids for CO_(2) electrochemical reduction

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Chinese Journal of Chemical Engineering 2021年第3期34卷 75-93页

作者： Fangfang Li Francesca Mocci xiangping zhang Xiaoyan Ji Aatto Laaksonen Energy Engineering Division of Energy ScienceLuleåUniversity of TechnologyLuleå97187Sweden Department of Chemical and Geological Sciences University of CagliariMonserrato 09042Italy CAS Key Laboratory of Green Process and Engineering Beijing Key Laboratory of Ionic Liquids Clean ProcessState Key Laboratory of Multiphase Complex SystemsInstitute of Process EngineeringChinese Academy of SciencesBeijing 100190China Division of Physical Chemistry Department of Materials and Environmental ChemistryArrhenius LaboratoryStockholm UniversityStockholm 10691Sweden Center of Advanced Research in Bionanocojugates and Biopolymers “Petru Poni”Institute of Macromolecular ChemistryIasi 700469Romania State Key Laboratory of Materials-Oriented and Chemical Engineering Nanjing Tech UniversityNanjing 211816China

Electrochemical reduction of CO_(2) is a novel research field towards a CO_(2)-neutral global economy and combating fast accelerating and disastrous climate changes while finding new solutions to store renewable energy in value-added chemicals and *** liquids(ILs),as medium and catalysts(or supporting part of catalysts)have been given wide attention in the electrochemical CO_(2) reduction reaction(CO_(2) RR)due to their unique advantages in lowering overpotential and improving the product selectivity,as well as their designable and tunable *** this review,we have summarized the recent progress of CO_(2) electro-reduction in IL-based electrolytes to produce higher-value *** then have highlighted the unique enhancing effect of ILs on CO_(2) RR as templates,precursors,and surface functional moieties of electrocatalytic ***,computational chemistry tools utilized to understand how the ILs facilitate the CO_(2) RR or to propose the reaction mechanisms,generated intermediates and products have been discussed.

关键词： Carbon dioxide Ionic liquids Electro-reduction Electrolyte Electrocatalytic material Computer simulation

Revolutionary technology of low-carbon chemical processes

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National Science Review 2023年第9期10卷 15-17页

作者： Suojiang zhang xiangping zhang Chunyan Shi Ke Wang Lei Yuan Institute of Process Engineering Chinese Academy of Sciences Longzihu New Energy Laboratory Zhengzhou Institute of Emerging Industrial Technology 3. College of Energy Science and Technology Henan University

The chemical industry is one of the key sectors in *** chemical processes heavily rely on fossil fuels as energy resources and feedstocks,which inevitably emits a huge amount of *** the global initiative and actions of carbon neutrality,the energy revolution of renewable energy replacing fossil fuels is further promoted towards the ultimate goal that fossil fuels will be fully replaced in the future [1].

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Numerical simulation of CO2-ionic liquid flow in a stirred tank

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Science China Chemistry 2015年第12期58卷 1918-1928页

作者： Zailong Ouyang Di Bao Xin zhang Haifeng Dong Ruiyi Yan xiangping zhang Suojiang zhang Beijing Key Laboratory of Ionic Liquids Clean Processing State Key Laboratory of Multiphase Complex Systems Institute of Process Engineering Chinese Academy of Sciences College of Chemistry and Chemical Engineering University of Chinese Academy of Sciences

Ionic liquids(ILs) are new solvents that represent a breakthrough for absorption and conversion of CO2. However, there has been little research on the hydrodynamics of gas-IL systems in stirred tanks, and this has become a bottleneck for development of IL-based reactors. In the present study, a CO2-IL([bmim][BF4]) flow in a stirred tank was studied using computational fluid dynamics(CFD). A new drag coefficient model that is specific to a gas-ionic liquid system and a population balance model(PBM) were adopted to describe the bubble behavior, such as gas holdup and bubble size evolution, precisely. The predicted results for the total gas holdup and local Sauter diameter agree well with the experimental data. The influences of the gassing rate, agitation speed, and temperature on local gas holdup, bubble size distribution, and interfacial area for the CO2-[bmim][BF4] system were also investigated. The results of this study provide fundamental information for designing gas-IL systems for stirred tanks.

关键词： multiphase flow ionic liquids carbon dioxide stirred tank computational fluid dynamics population balance model

Estimating Hansen solubility parameters of organic pigments by group contribution methods

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Chinese Journal of Chemical Engineering 2021年第3期34卷 186-197页

作者： Markus Enekvist Xiaodong Liang xiangping zhang Kim Dam-Johansen Georgios MKontogeorgis Center for Energy Resources Engineering(CERE) Department of Chemical and Biochemical EngineeringTechnical University of DenmarkBuilding 229Søltofts Plads 229DK-2800 Kgs.LyngbyDenmark Hempel Foundation Coatings Science and Technology Centre(CoaST) Department of Chemical and Biochemical EngineeringTechnical University of DenmarkBuilding 229Søltofts Plads 229DK-2800 Kgs.LyngbyDenmark Sino-Danish Center for Education and Research(SDC) IPEUniversity of Chinese Academy of SciencesBeijing 100049China 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

The Hansen solubility parameters(HSP)are frequently used for solvent selection and characterization of polymers,and are directly related to the suspension behavior of pigments in solvent *** performance of currently available group contribution(GC)methods for HSP were evaluated and found to be insufficient for computer-aided product design(CAPD)of paints and coatings.A revised and,for this purpose,improved GC method is presented for estimating HSP of organic compounds,intended for organic *** to the significant limitations of GC methods,an uncertainty analysis and parameter confidence intervals are provided in order to better quantify the estimation accuracy of the proposed *** to other applicable GC methods,the prediction error is reduced significantly with average absolute errors of 0.45 MPa^(1/2),1.35 MPa^(1/2),and 1.09 MPa^(1/2) for the partial dispersion(δD),polar(δP)and hydrogen-bonding(δH)solubility parameters respectively for a database of 1106 *** performance for organic pigments is comparable to the overall method performance,with higher average errors forδD and lower average errors forδP andδH.

关键词： Hansen solubility parameters Group contribution method Organic pigments Computer-aided product design Parameter estimation Uncertainty analysis

Pebax/TSIL blend thin film composite membranes for CO_2 separation

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Science China Chemistry 2016年第5期59卷 538-546页

作者： Zhongde Dai Lu Bai Karoline Navik Hval xiangping zhang Suojiang zhang Liyuan Deng Department of Chemical Engineering Norwegian University of Science and TechnologyTrondheim 7491Norway Beijing Key Laboratory of Ionic Liquids Clean Process Institute of Process EngineeringChinese Academy of SciencesBeijing 100190China

In this study a thin film composite （TFC） membrane with a Pebax/Task-specific ionic liquid （TSIL） blend selective layer was prepared. Defect-flee Pebax/TSIL layers were coated successfully on a polysulfone ultrafiltration porous support with a poly- dimethylsiloxane （PDMS） gutter layer. Different parameters in the membrane preparation （e.g. concentration, coating time） were investigated and optimized. The morphology of the membranes was studied by scanning electron microscopy （SEM）, while the thermal properties and chemical structures of the membrane materials were investigated by thermo-gravimetric ana- lyzer （TGA）, differential scanning calorimetry （DSC） and Fourier transform infrared spectroscopy （FTIR）. The CO2 separation performance of the membrane was evaluated using a mixed gas permeation test. Experimental results show that the incorpora- tion of TSIL into the Pebax matrix can significantly increase both C02 permeance and CO2/N2 selectivity. With the presence of water vapor, the membrane exhibits the best CO2/N2 selectivity at a relative humidity of around 75%, where a CO2 permeance of around 500 GPU and a CO2/N2 selectivity of 46 were documented. A further increase in the relative humidity resulted in higher CO： permeance but decreased COIN2 selectivity. Experiments also show that CO2 permeance decreases with a CO2 partial pressure increase, which is considered a characteristic in facilitated transport membranes.

关键词： CO2 capture thin film composite membrane task specific ionic liquids Pebax post combustion

Machine learning models for the density and heat capacity of ionic liquid-water binary mixtures

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Chinese Journal of Chemical Engineering 2024年第9期73卷 244-255页

作者： Yingxue Fu Xinyan Liu Jingzi Gao Yang Lei Yuqiu Chen xiangping zhang School of Chemistry and Chemical Engineering Hubei Key Laboratory of Coal Conversion and New Carbon MaterialsWuhan University of Science and TechnologyWuhan 430081China Department of Chemical and Biomolecular Engineering University of Delaware150 Academy StreetNewarkDE 19716United States College of Chemical Engineering and Environment China University of PetroleumBeijing 102249China

Ionic liquids(ILs),because of the advantages of low volatility,good thermal stability,high gas solubility and easy recovery,can be regarded as the green substitute for traditional ***,the high viscosity and synthesis cost limits their application,the hybrid solvent which combining ILs together with others especially water can solve this *** with the pure IL systems,the study of the ILs-H_(2)O binary system is rare,and the experimental data of corresponding thermodynamic properties(such as density,heat capacity,etc.)are ***,it is also difficult to obtain all the data through ***,this work establishes a predicted model on ILs-water binary systems based on the group contribution(GC)*** different machine learning algorithms(ANN,XGBoost,LightBGM)are applied to fit the density and heat capacity of ILs-water binary *** then the three models are compared by two index of MAE and R^(2).The results show that the ANN-GC model has the best prediction effect on the density and heat capacity of ionic liquid-water mixed ***,the Shapley additive explanations(SHAP)method is harnessed to scrutinize the significance of each structure and parameter within the ANN-GC model in relation to prediction *** results reveal that system components(XIL)within the ILs-H_(2)O binary system exert the most substantial influence on density,while for the heat capacity,the substituents on the cation exhibit the greatest *** study not only introduces a robust prediction model for the density and heat capacity properties of IL-H_(2)O binary mixtures but also provides insight into the influence of mixture features on its density and heat capacity.

关键词： Ionic liquids Density Heat capacity Group contribution method Machine learning