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Design of Dual Stimuli-Responsive Copolymerized Ionic Liquid with Flexible Phase Transition Temperature and Its Application in Selective Separation of Artemisitene/Artemisinin

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ACS SUSTAINABLE CHEMISTRY & ENGINEERING 2023年第11期11卷 4463-4472页

作者： Cao, Yingying Wang, Yaofeng Chen, Bingtong Zhu, Yiwei Wang, Hui Chinese Acad Sci Beijing Key Lab Ion Liquids Clean Proc CAS Key Lab Green Proc & Engn State Key Lab Multiphase Complex SystInst Proc En Beijing 100190 Peoples R China Univ Chinese Acad Sci Coll Chem Engn Beijing 100049 Peoples R China

Smart materials are a kind of material which can respond to subtle changes in the environmental conditions, and their use in chemical processes is becoming increasingly widespread. In this work, stimuli-responsive copolymerized ionic liquids (ILs) were designed to ease the recycling of IL, and they were prepared by free radical polymerization of isopropylacrylamide and 1-methyl-3-(4-vinylbenzyl)imidazolium chloride. The turbidity point temperature (for phase transition) of the copolymerized IL aqueous solution can be precisely controlled by varying the IL concentration in the copolymerized IL, adding inorganic salt, and changing the salt content. It was demonstrated that the introduction of IL increased the interaction between the copolymerized IL and water, resulting in higher turbidity point temperature of the copolymerized IL than that of polyisopropylacrylamide. The addition of salt weakened the electrostatic shielding and increased the cation-pi interaction, resulting in particle agglomeration and precipitation of the copolymerized IL. Moreover, the copolymerized IL aqueous solution exhibited excellent performance for selective separation of artemisitene/artemisinin (ARE/ ART), two structural analogues. The separation selectivity of ARE/ART increased with the increase of IL content in the copolymerized IL, reaching 3.62 for the copolymer containing 11.25 mol % IL. Additionally, the copolymerized IL can be easily recycled by the dual stimuli response of heating and addition of salt.

关键词： copolymerized ionic liquid dual stimuli responsiveness structural analogue separation cation-pi interaction recycling

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Generation features and kinetics of gas products in bio-tar catalytic cracking by char for biomass gasification

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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY 2023年第82期48卷 31905-31919页

作者： Zeng, Xi Shen, Mengjie Wang, Fang Ma, Xiaohong Hu, Dandan Wang, Tingting Cui, Yanbin Beijing Technol & Business Univ Sch Ecol & Environm Beijing 100048 Peoples R China Chinese Acad Sci State Key Lab Multiphase Complex Syst Inst Proc Engn Beijing 100190 Peoples R China

This research focused on the reaction features and kinetics of tar catalytic conversion by char based on the generation and evolution of gas products. To probe the roles of heat and catalysis in tar conversion, a micro fluidized bed reaction analyzer (MFBRA) was used to assess tar thermal cracking (TC) and catalytic cracking (CC) by char at 1073, 1123, 1173, and 1223 K. The tar cracking behavior of the individual gas components (H2, CO, CO2, and CH4), generation rates, and reaction kinetics were thoroughly investigated. The results show that TC and CC included a fast (Stage-1) and slow (Stage-2) conversion stage, in which Stage-1 contributed more than 80% of the total conversion. Compared to TC, tar CC required a longer reaction time but obtained higher conversions to individual gas components and the total gas products. The final conversion ratios (XCC/TC) of H2, CO, CO2, and CH4 were kept above 1 at the tested temperature. The char catalytic action was very remarkable, especially at low temperatures. In tar CC, the generation rate of individual gas components slowly declined after quickly reaching the peak, forming a relatively stable zone. The volume reaction model (VRM) well described the tar conversion behavior with and without char. Compared to TC, char lowered the activation energy (Ea) of gas generation. For individual gas components (H2, CO, CO2, CH4) and the total gas products, the corresponding reduction degree of Ea was 25.56%, 24.18%, 22.14%, 4.75%, and 21.71%, respectively, further displaying the promoting impact of char. The evaluated generation features and kinetics of individual components in the gas products will benefit the in-situ tar removal in the biomass gasification process. & COPY;2023 Hydrogen Energy Publications LLC. Published by Elsevier Ltd. All rights reserved.

关键词： Biomass gasification Tar Catalytic cracking Char Fluidized bed Kinetics

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Germanium doping effect on the photoelectronic performance of alternating cations in the interlayer space GA(MA)3(Pb1-xGex)3I10

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JOURNAL OF MATERIALS CHEMISTRY A 2024年第27期12卷 16466-16475页

作者： Sun, Ping-Ping Yuan, Shuai Chi, Weijie Cai, Guilong Hainan Univ Sch Chem & Chem Engn Haikou 570228 Peoples R China Chinese Acad Sci Inst Proc Engn Beijing Key Lab Ion Liquids Clean Proc State Key Lab Multiphase Complex SystCAS Key Lab Beijing 100190 Peoples R China Henan Univ Zhengzhou Inst Emerging Ind Technol Longzihu New Energy Lab Zhengzhou 450000 Peoples R China

The perovskite solar cells (PSCs), based on the two-dimensional (2D) perovskites stabilized by alternating cations in the interlayer space (ACI), have recently received remarkable attention due to the impressive power conversion efficiency (PCE) exceeding 18%. Pursuing ways to alleviate the toxicity of lead has emerged as a hot topic in the community of PSCs. Herein, we investigate potential alternatives to ACI 2D GA(MA)(3)Pb3I10 perovskites by replacing lead with germanium (Ge) of various compositions using first-principles calculations. We demonstrate the pivotal role of Ge doping in finely adjusting the bandgap, enhancing broad-emission features, and improving Stokes shifts and Huang-Rhys factors. Fabricating GA(MA)(3)(Pb1-xGex)(3)I-10 candidates, especially within the range from 8.3% to 50% Ge content, demonstrate minor energy level offsets at the conduction band minimum adjacent to the electron transport layer. Significantly, GA(MA)(3)(Pb0.083Ge0.917)(3)I-10 exhibits the strongest carrier transport ability, with the highest electron mobility of 2492.9 cm(2) V-1 s(-1). Moreover, compositions ranging from 8.3% to 75% exhibit improved optical-electronic properties and photovoltaic response compared to GA(MA)(3)Pb3I10, with GA(MA)(3)(Pb0.75Ge0.25)(3)I-10 and GA(MA)(3)(Pb0.667Ge0.333)(3)I-10 standing out with PCE values exceeding 22%, positioning them as promising photo-absorber candidates for photovoltaic applications. Our findings provide valuable insights into the significant role of Ge doping in shaping the distinctive photoelectronic properties of ACI 2D GA(MA)(3)(Pb1-xGex)(3)I-10 perovskites, thereby paving the way for innovative approaches to advance their applications in optoelectronics.

关键词： Perovskite

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Phase transfer-based high-efficiency recycling of precious metal electrocatalysts

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Green Chemical Engineering 2024年第1期5卷 68-74页

作者： Qing Zeng Shaonan Tian Yu Zhang Hui Liu Dong Chen Xinlong Tian Chaoquan Hu Jun Yang State Key Laboratory of Multiphase Complex Systems Institute of Process EngineeringChinese Academy of SciencesBeijing100190China State Key Laboratory of Marine Resource Utilization in South China Sea Hainan Provincial Key Lab of Fine ChemistrySchool of Chemical Engineering and TechnologyHainan UniversityHaikou570228China Nanjing IPE Institute of Green Manufacturing Industry Nanjing211100China Center of Materials Science and Optoelectronics Engineering University of Chinese Academy of SciencesBeijing100049China

Recycling precious metals with high-efficiency is undoubtedly beneficial to optimize resource utilization for environmental remediation and sustainable ***,we report an efficient route to recycle the palladium(Pd)and platinum(Pt)electrocatalysts using a phase transfer *** strategy involves acidic dissolution of deactivated precious metal(Pd/Pt)electrocatalysts from their loading substrates,mixing with an ethanolic solution of dodecylamine(DDA),subsequent extraction of metal ions into a non-polar organic phase,and final reduction by sodium borohydride to reproduce high-performance electrocatalysts towards typical electrochemical reactions,e.g.,oxygen reduction reaction(ORR)and ethanol oxidation reaction(EOR).In specific,the transfer efficiencies are up to 98%and the final recovery rate is over 85%for Pd and Pt electrocatalysts in each *** approach symbolizes a facile and efficient way to recover precious metals,which might be applied to recycling a wide range of metals in various realms after appropriate modifications.

关键词： Precious metal Phase transfer Extraction Recovery Electrocatalyst

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Dynamic breakthrough performance of low concentration CO2 adsorption in fixed-bed column with porous amino acid ionic liquid composites

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SEPARATION AND PURIFICATION TECHNOLOGY 2024年 349卷

作者： Li, Bowen Zeng, Shaojuan Jiang, Chongyang Li, Guilin Bai, Lu Xu, Fei Zhang, Xiangping Zhengzhou Univ Henan Inst Adv Technol Zhengzhou 450051 Peoples R China Chinese Acad Sci Beijing Key Lab Ion Liquids Clean Proc State Key Lab Multiphase Complex Syst Inst Proc Engn Beijing 100190 Peoples R China Univ Chinese Acad Sci Beijing 100049 Peoples R China

Low concentration carbon dioxide (CO2) capture from air or confined spaces currently faces significant challenges, such as relatively poor dynamic adsorption breakthrough performance and cyclic stability. In our previous work, functionalized ionic liquid (IL) tetraethylammonium glycine ([N2222][Gly]) and porous molecular sieve (SBA-15) were combined to synthesize porous amino acid IL composite 60 wt% [N2222][Gly]@SBA-15 with microporous and ultra-microporous structures, which provide a new pathway for low concentration CO2 capture. In order to further obtain the dynamic CO2 adsorption breakthrough performance of this material under simulated actual working conditions, the effects of temperatures, relative humidity (RH) and CO2 concentrations on CO2 adsorption and desorption breakthrough performance of 60 wt% [N2222][Gly]@SBA-15 in a fixed-bed column were systematically studied in this work. The results indicated that CO2 adsorption capacity is up to 1.81 mmolCO2/g-adsorbent at 298.15 K, 1 bar and 0 % RH under 1 vol% CO2-containing gas mixture balanced with N2 and reaches 2.44 mmolCO2/g-adsorbent at 15 % RH due to the mechanism change of CO2 reaction with primary amine from 2: 1 under dry gas to 1: 1 stoichiometry in the presence of moisture. Moreover, the adsorbent maintains good cyclic adsorption-desorption performance. Further, CO2 adsorption breakthrough behaviors were well fitted by Avrami kinetic model, and the CO2 adsorption rate of 60 wt% [N2222][Gly]@SBA-15 was controlled by intra-particle diffusion. This work implied that IL-modified adsorbents have great potentials for low concentration CO2 capture applications.

关键词： CO 2 capture Porous ionic liquid composites Low CO 2 concentration Adsorption kinetics Fixed -bed column

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Ionic liquids: a novel material for efficient nanofiltration membranes

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CURRENT OPINION IN CHEMICAL ENGINEERING 2025年 47卷

作者： Xiao, Luqi Cui, Jinfeng Shan, Linglong Zhang, Xiangping Chinese Acad Sci Inst Proc Engn CAS Key Lab Green Proc & Engn State Key Lab Multiphase Complex SystBeijing Key Beijing 100190 Peoples R China China Univ Petr Coll Chem Engn & Environm State Key Lab Heavy Oil Proc Beijing 102249 Peoples R China Univ Sci & Technol China Sch Rare Earths Hefei 230026 Peoples R China Chinese Acad Sci Ganjiang Innovat Acad Ganzhou 341000 Peoples R China

Ionic liquids (ILs) have recently emerged as a new membrane material for efficient separation. In this review, current achievements of nanofiltration (NF) membranes modified by ILs are highlighted. ILs, comprising cations and anions, possess excellent tunability of functionalized groups, high polarity, high chargeability, good antimicrobial properties, low vapor pressure, and eco-friendly characteristics, which can enhance the hydrophilicity and chargeability of the NF membrane, provide additional water transport channels and water transport efficiency, as well as improve the ion selectivity, antifouling, and antibacterial properties of the NF membrane for green and sustainable separation process. Meanwhile, the challenges and future research interests toward the interaction behavior between ILs and targeted substance, the regulation of membrane surface interface properties, the separation mechanism, and the inadequacies of s-based NF membranes are discussed.

关键词： Nafion membranes

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Mass Transfer Characteristics of CO2 and Blended Aqueous Solutions of [C2OHmim][Lys]/MDEA in a Microchannel

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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH 2023年第22期62卷 8926-8938页

作者： Xu, Zhenbin Wang, Tingting Wu, Jianmeng Wang, Lulu Zhang, Xiangping Dong, Haifeng Sun, Changyu China Univ Petr State Key Lab Heavy Oil Proc Beijing 102249 Peoples R China Chinese Acad Sci Inst Proc Engn Beijing Key Lab Ion Liquids Clean Proc State Key Lab Multiphase Complex Syst Beijing 100190 Peoples R China Adv Energy Sci & Technol Guangdong Lab Huizhou 516227 Guangdong Peoples R China

Inthis paper, the two-phase flow and mass transfer process ofCO(2) and [C(2)OHmim]-[Lys]/MDEA mixed aqueous solutionin a T-shaped microchannel were investigated systematically. By usinga high-speed camera connected to a computer, the two-phase flow patternswere recorded online, including the Taylor flow and a small amountof Taylor-bubbly flow. And the effects of ionic liquid concentrationand two-phase flow ratio (Q (G)/Q (L)) on bubble length, specific surface area, gas holdup,and mass transfer coefficient were studied experimentally. The resultsindicate that the blended solution of [C(2)OHmim]-[Lys]/MDEAcould significantly enhance two-phase mass transfer compared to single N-methyldiethanolamine aqueous solution. The reaction mechanismbetween CO2 and ionic liquid/amine mixed aqueous solutionwas also analyzed. On the basis of experimental data, some new correlationsfor predicting the bubble initial length and the volumetric mass transfercoefficient were proposed, which matched well with the experimentaldata. This work is helpful to provide new ideas for the design ofCO(2) absorbents and further improve the data of gas-liquidmass transfer in microchannels.

关键词： Absorption Bubbles Liquids Mass transfer Solvents

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Smart ionic liquid/water mixture system with dual stimuli-response to temperature and CO_(2)

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Nano Research 2023年第3期16卷 4152-4159页

作者： Xiaoqing Yuan Ju Liu Jingyu Qin Weili Ma Guangyong Liu Yanlei Wang Hongyan He Beijing Key Laboratory of Ionic Liquids Clean Process State Key Laboratory of Multiphase Complex SystemsCAS Key Laboratory of Green Process and EngineeringInstitute of Process EngineeringChinese Academy of SciencesBeijing 100190China University of Chinese Academy of Sciences Beijing 100049China Innovation Academy for Green Manufacture Chinese Academy of SciencesBeijing 100190China

Stimuli-responsive materials have important applications in chemistry and chemical ***,we synthesized five different polyetheramine-fatty acids(PEFA)ionic liquids(ILs),possessing the dual stimuli-responsive ability to temperature and CO_(2).These PEFA ILs have reversible lower critical solution temperature(LCST)phase behavior over a wide temperature range of 37-91℃,and reversible heterogeneous-homogeneous phase transition towards the addition and removal of CO_(2).Furthermore,the droplet size of the IL-water mixture system increased from 6.5 to 21.0 nm as the temperature increased from 25 to 56℃,and then recovered to 6.5 nm when the temperature decreased to 25℃.The addition and removal of CO_(2)also reversibly modulated the droplet size of the *** from nuclear magnetic resonance(NMR)and Fourier transform infrared(FTIR)spectra further showed that the temperature-dependent conformation of polyether amine chain in the cation dominates the temperature response,while the reversible formation of bicarbonate and fatty acids(FA)from CO_(2)and anion controls the CO_(2)-based reversible phase *** simulations revealed a microscopic response mechanism of the IL-water system to temperature and CO_(2),and a synergistic effect between the dual stimuli of temperature and CO_(2).These findings may provide a basis for the rational design and understanding of ILs-based stimuli-responsive materials and nanoreactors.

关键词： stimuli-responsive ionic liquids phase transitions temperature CO_(2)

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Anions mediated electron-rich metalloporphyrin ionic framework as recyclable catalyst for conversion of urea into cyclic carbonates

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JOURNAL OF MOLECULAR LIQUIDS 2024年 399卷

作者： Deng, Lili Su, Qian Ding, Weilu Liu, Shuaifei Li, Zengxi Cheng, Weiguo Univ Chinese Acad Sci Sch Chem Sci Beijing 100049 Peoples R China Chinese Acad Sci Beijing Key Lab Ion Liquids Clean Proc State Key Lab Multiphase Complex Syst CAS Key Lab Green Proc & EngnInst Proc Engn Beijing Peoples R China Henan Univ Sch Chem & Chem Engn Kaifeng 475001 Peoples R China

As CO2 typical derivative, urea has the potential to be uniquely economical and green raw materials in generating cyclic carbonates via alcoholysis. Nonetheless, the existing processes for obtaining cyclic carbonates from urea alcoholysis reaction pose considerable challenges in achieving efficient catalyst recycling. Functional organic heterogeneous compounds are emerging materials for catalysis and enhanced reusability due to their large number of coordination sites, but they still fall short of effectively modulating the charge distribution of metal ions. Herein, drawing inspiration from the capacity of ionic liquids (ILs) to effectively control the distribution and transfer of spatial charges within materials, metalloporphyrin ionic framework catalysts were developed by combining metal ions and ILs for the transformation of urea into cyclic carbonates. This heterogeneous catalyst, featuring an adjustable structure and stable metal coordination sites on its surface, exhibits remarkable stability, resulting in a 2.7-fold reduction in catalyst dosage compared to other reported supported catalysts. Based on detailed experiments and DFT calculations, this tunable performance can be mainly explained by the effect of porphyrin zinc (II) and IL anions via molecular engineering. These atom-economical transformations provide a direct and selective access to valuable compounds from cheap and available urea using an efficient organic heterogeneous catalyst.

关键词： Metalloporphyrin ionic framework Ionic liquids Urea alcoholysis Cyclic carbonates

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Effect of MnO2 Morphology on Kinetics and Stability in Zinc-Ion Batteries

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ACS APPLIED MATERIALS & INTERFACES 2023年第23期15卷 28044-28054页

作者： Gao, Ning Song, Yang Li, Chang Hu, Chaoquan Zhongke Nanjing Inst Green Mfg Ind Nanjing 211135 Jiangsu Peoples R China Chinese Acad Sci Inst Proc Engn State Key Lab Multiphase Complex Syst Beijing 100190 Peoples R China

Researchon zinc-ion batteries (ZIBs) with manganese-based cathodeshas been severely hindered by their poor cycle stability. This studyexplores the fundamental parameters that affect the cycle stabilityof battery systems from a structural stability perspective. MnO2 electrodes with different classical morphologies and sizeswere synthesized via a temperature-controlled coprecipitation *** effects of the morphology and size of the MnO2 on theoverall electrical properties and kinetics of ZIBs were analyzed andcompared. The one-dimensional nanofibrous alpha-MnO2 producedusing this method exhibited the most stable nanostructure with a favorableaspect ratio, which resulted in faster chemical kinetics. A more uniformparticle distribution and better aspect ratios not only enabled afaster ion migration rate but also affected the remolding of the anodemorphology. After 2000 cycles at a high current density of 1 A g(-1), the material maintained an excellent discharge-specificcapacity, highlighting it as a promising electrode material for *** construction of nanoenergy materials with controllable morphologiesand sizes will significantly advance battery applications.

关键词： zinc-ion batteries MnO2 coprecipitationmethod chemical kinetics Zn dendrites

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