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Sequence engineering in Tuning the Circularly Polarized Luminescence of Aggregation-Induced Emission-Active Heterorotaxanes

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CCS Chemistry 2024年第10期6卷 2489-2501页

作者： Zhiyong Peng Pei-Pei Jia Xu-Qing Wang Xiao-Li Zhao Hai-Bo Yang Wei Wang Shanghai Key Laboratory of Green Chemistry and Chemical Processes State Key Laboratory of Petroleum Molecular&Process EngineeringSchool of Chemistry and Molecular EngineeringEast China Normal UniversityShanghai 200062 Shanghai Center of Brain-Inspired Intelligent Materials and Devices East China Normal UniversityShanghai 200241

Based on a[2]rotaxane precursor with exchangeable pentafluorophenyl ester stoppers,a new wheelassembling approach has been successfully developed for the precise sequence control of hetero[3]rotaxanes,leading to the facile and efficient synthesis of both sequence isomers of hetero[3]*** importantly,taking advantage of the chirality retention along with the wheel-assembling process,corresponding sequence isomers of chiral AIEgenfunctionalized hetero[3]rotaxanes were further precisely ***,the resultant hetero[3]rotaxanes revealed remarkable sequencedependent aggregation-induced emission(AIE)behavior and circularly polarized luminescence performance with large dissymmetry factors up to 0.012,highlighting the great power of the newly coined sequence engineering concept in developing novel AIE-active chiroptical *** proof-ofconcept study lays the foundation for investigation of the structure-property relationships of heterorotaxanes that can further direct the rational design and precise synthesis of sequence-defined heterorotaxanes with desirable properties for practical applications.

关键词： mechanically interlocked molecules rotaxanes sequence isomerism aggregationinduced emission circularly polarized luminescence

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Self-assembly of nanoparticles at solid-liquid interface for electrochemical capacitors

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Rare Metals 2022年第11期41卷 3591-3611页

作者： Xue Li Chen Chen Qian Niu Nian-Wu Li Le Yu Bao Wang State Key Laboratory of Biochemical Engineering Institute of Process EngineeringChinese Academy of SciencesBeijing 100190China StateKey Lab of Organic-Inorganic Composites Beijing UniversityofChemicalTechnologyBeijing100029China

Self-assembly of nanoparticles at solid-liquid interface could be promising to realize the assembled functions for various applications,such as rechargeable batteries,supercapacitors,and *** review summarizes the self-assembly of the nanoparticles at solid-liquid interface according to the different driving forces of assembly,including hydrophilic-hydrophobic interactions,solvophobic and electrostatic *** be specific,the self-assembly can be divided into the following two types:surfactant-assisted self-assembly and direct self-assembly of Janus particles(inorganic and amphiphilic copolymer-inorganic Janus nanoparticles).Using the emulsion stabilized by nanoparticles as the template,the self-assembly constructed by the interaction of the nanostructure unit(including metal,metal oxide,and semiconductor,etc.)not only possesses the characteristic of nanostructure unit,but also exhibits the excellent assembly performance in electrochemistry *** application of these assemblies in the area of electrochemical capacitors is ***,the current research progress and perspectives toward the self-assembly of nanoparticles at stabilized solid-liquid interface are proposed.

关键词： Self-assembly Solid-liquid interface Driving force Electrochemical capacitors

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Molecular level understanding of CO_(2) capture in ionic liquid/polyimide composite membrane

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Frontiers of Chemical Science and engineering 2022年第2期16卷 141-151页

作者： Linlin You Yandong Guo Yanjing He Feng Huo Shaojuan Zeng Chunshan Li Xiangping Zhang Xiaochun 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 Mathematics and Physics Bohai UniversityJinzhou 121013China School of Chemical Engineering University of Chinese Academy of SciencesBeijing 100049China Zhengzhou Institute of Emerging Industrial Technology Zhengzhou 450001China

Ionic liquid(IL)/polyimide(PI)composite membranes demonstrate promise for use in CO_(2)separation ***,few studies have focused on the microscopic mechanism of CO_(2)in these composite systems,which is important information for designing new *** this work,a series of systems of CO_(2)in 1-butyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide composited with 4,4-(hexafluoroisopropylidene)diphthalic anhydride(6FDA)-based PI,6FDA-2,3,5,6-tetramethyl-1,4-phenylene-diamine,at different IL concentrations were investigated by all-atom molecular dynamics *** formation of IL regions in PI was found,and the IL regions gradually became continuous channels with increasing IL *** analysis of the radial distribution functions and hydrogen bond numbers demonstrated that PI had a stronger interaction with cations than ***,the hydrogen bonds among PI chains were destroyed by the addition of IL,which was favorable for transporting CO_(2).Furthermore,the self-diffusion coefficient and free energy barrier suggested that the diffusion coefficient of CO_(2)decreased with increasing IL concentrations up to 35 wt-%due to the decrease of the fractional free volume of the composite ***,the CO_(2)selfdiffusion coefficients increased when the IL contents were higher than 35 wt-%,which was attributed to the formation of continuous IL domain that benefitted the transportation of CO_(2).

关键词： carbon dioxide ionic liquid 6FDA-TeMPD composite membrane molecular dynamics simulation

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A Web-like Three-dimensional Binder for Silicon Anode in Lithium-ion Batteries

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Energy & Environmental Materials 2024年第1期7卷 21-27页

作者： Liyuan Li Tao Li Yifan Sha Baozeng Ren Lan Zhang Suojiang Zhang 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 School of Chemical Engineering Zhengzhou UniversityZhengzhou 450001China Langfang Green Industrial Technology Center Langfang 065001China Henan Key Laboratory of Energy Storage Materials and Processes Zhengzhou Institute of Emerging Industrial TechnologyZhengzhou 450003China

Si anode is of paramount importance for advanced energy-dense lithium-ion batteries(LIBs).However,the large volume change as well as stress generates during its lithiation-delithiation process poses a great challenge to the long-term cycling and hindering its *** this work,a composite binder is prepared with a soft component,guar gum(GG),and a rigid linear polymer,anionic polyacrylamide(APAM).Rich hydroxy,carboxyl,and amide groups on the polymer chains not only enable intermolecular crosslinking to form a web-like binder,A2G1,but also realize strong chemical binding as well as physical encapsulating to Si *** resultant electrode shows limited thickness change of merely 9%on lithiation and almost recovers its original thickness on *** demonstrates high reversible capacity of 2104.3 mAh g^(-1)after 100 cycles at a current density of 1800 mA g^(-1),and in constant capacity(1000 mAh g^(-1))test,it also shows a long life of 392 ***,this soft-hard combining web-like binder illustrates its great potential in the future applications.

关键词： anionic polyacrylamide lithium-ion batteries Si anode thickness change web-like binder

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Enhanced carbon capture with motif-rich amino acid loaded defective robust metal-organic frameworks

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Nano Research 2024年第3期17卷 2004-2010页

作者： Qi-Ye Ju Jia-Jia Zheng Li Xu Hai-Yan Jiang Zi-Qian Xue Lu Bai Yang-Yang Guo Ming-Shui Yao Ting-Yu Zhu State Key Laboratory of Multi-phase Complex Systems CAS Key Laboratory of Green Process and EngineeringBeijing Key Laboratory of Ionic Liquids Clean ProcessInstitute of Process EngineeringChinese Academy of SciencesBeijing 100190China Laboratory of Theoretical and Computational Nanoscience National Center for Nanoscience and TechnologyChinese Academy of SciencesBeijing 100190China School of Rare Earths University of Science and Technology of ChinaHefei 230026China Ganjiang Innovation Academy Chinese Academy of SciencesGanzhou 341000China University of Chinese Academy of Sciences Chinese Academy of SciencesBeijing 100049China Institute for Integrated Cell-Material Sciences Kyoto UniversityInstitute for Advanced StudyKyoto UniversityYoshidaUshinomiya-choSakyokuKyoto 606-8501Japan

The use of metal-organic frameworks(MOFs)as solid adsorption materials for carbon capture is promising,but achieving efficient and reversible adsorption with a balance of capacity and selectivity for carbon dioxide(CO_(2))over N_(2) remains a *** take full advantage of the strong channel traffic and robustness of MOFs with relatively small pores,it is highly necessary to employ a defect-engineering strategy to construct a broader channel structure that can facilitate the loading of functional motif-rich amino acids(AAs).This strategy can greatly enhance the CO_(2) adsorption performance of *** this study,motif-rich amino acids are loaded into the defective and robust porous frameworks via combined defect-engineering and post-synthetic *** defective Zr/Hf-MOF-808s modified with AAs,especially for the 18 mol%4-nitroisophthalic acid,generated defective products allowing for the loading of L-serine(L-Ser).This modification resulted in a significant improvement in both the adsorption capacity(248%improvement at 298 K,100 kPa)and the selectivity of CO_(2)/N_(2) using the ideal adsorbed solution theory(IAST),with the selectivity increasing to 120.55 and 38.27 at 15 and 100 kPa,respectively,while maintaining good cycling *** functional theory(DFT)simulation,CO_(2) temperature-programmed desorption(CO_(2)-TPD),and in situ Fourier transform infrared spectroscopy(FTIR)were further employed to have a better understanding of the enhanced CO_(2) adsorption ***,unlike the AAs loaded pristine MOF-808s that showed the best CO_(2) adsorption capacity with the loading of short and small glycine(Gly),the broadened channel size in our work enables the loading of functional motif-rich L-serine,which brings more active binding sites,improving CO_(2) adsorption.

关键词： carbon capture and storage metal-organic framework(MOF) amino acids(AAs) defect-engineering motif-rich

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Balanced Polysulfide Containment and Lithium Ion Transport in Lithium-Sulfur Batteries via Nitrogen-doped Carbon Hollow Multi-shelled Structures on Modified Separators

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Chemical Research in Chinese Universities 2024年第4期40卷 690-698页

作者： RAO Fu XIAO Qian WEI Yanze WANG Jiangyan YU Ranbo WANG Dan State Key Laboratory of Biochemical Engineering Institute of Process EngineeringChinese Academy of SciencesBeijing100190P.R.China Key Laboratory of Biopharmaceutical Preparation and Delivery Chinese Academy of SciencesBeijing100190P.R.China University of Chinese Academy of Sciences Beijing100049P.R.China Department of Physical Chemistry School of Metallurgical and Ecological EngineeringUniversity of Science&Technology BeijingBeijing100083P.R.China

Representing the next-generation technology in lithium-ion batteries,lithium-sulfur(Li-S)batteries offer increased specific energy without relying on scarce metals like nickel and cobalt,but suffer from a low practical specific energy due to poor conductivity and a short lifespan due to the shuttle effect of *** the confinement of polysulfides and the transport of lithium ions requires highly elaborate modifiers for *** multi-shelled structures(HoMSs)show promise as hierarchical mesostructures for separators,offering multiple shell layers and internal cavities that effectively inhibit polysulfide *** design of these structures is crucial to address these challenges *** this study,nitrogen-doped carbon HoMS(NC HoMS)was created using polymer templates through a precisely controlled polymerization *** featuring NC HoMS-modified separators exhibit improved capacity and cycling stability in comparison to those utilizing commercial ***,triple-shelled NC HoMS strikes a balance in polysulfide containment and lithium ion *** a sulfur loading of 6.34 mg/cm^(2),the Li-S battery can consistently complete 100 charge-discharge cycles,starting with a discharge capacity of 966.4 mA·h/g with a 75.8%capacity retention *** HoMS holds potential as the separator modifier in addressing the polysulfide shuttle problem and facilitating the Li-ion transportation for advanced Li-S batteries.

关键词： Hollow multi-shelled structure Carbon material Li-S battery Separator modification Shuttle effect

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Review on electrochemical carbon dioxide capture and transformation with bipolar membranes

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Chinese Chemical Letters 2023年第8期34卷 114-129页

作者： Jinyun Xu Guoqiang Zhong Minjing Li Di Zhao Yu Sun Xudong Hu Jiefang Sun Xiaoyun Li Wenju Zhu Ming Li Ziqi Zhang Yu Zhang Liping Zhao Chunming Zheng Xiaohong Sun School of Chemical Engineering Tianjin Key Laboratory of Green Chemical Technology and Process EngineeringState Key Laboratory of Separation Membrane and Membrane ProcessesTiangong UniversityTianjin 300387China School of Materials Science and Engineering Key Laboratory of Advanced Ceramics and Machining TechnologyMinistry of EducationTianjin UniversityTianjin 300072China Beijing Key Laboratory of Diagnostic and Traceability Technologies for Food poisoning Beijing Center for Disease Prevention and ControlBeijing 100013China Advanced Materials Research Laboratory CNOOC Tianjin Chemical Research and Design InstituteTianjin 300131China

Anthropogenic carbon dioxide(CO_(2))emission from the combustion of fossil fuels aggravates the global greenhouse *** implementation of CO_(2)capture and transformation technologies have recently received great attention for providing a pathway in dealing with global climate *** these technologies,electrochemical CO_(2)capture technology has attracted wide attention because of its environmental friendliness and flexible operating *** membranes(BPMs)are considered as one of the key components in electrochemical devices,especially for electrochemical CO_(2)reduction and electrodialysis *** create an alkaline environment for CO_(2)capture and a stable pH environment for electrocatalysis on a single *** key to CO_(2)capture in these devices is to understand the water dissociation mechanism occurring in BPMs,which could be used for optimizing the operating conditions for CO_(2)capture and *** this paper,the references and technologies of electrochemical CO_(2)capture based on BPMs are reviewed in detail,thus the challenges and opportunities are also discussed for the development of more efficient,sustainable and practical CO_(2)capture and transformation based on BPMs.

关键词： Bipolar membranes Carbon dioxide Electrochemical capture Transformation CO_(2)reduction Electrodialysis devices Water dissociation

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Constructing mesoporous CeO_(2)single-crystal particles in ionic liquids for enhancing the conversion of CO_(2)and alcohols to carbonates

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Chinese Journal of Catalysis 2024年第11期66卷 152-167页

作者： Jielin Huang Jie Wang Haonan Duan Songsong Chen Junping Zhang Li Dong Xiangping Zhang School of Chemical Engineering University 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 Mesoscience and EngineeringInstitute of Process EngineeringChinese Academy of SciencesBeijing 100190China Longzihu New Energy Laboratory Zhengzhou Institute of Emerging Industrial TechnologyHenan UniversityZhengzhou 450000HenanChina

Catalysts for CO_(2)value-added conversion have been extensively explored,but there is still a lack of systematic design for catalysts that achieve efficient CO_(2)conversion under mild ***,we explored a mesoporous CeO_(2)single-crystal formed with the regulation of ionic liquids,which catalyzed the effective carbonylation reaction with CO_(2)under mild reaction *** altering the synthetic environment,a series of uniform mesoporous CeO_(2)particles with atomically aligned single-crystal frameworks were constructed,which have different surface physicochemical properties and primary aggregation *** prepared mesoporous CeO_(2)single-crystal achieved efficient activation of CO_(2)and alcohols at 0.5 MPa CO_(2)and 100℃,and the CeO_(2)-IL-M catalyst shows optimal catalytic performance in the synthesis of ethylene carbonate with 46.22 mmol g^(–1)h^(–1),which was 50.6 times as high as that of the CeO_(2)obtained without ionic ***,the catalytic pathway and mechanism of carbonylation reaction with CO_(2)on mesoporous CeO_(2)single-crystal were studied via React-IR spectra and C18O_(2)labeling *** research provides a new strategy for controllable nanoscale assembly of mesoporous single-crystal materials and expands the application range of single-crystal materials,aiming to develop novel catalytic materials to meet industrial needs.

关键词： Cerium dioxide Ionic liquid Single-crystal material Surface oxygen vacancy Carbonylation reaction

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Bio-inspired short peptide self-assembly:From particles to functional materials

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Particuology 2022年第5期20卷 14-34页

作者： Li Wang Guizhi Shen Xuehai Yan State Key Laboratory of Biochemical Engineering Institute of Process EngineeringChinese Academy of SciencesBeijing 100190China School of Chemical Engineering University of Chinese Academy of SciencesBeijing 100049China Center for Mesoscience Institute of Process EngineeringChinese Academy of SciencesBeijing 100190China

Natural systems are typically featured with tremendous molecular complexity and construct exquisite architectures and functional materials through precise spatial and temporal *** self-assembly from peptides and proteins is believed to be the key ***,knowledge of the fundamental mechanisms driving peptides into vast functional hierarchical structures will certainly help the rational control of self-assembly process,leading to more precise structural organization and functional *** this review,we briefly summarize the recent progress of this burgeoning field mainly from two directions:peptide-based self-assembly and co-assembly with other functional molecules,each part is further divided into two subparts and representative examples are given for each subpart according to their development *** the end of each part,brief summaries of the closely related applications are *** the closing remarks,we conclude with our own understanding of the area and perspectives are given based on recent ***,this review could be suitable for both new readers to gain a comprehensive overview of the area and experienced readers to get a summary of the development in short peptide self-assembly from particles to functional materials.

关键词： Peptide Self-assembly Intermolecular interactions Particles Functional materials

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engineering W/O/W pickering emulsion for the enhanced antigen delivery and immune responses

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Particuology 2024年第9期92卷 224-233页

作者： Sihua Wu Xiaonan Huang Yin Ma Naoki Asakawa Yufei Xia State Key Laboratory of Biochemical Engineering Institute of Process EngineeringChinese Academy of SciencesBeijing100081China Key Laboratory of Biopharmaceutical Preparation and Delivery Chinese Academy of SciencesBeijing100190China Division of Molecular Science Graduate School of Science and TechnologyGunma University1-5-1Tenjin-choKiryu376-8515Japan Sinovac Biotech Ltd. Beijing100085China School of Chemical Engineering Nanjing Tech UniversityNanjing211816China School of Chemical Engineering University of Chinese Academy of SciencesBeijing100049China

Tumor immunotherapy,particularly cancer vaccines,holds promise for combating cancer by harnessing tailored immune responses against malignant ***,conventional approaches face challenges in efficiently delivering antigens for optimal immune *** adjuvants,like MF59,enhance cellular uptake but struggle to induce robust CD8^(+)T cell ***,we introduce a novel strategy employing a water-in-oil-in-water(W/O/W)multiple Pickering emulsion(mPE)for antigen *** mPE,utilizing biocompatible,pH-sensitive particles,encapsulates antigens within the inner water phase,ensuring enhanced intracellular processing and dictating the intracellular fate of antigens for improved *** vitro and in vivo studies demonstrated that mPEs induced robust dendritic cells activation and antigen cross-presentation,leading to a significantly enhanced immune ***,calcium phosphate-stabilized mPE(CaP-mPE)illustrated the more robust IFN-γ^(+)T cell *** comparison with traditional surfactant-stabilized multiple emulsions,CaP-mPE significantly inhibit tumor growth and effectively prolong the survival of tumor-bearing *** innovative approach offers a promising avenue for the development of effective cancer vaccines with potent cellular immune responses.

关键词： Cancer vaccine Multiple pickeringemulsion Adjuvant Antigen delivery Anti-tumor response

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