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Chinese Chemical Letters 2022年第12期33卷 5116-5119页

作者： Yao Wu Zhiyan Ma Jing Shi Xiaoqiang Sun Ke Yang Zheng-Yi Li Jiangsu Key Laboratory of Advanced Catalytic Materials and Technology School of Petrochemical EngineeringChangzhou UniversityChangzhou 213164China

A calix[4]arene ligand assisted directβ-C-H arylation of tertiary aliphatic aldehydes has been developed via a Pd-catalyzed C(sp3)-H functionalization process.This strategy exhibited good functional group compatibility and C-H bond site-selectivity.Mechanism studies have shown that both synergistic effect and cationic-πsupramolecular interaction between calixarene cavity and transition-metal catalytic center may play an important role in this catalytic cycle.This complementary method would be used in organic and medical chemistry due to the importance of tertiary aliphatic aldehydes.

关键词： supramolecular interaction Palladium-catalyzed C-H activation Calixarene Aliphatic aldehyde

In situ crosslink polymerization induced long-lived multicolor supramolecular hydrogel based on modifiedβ-cyclodextrin

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Chinese Chemical Letters 2024年第2期35卷 374-379页

作者： Yonghui Sun Linnan Jiang Yong Chen Yu Liu College of Chemistry State Key Laboratory of Elemento-Organic Chemistry Nankai UniversityTianjin 300071China

The construction of hydrogels with good mechanical properties and phosphorescent properties is full of challenges.Herein,we report a supramolecular phosphorescent hydrogel with long lifetime,high tensile strength and self-healing property,which can be easily constructed through in-situ thermalinitiated polymerization of isocyanatoethyl acrylate-modifiedβ-cyclodextrin(β-CD-DA)and acrylatemodified adamantane(Ad-DA),acrylic acid(AA),followed by the non-covalent association with carbon dots(CNDs).The lifetime of phosphorescent hydrogel can reach 1261 ms at room temperature,and the quantum yield is 11%.Importantly,through the efficient triplet to singlet Förster resonance energy transfer(TS-FRET),the phosphorescent hydrogel shows the good phosphorescence energy transfer property for organic dyes Rhodamine B and Eosin Y with the delayed fluorescence lifetime up to 730 ms and 585 ms as well as the energy transfer efficiency(Φ_(ET))up to 99.9%and 99.3%,respectively.Moreover,owing to the host-guest interactions betweenβ-CD-DA and Ad-DA,the three-dimensional cross-linked network phosphorescent hydrogel can be easily stretched to 18 times of its original length,and can achieve self-healing of the cut surfaces within 30 min.These results will expand the scope of phosphorescent materials and provide new ideas and opportunities for materials science.

关键词： Room temperature phosphorescence Hydrogel Phosphorescence energy transfer Cyclodextrin supramolecular interaction

supramolecular Bonding Competition Enabled Nanostructure Evolution and Mechanical Reinforcement

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CCS Chemistry 2024年第1期6卷 157-164页

作者： Yuting Wang Peng Meng Aidan Brock Yanan Xu Hang Meng Zixuan Liu Kan Zhang John McMurtrie Jingsan Xu School of Chemistry and Physics and Centre for Materials Science Queensland University of TechnologyBrisbaneQueensland 4000 Central Analytical Research Facility Institute for Future EnvironmentsQueensland University of TechnologyBrisbaneQueensland 4000 State Key Laboratory of Superhard Materials Department of Materials Science and Key Laboratory of Automobile MaterialsMOEJilin UniversityChangchun 130012

In this work,competition between different supramolecular interactions is investigated based on a fibrous crystal composed of hydrogen-bonded cyanuric acid(CA)and amidinothiourea(ADT).Melamine(M)is found to prevail over ADT and bond to CA due to its stronger triple H-bonding affiliation,forming hollow microtubes assembled by oriented CAM crystalline arrays,as guided by the directionality of peripheral hydrogen bonds.Furthermore,competitive interaction between hydrogen bonding and ionic/covalent bonding is demonstrated by mixing Ag+ions with the CA-ADT fibers,where sulfur atoms are abstracted from ADT molecules to produce Ag_(2)S ligaments.The in situ-formed Ag_(2)S serves as a binding glue to generate CA-ADT/Ag_(2)S composites with significantly enhanced mechanical strength compared to the pristine CA-ADT fiber pellet.

关键词： supramolecular interaction hydrogen bonds chemical bond competition hollow crystal array organic-inorganic composite

A polymeric co-assembly of subunit vaccine with polyoxometalates induces enhanced immune responses

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Nano Research 2022年第5期15卷 4175-4180页

作者： Xinpei Li Xiaofeng He Dongrong He Yuan Liu Kun Chen Panchao Yin South China Advanced Institute for Soft Matter Science and Technology School of Molecular Science and EngineeringSouth China University of TechnologyGuangzhou 510640China Guangdong Provincial Key Laboratory of Functional and Intelligent Hybrid Materials and Devices South China University of TechnologyGuangzhou 510640China

Long-lasting protective immune responses are expected following vaccination.However,most vaccines alone are inability to evoke an efficient protection.The combinatory administration of adjuvants with vaccines is critical for generating the enhanced immune responses.Herein,with biocompatible poly(4-vinylpyridine)(P4VP)as template,2.5 nm iron/molybdenum oxide cluster,{Mo_(72)Fe_(30)},is applied as an adjuvant to co-assemble with antigens of Mycobacterium bovis via hydrogen bonding at molecular scale.Molecular scale integration of the antigens and{Mo_(72)Fe_(30)}and their full exposure to body fluid media contribute to the augmentation of both humoral and cellular immune responses of the vaccines after inoculation in mice.Anti-inflammatory factor IL-10 gradually increases after 2 weeks followed by a final back to normal level by the 5th week.The balance between proinflammatory cytokines and anti-inflammatory factors suggests that immune system can be activated in the early stage of infection by the antigens carried by the supra-particles and secrete acute inflammatory factors for host defense and anti-inflammatory factors for immune protection.

关键词： co-assembly immune response metal oxide cluster supramolecular interaction vaccine adjuvant

Sensitized effect of β-cyclodextrin on the fluorescence in the determination of carbaryl

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Journal of Environmental Sciences 2004年第5期16卷 829-831页

作者： LIUWen-li TANGBo CollegeofLifeSciencesandMedicineChemicalEngineering TaizhouUniversityTaizhou317000China CollegeofChemistry ChemicalEngineeringandMaterialsScienceShandongNormalUniversityJinan250014China

Based on the significant enhancement of fluorescence intensity of carbaryl in inclusion complex, a spetrofluorimetric method with high sensitivity was developed for the determination of carbaryl in aqueous solution. Under the optimum conditions, the complex had excitation and emission maxima at 278 nm and 332 nm, respectively. The linear range of the method was 7.0 ng/ml—1500 ng/ml with a detection limit of 1.2 ng/ml. The proposed method was successfully used to determine quantitatively of carbaryl in cottonseeds.

关键词： carbaryl β-cycclodextrin spectrofluorimetry supramolecular interaction determination

Determination of paraquat in water samples using a sensitive fluorescent probe titration method

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Journal of Environmental Sciences 2013年第6期25卷 1245-1251页

作者： Feihu Yao Hailong Liu Guangquan Wang Liming Du Xiaofen Yin Yunlong Fu Analytical and Testing Center Shanxi Normal University

Paraquat （PQ）, a nonselective herbicide, is non-fluorescent in aqueous solutions. Thus, its determination through direct fluorescent methods is not feasible. The supramolecular inclusion interaction of PQ with cucurbit[7]uril was studied by a fluorescent probe titration method. Significant quenching of the fluorescence intensity of the cucurbit[7]uril-coptisine fluorescent probe was observed with the addition of PQ. A new fluorescent probe titration method with high selectivity and sensitivity at the ng/mL level was developed to determine PQ in aqueous solutions with good precision and accuracy based on the significant quenching of the supramolecular complex fluorescence intensity. The proposed method was successfully used in the determination of PQ in lake water, tap water, well water, and ditch water in an agricultural area, with recoveries of 96.73% to 105.77%. The fluorescence quenching values （AF） showed a good linear relationship with PQ concentrations from 1.0 × 10^-8 to 1.2× 10^-5 mol/L with a detection limit of 3.35 x 10-9 mol/L. In addition, the interaction models of the supramolecular complexes formed between the host and the guest were established using theoretical calculations. The interaction mechanism between the cucurbit[7]uril and PQ was confirmed by 1H NMR spectroscopy.

关键词： paraquat coptisine cucurbituril supramolecular interaction fluorescent probe titration

Real-time and in-situ intracellular ATP assay with polyimidazolium brush-modified nanopipette

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Science China Chemistry 2020年第7期63卷 1004-1011页

作者： Kailin Zhang Tianyi Xiong Fei Wu Qingwei Yue Wenliang Ji Ping Yu Lanqun Mao Beijing National Laboratory for Molecular Sciences Key Laboratory of Analytical Chemistry for Living BiosystemsInstitute of Chemistrythe Chinese Academy of Sciences(CAS)Beijing 100190China University of Chinese Academy of Sciences Beijing 100049China

The level and dynamics of adenosine 5’-triphosphate(ATP) in single living cells are closely related to many kinds of important physiological and pathological processes. Herein, we report a nanosensor based on polyimidazolium brush(PimB)-modified nanopipette for intracellular ATP assay, which shows good selectivity, high spatiotemporal resolution and excellent stability.Both the specific supramolecular interaction between polyimidazolium and ATP, and the rationally tunable property of the ion transport at a confined nanopipette enable the selective assay of ATP even in complex intracellular environment. Moreover, the tiny tip(ca.300 nm) and the low polarized current(e.g., 1 nA) essentially make the as-prepared nanosensor safe to the living cells. The nanosensor is demonstrated to be useful for in-situ monitoring the basal ATP levels of chromaffin cells from wild-type mice and DJ-1 knockout mice, and for real-time monitoring the metabolism process of intracellular ATP.

关键词： intracellular ATP nanosensor ion transport single-cell analysis supramolecular interaction

supramolecular Polymer Emulsifiers for One-step Complex Emulsions

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Chinese Journal of Polymer Science 2018年第3期36卷 288-296页

作者： zhen wang shenglong liao yapei wang department of chemistry renmin university of chinaBeijing 100872China

Complex emulsions, such as double emulsions and high-internal-phase emulsions, have shown great applications in the fields of drug delivery, sensing, catalysis, oil-water separation and self-healing materials. Their controllable preparation is at the forefront of interface and material science. Surfactants and polymers have been widely used as emulsifiers for building complex emulsions. Yet some inherent disadvantages exist including multi-step emulsifications and low production efficiency. Alternatively, supramolecular polymer emulsifier for complex emulsions via one-step emulsification is rising as a new strategy due to the ease of preparation. In this feature article, we review our recent progresses in using supramolecular polymer emulsifiers for the preparation of complex emulsions. Double emulsions and high-internal-phase emulsions are successfully prepared via one-step emulsification with the help of different supramolecular interactions including electrostatic, hydrogen bond, coordination interaction and dynamic covalent bond, which will be particularly emphasized in detail. In the end, a comprehensive prospect is given for the future development of this field. This article is expected to provide new inspirations for preparing complex emulsions via supramolecular routes.

关键词： Complex emulsions Double emulsions High-internal-phase emulsions supramolecular interaction One-step emulsification

Azobenzene Based Photo-responsive Mechanical Actuator Fabricated by Intermolecular H-bond interaction

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Chinese Journal of Polymer Science 2021年第4期39卷 417-424,I0005页

作者： Chun-Yan Yu Jia-Hui Mu Yun-Lei Fu Yun-Chao Zhang Ji-Shu Han Rui-Yang Zhao Jia Zhao Zi-Hao Wang Zhong-Cheng Zhao Wei-Jun Li Fu-Sheng Liu State Key Laboratory Base of Eco-chemical Engineering College of Chemical EngineeringQingdao University of Science and TechnologyQingdao 266042China Taishan Scholar Advantage and Characteristic Discipline Team of Eco Chemical Process and Technology College of Chemistry and Molecular EngineeringQingdao University of Science and TechnologyQingdao 266042China State Key Laboratory Breeding Base of Green Chemistry Synthesis Technology College of Chemical EngineeringZhejiang University of TechnologyHangzhou 310014China

Photo-responsive mechanical actuator is a class of stimuli-responsive materials transferring light to mechanical energy through macroscopic transformation.To fabricate photo-responsive mechanical actuator,soft polymeric materials crosslinked with functional bridging structures are desired.supramolecular interaction is a relatively common way to fabricate crosslinked materials due to its excellent self-assembly performance.And azobenzene and derivatives are ideal candidates of photo-responsive materials because of the unique photo-induced trans-cis isomerization.Here,a new kind of crosslinked materials based on supramolecular interaction between 4,4'-dihydroxyazobenzene and chitosan is reported.Under 355 nm irradiation,the macroscopic bending of polymeric materials occurs rapidly due to the photo-isomerization of 4,4-dihydroxyazobenzene.Meanwhile,the photo-responsive mechanical actuator can also lift weight which is up to 200 times that of the actuator itself,and convert energy from light to mechanical work efficiently.This report suggests a new kind of photo-responsive actuator based on supramolecular interaction and may be helpful to contribute a theoretical basis to the design and synthesis of photo-responsive mechanical actuator suitable for large-scale manufacturing industrialization in future.

关键词： Photo-response supramolecular interaction Mechanical actuator Azobenzene Energy conversion

Crossed Ladders in a 2-D Mixed-ligand Lanthanide Coordination Polymer:Synthesis,Crystal Structure and Photoluminescence

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Chinese Journal of Structural Chemistry 2011年第7期30卷 969-974页

作者：张明星王新芳陈新彭大权刘玺付文升黄坤林 College of Chemistry Chongqing Normal University State Key Laboratory of Explosion Science and Technology Department of Chemistryand Institute for Chemical PhysicsBeijing Institute of Technology Department of Chemistry Dezhou University

A new metal-organic coordination polymer, [Ce（L1）（L2）（H2O）]2H2O （1, H2L1 = 2,6-dimethylpyridine-3,5-diearboxylie acid, H2L2 = （E）-2,6-dimethyl-4-styrylpyridine-3,5-dieerboxylie acid）, has been synthesized and characterized by elemental analysis, IR, and X-ray single-crystal diffraction. Compound 1 crystallizes in trielinic, space group P1 and displays a two-dimensional coordination network structure. In 1, the relatively rare crossed ladders constructed by mixed ligands organize a 2-D grid with the topology of （426）2（48668）, and the layers further build up a 3-D supramoleeular architeetttre via interlaminar hydrogen bonds.

关键词： lanthanide pyridinedicarboxylate supramolecular interaction photoluminescence