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Precise supramolecular polymerization of Liquid Crystalline Block Copolymer Initiated by Heavy Metallic Salts

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Chinese Journal of Polymer Science 2022年第6期40卷 624-630页

作者： Yi-Qi Chen Bi-Xin Jin Qin Li Yun-Jun Luo Shu-Meng Chi Xiao-Yu Li School of Materials Science and Engineering Beijing Institute of TechnologyBeijing100081China Key Laboratory of High Energy Density Materials Ministry of EducationBeijing Institute of TechnologyBeijing100081China Experimental Center of Advanced Materials Beijing Institute of TechnologyBeijing100081China

Heavy metallic salts are capable to bind with proteins and cause detrimental fibrilization in living cells.Herein,we report a similar case of supramolecular polymerization and thus fibrilization from a liquid crystalline(LC)block copolymer(BCP)initiated by heavy metallic salts.Analogous to the naturally-occurring process,LC BCP“monomers”could bind with metallic salts to form small aggregates,which functioned as seeds to trigger the subsequent supramolecular polymerization of the rest BCP monomers,to produce highly uniform supramolecular polymers.The lengths of the resultant supramolecular polymer fibrils were linearly proportional to the ratios between the BCP and the metallic salts,and largely influenced by the choice of metallic cations,as well as the counterions.Lastly,this method was used to polymerize two different diblock copolymer“monomers”to produce pentablock supramolecular polymers in a one-pot manner.

关键词： Liquid crystalline block copolymer supramolecular polymerization Self assembly Controllability

supramolecular polymerization Driven by the Dimerization of Single-stranded Helix to Double-stranded Helix

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Chinese Journal of Polymer Science 2018年第3期36卷 261-261,262-265页

作者： Chao Zeng Chen-Yang Zhang Jun-Yan Zhu Ze-Yuan Dong State Key Laboratory of supramolecular Structure and Materials College of ChemistryJilin UniversityChangchun 130012China

We reported a type of strong and highly directional non-covalent interactions based on the dimerization of single-stranded helix to double-stranded helix that can achieve supramolecular polymerization, giving rise to ... 详细信息

关键词： Helix Double-stranded helix supramolecular polymers supramolecular polymerization Dimerization

In Situ supramolecular polymerization via Organometallic-Catalyzed Macromolecular Metamorphosis

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CCS Chemistry 2023年第3期5卷 761-771页

作者： Xiwen Yang Qianqian Ji Jiaxiong Liu Yiliu Liu South China Advanced Institute for Soft Matter Science and Technology School of Emergent Soft MatterSouth China University of TechnologyGuangzhou 510640

Integrating catalytic reactions with molecular assembly is a promising means of achieving controllable supramolecular polymerization.We report herein a novel and controllable method for in situ supramolecular polymerization via organometallic-catalyzed macromolecular metamorphosis.To this end,covalent polymers with polypentenamer backbones and pendant supramolecular motifs are designed and synthesized.By depolymerizing the polymers with Grubbs catalysts,the supramolecular motifs can be gradually released from the polymers to the solution.supramolecular polymerization occurs when a critical concentration is reached.The supramolecular polymerization process was readily controlled by varying the rate of the depolymerization reaction.This work presents a novel approach that uses organometallic catalysis to transform covalent polymers into supramolecular polymers.It offers a new means of constructing complex molecular systems in a controllable manner.

关键词： supramolecular polymerization organometallic catalysis macromolecular metamorphosis in situ self-assembly polymer depolymerization

A General Approach for Synthesis of Circularly Assembled supramolecular Polymers by Means of Region-confined Amphiphilic supramolecular polymerization

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Chemical Research in Chinese Universities 2023年第5期39卷 736-740页

作者： ZHANG Lei ZHANG Chenyang MIN Jing LIU Chenglong MAO Shizhong WANG Liyan YANG Bing DONG Zeyuan State Key Laboratory of supramolecular Structure and Materials Center for Supramolecular Chemical BiologyCollege of ChemistryJilin UniversityChangchun 130012P.R.China

Topological supramolecular polymers are responsible for design of innovative materials with unique physical properties but remain a challenging task to prepare by means of supramolecular polymerization.In this contribution,we present a novel method of region-confined amphiphilic supramolecular polymerization(RASP)in a controllable two-step self-organization pathway,which was certified by a new type of pyridine-oxadiazole alternating 48-membered macrocycles with structurally regional distribution of distinct self-assembling groups that can self-organize into circular supramolecular architectures.Meanwhile,water molecule plays a crucial role in RASP,and the water content in nonpolar solvent chloroform is sensitive to trigger controllable amphiphilic self-organization.Moreover,differing from the traditional rodlike micelles formed by self-assembly of linearly amphiphilic molecules,this approach of RASP exclusively gives rise to the formation of circularly assembled supramolecular polymers.

关键词： supramolecular polymerization Circular supramolecular architecture Controllable self-assembly Organic macrocycle Region-confined amphiphilic supramolecular polymerization

Mechanistic Insight into supramolecular polymerization in Water Tunable by Molecular Geometry

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CCS Chemistry 2022年第7期4卷 2212-2220页

作者： Fan Xu Stefano Crespi Lukas Pfeifer Marc C.A.Stuart Ben L.Feringa Stratingh Institute for Chemistry University of GroningenGroningen 9747 AG Key Laboratory for Advanced Materials and Joint International Research Laboratory of Precision Chemistry and Molecular Engineering Feringa Nobel Prize Scientist Joint Research CenterFrontiers Science Center for Materiobiology and Dynamic ChemistryInstitute of Fine ChemicalsSchool of Chemistry and Molecular EngineeringEast China University of Science and TechnologyShanghai 200237 Angstrom Laboratory Department of ChemistryUppsala UniversityUppsala 75120 Laboratory of Photonics and Interfaces Department of Chemistry and Chemical EngineeringÉcole Polytechnique Fédérale de LausanneLausanne CH-1015

supramolecular self-assembly in water based on non-covalent bonding is attracting major attention due to the potential of hydrogels and aqueous polymers in biomedical applications.Although supramolecular polymerization in organic solvents is well established,the key design features,the assembly mechanisms in water and achieving control over the aggregate structures remain challenging.Here,we present the assembly and disassembly of geometrical isomers of a stiff-stilbene bis-urea amphiphile(SA)in pure water.A remarkable feature of this system is that the(E)-isomer forms supramolecular polymers in both pure water and organic solvents.Taking advantage of this unique property,the hydrophobic effect was studied by comparing the supramolecular assembly in both systems.The assembly process inwater follows an enthalpy-driven nucleation-elongation(cooperative)supramolecular polymerization mechanism with a standard Gibbs free energy(ΔG°=−53 kJ mol^(−1))double the value of the one found in toluene.We attributed this distinctive feature to the hydrophobic effect in water.Furthermore,we discovered an isomer-dependent assembly process,which can be used to control aggregation in aqueous media.Due to the substantial geometric difference between(E)-SA and(Z)-SA,we compared their assembly in water to study the influence of different driving forces involved in the process.The supramolecular polymerization of(E)-SA was cooperatively influenced by hydrogen bonding,π-stacking,and hydrophobic effects,whereas the assembly of(Z)-SAwasmainly driven by hydrophobic effects.As a result,the fiber length of(E)-SA in water is much longer than that of(Z)-SA,presenting opportunities for geometrical control of aggregation in aqueousmedia.

关键词： supramolecular polymerization stiff-stil-bene bis-urea hydrogen bonding π-stacking hydro-phobic effects

Concentration Insensitive supramolecular polymerization Enabled by Kinetically Interlocking Multiple-Units Strategy

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CCS Chemistry 2019年第3期1卷 296-303页

作者： Jiezhong Shi Haoyang Jia Hao Chen Xi Wang Jiang-Fei Xu Weibin Ren Jiang Zhao Xin Zhou Yuanchen Dong Dongsheng Liu Key Laboratory of Organic Optoelectronics&Molecular Engineering of the Ministry of Education Department of ChemistryTsinghua UniversityBeijing 100084China School of Physical Sciences University of Chinese Academy of ScienceBeijing 100049China Institute of Chemistry Chinese Academy of SciencesBeijing 100190China

We proposed and demonstrated a kinetically interlocking multiple-units supramolecular polymer-ization strategy.Through rationally designed multi-ple-units monomers,the degree of polymerization(X w)detected was more than 50 with a polydispersi-ty index of∼1.4.The prepared polymers were stable when diluted to 20μM or lower concentrations.

关键词： DNA supramolecular polymerization kinetically interlocking multiple units concentration insensitive

Controlling Molecular Packing in Aqueous Metallosupramolecular Self-assembly by Ligand Geometry

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Precision Chemistry

Precision Chemistry 2023年第5期1卷 332-340页

作者： Papri Sutar Torsten Dunnebacke Zulema Fernández Timo Krüer Christina Rest Gustavo Fernández Organisch-Chemisches Institut Westfälische-Wilhelms Universität Münster48149 MünsterGermany

The coordination geometry of d8 transition metal complexes has been successfully exploited as a tool to tune photophysical properties and self-assembly pathways of supramolecular polymerization processes,with a focus being primarily placed on organic media.Expanding such controlled supramolecular and photophysical properties to assemblies in aqueous media by molecular design is,however,still challenging due to the difficulty in programming noncovalent interactions in water.Herein,we tackle this challenge by analyzing the aqueous self-assembly of amphiphilic Pt(II)complexes of different molecular geometry in order to control self-assembly and metal−metal interactions in aqueous media.To this end,we have designed two Pt(II)complexes,1 and 2,containing an identical oligophenyleneethynylene(OPE)-based aromatic scaffold that differ in the molecular geometry(linear vs V-shaped)imposed by ligand substitution and studied their comparative self-assembly behavior in aqueous media.Even though both molecules follow the isodesmic mechanism of self-assembly,their structural difference strongly influences the molecular packing in aqueous media,which in turn impacts the photophysical properties(i.***.absence or presence of MMLCT)and the self-assembly outcome.While the molecular geometry for 2 enforces short Pt…Pt contacts driven by an efficient face-to-face stacking of the OPE backbone,the antiparallel packing of 1 with slight translational offset does not allow the formation of short Pt…Pt contacts.Such a distinct interplay of interactions for 1 and 2 in aqueous media leads to significant differences in photoluminescence.

关键词： Self-assembly supramolecular polymerization amphiphilic systems π-conjugated systems Pt(II)complexes

supramolecular Adhesive Materials from Natural Acids and Sugars with Tough and Organic Solvent-Resistant Adhesion

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CCS Chemistry 2021年第6期3卷 1690-1700页

作者： Shuanggen Wu Changyong Cai Fenfang Li Zhijian Tan Shengyi Dong College of Chemistry and Chemical Engineering Hunan UniversityHunan 410082 Institute of Bast Fiber Crops Chinese Academy of Agricultural SciencesHunan 410205 College of Chemistry and Chemical Engineering Central South UniversityHunan 410083

Natural adhesives have been widely replaced by industrial adhesives made from petroleum-based products.Compared with that of traditional natural adhesives,modern industrial adhesives show improved adhesion performance.However,the drawbacks of modern adhesives,including toxicity and nonbiodegradability,drive the need for new and high-performance adhesive materials from renewable and biocompatible natural feedstock.In this study,a new family of acid-sugar adhesive materials exhibiting excellent and long-term adhesion effects was developed inspired by the concept of deep eutectic solvents(DESs).The supramolecular polymerization between natural sugars and acids gave rise to both strong cohesion and adhesion properties.Moreover,high resistance to organic solvents is an advantage of acid-sugar supramolecular adhesive materials.This study not only dramatically expands the applications of DESs but also sheds light on the development of supramolecular adhesive materials as promising alternatives to polymeric adhesives.

关键词： supramolecular adhesive materials deep eutectic solvents supramolecular polymerization supramolecular adhesion supramolecular polymers

Unconventional assemblies of bisacylhydrazones:The role of water for circularly polarized luminescence

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Aggregate

Aggregate 2022年第5期3卷 185-193页

作者： Hye Jin Cho Dong Yeun Jeong Hwihyun Moon Taewoo Kim You Kyoung Chung Yeongdong Lee Zonghoon Lee Joonsuk Huh Youngmin You Changsik Song Department of Chemistry Sungkyunkwan UniversitySuwonGyeonggi 16419Republic of Korea Division of Chemical Engineering and Materials Science Graduate Program in System Health Science and EngineeringEwha Womans UniversitySeoul 03760Republic of Korea Center for Multidimensional Carbon Materials Institute for Basic Science(IBS)Department of Materials Science and EngineeringUlsan National Institute of Science and Technology(UNIST)Ulsan 44919Republic of Korea

Understanding the precise molecular arrangement of chiral supramolecular polymers is essential not only to comprehend complex superstructures like proteins and DNA but also for the development of next-generation optoelectronic materials,including materials displaying high-performance circularly polarized luminescence(CPL).Herein,we report the first chiral supramolecular polymer systems based on hydrazone–pyridinium conjugates comprising alkyl chains of different lengths,which afforded control of the apparent supramolecular chirality.Although supramolecular chirality is governed basically by the remote chiral centers of alkyl chains,helicity inversion was achieved by controlling the conditions under which the hydrazone building blocks underwent aggregation(i.e.,solvent compositions or temperature).More importantly,the addition of water to the system led to aggregationinduced hydrazone deprotonation,which resulted in a completely different selfassembly behavior.Structural water molecules played an essential role,forming the assembly’s channel-like backbone,around which hydrazone molecules gathered as a result of hydrogen bonding interactions.Further co-assembly of an achiral hydrazone luminophore with the given supramolecular polymer system allowed the fabrication of a novel CPL-active hydrazone-based material exhibiting a high maximum value for the photoluminescence dissymmetry factor of -2.6×10^(-2).

关键词： circularly polarized luminescence(CPL) helicity control hydrazone self-assembly structural water supramolecular polymerization