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Chinese Chemical Letters 2022年第5期33卷 2455-2458页

作者： Wei Zhang Yang Luo Jie Zhao Chao Zhang Xin-Long Ni Zhu Tao Xin Xiao Key Laboratory of Macrocyclic and Supramolecular Chemistry of Guizhou Province Guizhou UniversityGuiyang 550025China

A linear supramolecular polymer with controllable features based on twisted cucurbit[14]uril(tQ[14])and cucurbit[8]uril(Q[8])was firstly fabricated via an effective self-sorting strategy.Herein we designed a monomer,1–butyl–1?-(naphthalen-2-ylmethyl)-4,4?-bipyridinium bromide(BNB),that contains bipyridyl,aliphatic butyl and aromatic naphthyl groups,simultaneously.Two host molecules,tQ[14]and Q[8]were employed to develop an effective strategy for constructing a linear supramolecular polymer with con-trollable features.The alkyl groups on both sides of BNB could insert into the two cavities of tQ[14],the naphthyl part of BNB viaπ-πstacking in Q[8]cavity,serving as the driving force for supramolecular polymerization.Through self-sorting of the monomer,tQ[14]and Q[8],led to the formation of the linear supramolecular polymer.Depolymerization could be achieved by addition of adamantane hydrochloride(AH)which driven two BNB guest molecules out of the Q[8]cavity.This self-sorting strategy has great potential,not only for designing supramolecular polymer materials with different controllable structures through introduction of multiple functional groups,but also for broadening the application of twisted cucurbit[14]uril in supramolecular chemistry.

关键词： Cucurbit[n]urils Twisted cucurbituril Supramolecular polymer self-sorting Host-guest interaction

Micelle-crosslinked hydrogels with stretchable,self-healing,and selectively adhesive properties:Random copolymers work as dynamic yet self-sorting domains

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聚集体(英文)

聚集体(英文) 2023年第3期4卷 71-83页

作者： Hiroaki Asai Motoki Shibata Mikihito Takenaka Shinichi Takata Kosuke Hiroi Makoto Ouchi Takaya Terashima Department of Polymer Chemistry Graduate School of EngineeringKyoto UniversityKatsuraKyotoJapan Office of Society-Academia Collaboration for Innovation Kyoto UniversityYoshida-honmachiKyotoJapan Institute for Chemical Research Kyoto UniversityUjiKyotoJapan RIKEN SPring-8 Center Sayo-choSayo-gunHyogoJapan J-PARC Center Japan Atomic Energy AgencyTokaiIbarakiJapan

The design of crosslinking domains is a vital factor to create functional hydrogels with controlled physical,mechanical,and adhesive properties.This paper demonstrates versatile synthetic systems of micelle-crosslinked hydrogels with highly stretchable,self-healing,and selectively adhesive properties.For this,methacrylate-bearing random copolymer micelles are designed as physical and covalent crosslink domains via the self-assembly of amphiphilic random copolymers carrying hydrophilic poly(ethylene glycol)(PEG),hydrophobic butyl or dodecyl groups,and methacrylate-terminal PEG in water.The size,aggregation number,and pendant methacrylate number of the micelles are controlled by the composition and degree of polymerization.Hydrogels are efficiently obtained from the free radical polymerization of hydrophilic monomers such as PEG acrylate and acrylamide in the presence of the micelle crosslinkers in water.Owing to the dynamic yet selective chain exchange properties of the micelle domains,the hydrogels are highly stretchable up to over 1000%and show self-healing and selectively adhesive properties.The self-healing of hydrogels is promoted upon heating due to the fast chain exchange of the micelle domains,whereas hydrogels consisting of micelles with different alkyl groups are never adhesive because of their self-sorting properties.

关键词： adhesion hydrogel random copolymer micelle self-assembly self-healing self-sorting

Proliferation-mediated asymmetric nanoencapsulation of singlecell and motility differentiation

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Science China(Technological Sciences) 2023年第7期66卷 2134-2146页

作者： WANG ShengLiang XU ZhiJun CHEN HaiXu WANG XiaoLiang LIN Song WANG Lei LIU XiaoMan HUANG Xin MIIT Key Laboratory of Critical Materials Technology for New Energy Conversion and Storage School of Chemistry and Chemical EngineeringHarbin Institute of TechnologyHarbin 150001China

The biointerface engineering of living cells by creating an abiotic shell has important implications for endowing cells with exogenous properties with improved cellular behavior,which then boosts the development of the emerging field of living cell hybrid materials.Herein,we develop a way to perform active nanoencapsulation of single cell,which then endows the encapsulated cells with motion ability that they do not inherently possess.The emerging motion characteristics of the encapsulated cells could be self-regulated in terms of both the motion velocity and orbits by different proliferation modes.Accordingly,by taking advantage of the emergence of differentiated moving abilities,we achieve the self-sorting between mother cells and daughter cells in a proliferated Saccharomyces cerevisiae cell community.Therefore,it is anticipated that our highlighted study could not only serve as a new technique in the field of single-cell biology analysis and sorting such as in studying the aging process in Saccharomyces cerevisiae,but also open up opportunities to manipulate cell functionality by creating biohybrid materials to fill the gap between biological systems and engineering abiotic materials.

关键词： biointerface engineering micromotors self-propulsion self-sorting urease

Design of Metal-Organic Assemblies via Shape Complementarity and Conformational Constraints in Dual Curvature Ligands

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CCS Chemistry 2023年第11期5卷 2506-2518页

作者： Cui-Lian Liu Eduard O.Bobylev Sébastien Dauriac Brice Kauffmann Koen Robeyns Yann Garcia Joost N.H.Reek Michael L.Singleton Institute of Condensed Matter and Nanosciences Universitécatholique de LouvainLouvain-la-Neuve 1348 Van’t Hoff Institute for Molecular Sciences University of AmsterdamAmsterdam 1098 XH Universitéde Bordeaux CNRS INSERMUMS3033Institut Européen de Chimie et Biologie(IECB)33600 Pessac

While common in biological systems,building blocks with low symmetry and flexibility pose numerous problems for synthetic self-assembly,such as the formation of isomers of assemblies that are difficult to distinguish and purify.In this work,three aromatic amide-based ligands(L1–L3)with a central 1,8-diazatriptycene core were designed and used for selfassembly with Pd^(2+).While hundreds of stereoisomers based on the conformational flexibility around the amides and the unsymmetrical nonplanar structure of the core are possible upon coordination with the metal,the constraints designed into the ligands direct the self-assembly toward only a single Pd_(2)L_(4)cage(L1)or Pd_(4)L_(8)double-walled metallomacrocycle(L2)structure,even in mixtures of the ligands.This structural approach and the modularity of the ligand synthesis affords ready access to deep cavitands with endohedral functionalization(L3).These results highlight the potential of this new design strategy and open the door to selectively functionalized cavity-based architectures for numerous applications.

关键词： metal-organic cageopis isomer selectivity low-symmetry ligands self-sorting self-assembly

self-sorting Phenomena in Complex Reaction Systems

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Self-Sorting Phenomena in Complex Reaction Systems

中国化学会第29届学术年会

作者： An-Xin Wu Key Laboratory of Pesticide ＆ Chemical Biology Ministry of Education College of ChemistryCentral China Normal University

The term "self-sorting" has been discussed extensively during the past decade in chemistry.[1] Usually, "sorting" is defined as a process in which different subunits are controlled with precise constitutional and / or positional order according to certain features or criteria. Thus "self-sorting" refers to not only the ability to distinguish "self" from "nonself", but also the operation completed simultaneously and orthogonally within the mixtures.[2] Intuitively, self-sorting phenomena are very common in biological systems and complex supramolecular systems but rare in synthetic systems.[3] Based on the self-sorting property of molecular clusters, we have proposed a novel synthetic strategy of self-sorting reaction systems, which could also be described as multi-domino routes converging strategy. We have developed an efficient carbon-carbon double bond-forming reaction via homo-coupling of aryl methyl ketones or hetreo-coupling of methyl ketones with β-ketone esters and have investigated novel synthetic methods for some structurally diverse heterocyclic library via self-sorting domino strategy.[4]

关键词： self-sorting domino reaction reaction system self-organization.

self-sorting Phenomena:From Study in Complex Supramolecular Systems To Study in Complex Reaction Systems

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Self-Sorting Phenomena:From Study in Complex Supramolecular ...

全国第十七届大环化学暨第九届超分子化学学术研讨会

作者： An-Xin Wu College of Chemistry Central China Normal University

＜正＞Introduction The term"self-sorting"has been discussed extensively during the past decade in chemistry.Usually,"sorting"is defined as a process in which different subunits are controlled with precise constitutional and/or positional order according to certain features or criteria.Thus"self-sorting"refers to not only the ability to distinguish"self"from

关键词： self-sorting domino reaction:reaction system self-organization

从新型分子集群行为的研究延伸到有机合成新策略的产生——简述自分类集成反应网络的模型构建及应用

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从新型分子集群行为的研究延伸到有机合成新策略的产生——简述自...

中国化学会全国第十二届有机合成化学学术研讨会

作者：吴安心 Key Laboratory of Pesticide＆Chemical Biology Ministry of Education College of Chemistry Central China Normal University

揭示新颖的分子集群行为是开创新的学术生长点和新的学科分支的重要发端,也是了解微观分子自组织水平的重要媒介!尤其在有机合成方法学上所取得的众多创造性策略与复杂结构体的精确控制性构造,都是具有相同的逻辑演绎轨迹:即从新的分子... 详细信息

揭示新颖的分子集群行为是开创新的学术生长点和新的学科分支的重要发端,也是了解微观分子自组织水平的重要媒介!尤其在有机合成方法学上所取得的众多创造性策略与复杂结构体的精确控制性构造,都是具有相同的逻辑演绎轨迹:即从新的分子行为发现所揭示出的原理来提出了新的合成策略,并依据这些新颖的设计理念来创建了新的反应类型和新的结构形态,从而开启一些重要的学术分支。小分子集群自分类"self-sorting"现象是具有亚单元或子系统的分子集群中产生的一种区别自我与非自我的高度选择性堆积行为!多年来,我们基于小分子集群的自分类原理提出了研究有机反应的新策略——自分类多米诺汇聚集成反应的理论模式,设计完成了与模型相对应的系列反应例证,被国际诸多学者评论是有机化学中一种重要的新型合成策略,并被归纳为"MPCD合成策略",认为是开拓新型有机反应的有效工具。我们基于上述的设计策略,创建了以乙酰甲基二聚偶联成烯为主干的多样性导向反应系统,完成了5类28个天然产物的一锅全合成,对"化学合成的极限"难题——"复杂结构体的直接合成"提供了新思路。

关键词： self-sorting MPCD合成策略一锅全合成天然产物

The Bimolecular Devices Based on Asymmetric Molecular Clip

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The Bimolecular Devices Based on Asymmetric Molecular Clip

大环化学和超分子化学的新发展——当前学科交叉的一个重要...

作者：曹利平丁娇阳孙静静王军刚薛伟剑高蒙吴安心 Key Laboratory of Pesticide ＆ Chemical Biology Ministry of EducationCentral China Normal University

＜正＞Nature is the preeminent engineer of functional molecular systems.A key component of living systems is the biological proteins which are determined to a large extent by their precise three-dimensional structures.Consequently,although the constitution of these biological oligomers can be adequately described by their primary（1°） sequence,their functions are properly determined only by their secondary （2°,e.g.,α-helix orβ-sheet）,tertiary（3°）,and quaternary（4°） structures which involve folding, self-assembly,and higher order organization of lower order structural elements.

关键词： hierarchic assembly molecular clip dimerization self-sorting