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Supramolecular Assembly through Interactions between Molecular Dipoles and Alkali Metal Ions 下载免费PDF全文
Dr. Tomoko K. Shimizu Dr. Jaehoon Jung Dr. Hiroshi Imada Dr. Yousoo Kim 《Angewandte Chemie (International ed. in English)》2014,53(50):13729-13733
Establishing a way to fabricate well‐ordered molecular structures is a necessary step toward advancement in organic optoelectronic devices. Here, we propose to use interactions between electric dipoles of molecules and alkali metal ions to form a well‐developed homogeneous monolayer of diarylethene molecules on the Cu(111) surface with the aid of NaCl co‐deposition. Scanning tunneling microscopy and density functional theory calculation results indicate that the formation of a row‐type structure occurs as a result of interactions between the Na+ ions and the diarylethene molecular dipoles, drastically changing the adsorption configuration from that without Na+. 相似文献
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Spontaneous Reconstitution of Functional Transmembrane Proteins During Bioorthogonal Phospholipid Membrane Synthesis 下载免费PDF全文
Christian M. Cole Dr. Roberto J. Brea Young Hun Kim Michael D. Hardy Prof. Jerry Yang Prof. Neal K. Devaraj 《Angewandte Chemie (International ed. in English)》2015,54(43):12738-12742
Transmembrane proteins are critical for signaling, transport, and metabolism, yet their reconstitution in synthetic membranes is often challenging. Non‐enzymatic and chemoselective methods to generate phospholipid membranes in situ would be powerful tools for the incorporation of membrane proteins. Herein, the spontaneous reconstitution of functional integral membrane proteins during the de novo synthesis of biomimetic phospholipid bilayers is described. The approach takes advantage of bioorthogonal coupling reactions to generate proteoliposomes from micelle‐solubilized proteins. This method was successfully used to reconstitute three different transmembrane proteins into synthetic membranes. This is the first example of the use of non‐enzymatic chemical synthesis of phospholipids to prepare proteoliposomes. 相似文献
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Jun-Bo Chen Dr. Cen Zhou Ru-Qiang Lu Dr. Xin-Chang Wang Hang Qu Dr. Mithu Saha Hao-Liang Liu Prof. Hui Zhang Prof. Xiao-Yu Cao 《Chemistry (Weinheim an der Bergstrasse, Germany)》2019,25(5):1293-1299
Triindolo-truxene, a C3-symmetric molecule with a large π-conjugated plane, has six methylene carbon atoms and three aromatic carbon atoms that can be facilely functionalized. Herein, butyl, carbonyl, cyano, and/or malononitrile groups were introduced at six methylene carbon atoms (6-, 14-, 22- or 8-, 16-, 24-positions) and/or three aromatic carbon atoms (2-, 10-, and 18-positions) of triindolo-truxene to produce eight derivatives. Their photophysical properties, electrochemical properties, and molecular assembly can be effectively modulated by substituents and substitution patterns. Incorporation of electron-deficient groups led to redshifts in both the absorption and emission of these derivatives and also lowered their HOMO and LUMO levels. Different substitution patterns resulted in the different intramolecular donor–acceptor interactions. Electron-deficient substituents at the methylene carbon atoms in the 6-, 14-, and 22-positions led to intramolecular charge transfer from the fluorene arms to the truxene core, whereas the corresponding substitutions at the methylene carbon atoms in the 8-, 16-, and 24-positions resulted in intramolecular charge transfer from the truxene core to the fluorene arms. The molecular packing in single crystals and molecular aggregation in solution are also influenced by the substituents and substitution patterns. This work provides a straightforward strategy to alter the properties of triindolo-truxene. 相似文献
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Yiyuan Han Zhixing Lin Dr. Jiajing Zhou Dr. Gyeongwon Yun Rui Guo Dr. Joseph J. Richardson Prof. Frank Caruso 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(36):15748-15755
Functional materials composed of proteins have attracted much interest owing to the inherent and diverse functionality of proteins. However, establishing general techniques for assembling proteins into nanomaterials is challenging owing to the complex physicochemical nature and potential denaturation of proteins. Here, a simple, versatile strategy is introduced to fabricate functional protein assemblies through the interfacial assembly of proteins and polyphenols (e.g., tannic acid) on various substrates (organic, inorganic, and biological). The dominant interactions (hydrogen-bonding, hydrophobic, and ionic) between the proteins and tannic acid were elucidated; most proteins undergo multiple noncovalent stabilizing interactions with polyphenols, which can be used to engineer responsiveness into the assemblies. The proteins retain their structure and function within the assemblies, thereby enabling their use in various applications (e.g., catalysis, fluorescence imaging, and cell targeting). 相似文献
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ZHU Xiao-Yang 《高等学校化学学报》2000,21(Z1):348
The use of molecules as electronic devices is one of the focuses in the emerging field of nanotechnology. Two issues of relevance to this topic will be discussed in this lecture. In the first part, I will discuss the interfacial electronic structure and electron transport mechanism at molecular-metal junctions. Recent results from my laboratory revealed the role of chemical anchor in electron transport and the formation of molecular quantum wells at metal/organic interfaces. In the second part, I will present a general strategy to integrate molecular components into silicon technology. The application of this chemistry beyond molecular electronics will also be discussed. 相似文献
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Dr. Liulin Yang Aijie Liu Shuqin Cao Rindia M. Putri Prof. Pascal Jonkheijm Prof. Jeroen J. L. M. Cornelissen 《Chemistry (Weinheim an der Bergstrasse, Germany)》2016,22(44):15570-15582
The study of protein self‐assembly has attracted great interest over the decades, due to the important role that proteins play in life. In contrast to the major achievements that have been made in the fields of DNA origami, RNA, and synthetic peptides, methods for the design of self‐assembling proteins have progressed more slowly. This Concept article provides a brief overview of studies on native protein and artificial scaffold assemblies and highlights advances in designing self‐assembling proteins. The discussions are focused on design strategies for self‐assembling proteins, including protein fusion, chemical conjugation, supramolecular, and computational‐aided de novo design. 相似文献
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Emergent Molecular Recognition through Self‐Assembly: Unexpected Selectivity for Hyaluronic Acid among Glycosaminoglycans 下载免费PDF全文
Dr. Takao Noguchi Dr. Bappaditya Roy Dr. Daisuke Yoshihara Dr. Junji Sakamoto Dr. Tatsuhiro Yamamoto Prof. Dr. Seiji Shinkai 《Angewandte Chemie (International ed. in English)》2016,55(19):5708-5712
Oligophenylenevinylene (OPV)‐based fluorescent (FL) chemosensors exhibiting linear FL responses toward polyanions were designed. Their application to FL sensing of glycosaminoglycans (heparin: HEP, chondroitin 4‐sulfate: ChS, and hyaluronic acid: HA) revealed that the charge density encoded as the unit structure directs the mode of OPV self‐assembly: H‐type aggregate for HEP with 16‐times FL increase and J‐type aggregate for HA with 93‐times FL increase, thus unexpectedly achieving the preferential selectivity for HA in contrast to the conventional HEP selective systems. We have found that the integral magnitude of three factors consisting of binding mechanism, self‐assembly, and FL response can amplify the structural information on the target input into the characteristic FL output. This emergent property has been used for a novel molecular recognition system that realizes unconventional FL sensing of HA, potentially applicable to the clinical diagnosis of cancer‐related diseases. 相似文献
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Oleg E. Perelstein Viktor A. Ivanov Yury S. Velichko Pavel G. Khalatur Alexei R. Khokhlov Igor I. Potemkin 《Macromolecular rapid communications》2007,28(8):977-980
We propose a model of molecular motor based on diblock copolymer strongly adsorbed on a patterned surface. One of the blocks of the copolymer is modeled as field responsive. It is shown that time‐periodic collapse‐readsorption of the responsive block leads to the directed motion (reptation) of the molecule along the “track” provided by the surface pattern. Both the Langevin dynamics (LD) technique of computer simulation for the bead‐spring model and numerical solution of the Newton equations of a simplified (toy) model of the copolymer are used. The physical reason of directionality of the motion is shown to be an anisotropy of the friction of the molecule with the surface.
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Shan Mei Mark Staub Prof. Dr. Christopher Y. Li 《Chemistry (Weinheim an der Bergstrasse, Germany)》2020,26(2):349-361
Nanoparticles can be assembled into complex structures and architectures by using a variety of methods. In this review, we discuss recent progress of using polymer crystallization (particularly polymer single crystals, PSCs) to direct nanoparticle assembly. PSCs have been extensively studied since 1957. Mainly appearing as quasi-two-dimensional (2D) lamellae, PSCs are typically used as model systems to determine polymer crystalline structures, or as markers to investigate the crystallization process. Recent research has demonstrated that they can also be used as nanoscale functional materials. Herein, we show that nanoparticles can be directed to assemble into complex shapes by using in situ or ex situ polymer crystal growth. End-functionalized polymers can crystallize into 2D nanosheet PSCs, which are used to conjugate with complementary nanoparticles, leading to a nanosandwich structure. These nanosandwiches can find interesting applications for catalysis, surface-enhanced Raman spectroscopy, and nanomotors. Dissolution of the nanosandwich leads to the formation of Janus nanoparticles, providing a unique method for asymmetric nanoparticle synthesis. 相似文献
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Zhiqiang Feng Guoqiang Fan Hongxia Wang Changyou Gao Jiacong Shen 《Macromolecular rapid communications》2009,30(6):448-452
Hollow polyphosphazene microcapsules have been fabricated by the covalent layer‐by‐layer assembly of polydichlorophosphazene (PDCP) and hexamethylenediamine (HDA) on aminosilanized silica particles, followed by core removal in a HF/NH4F solution. The hollow and intact microcapsules in both wet and dry states have been characterized by transmission electron microscopy and confocal laser scanning microscopy. The chemical structure of the microcapsules has been verified by FT‐IR spectroscopy. The microcapsules could be hydrolytically degraded in a phosphate buffer at biological pH.
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Folding DNA into a Lipid‐Conjugated Nanobarrel for Controlled Reconstitution of Membrane Proteins 下载免费PDF全文
Dr. Yuanchen Dong Dr. Shuobing Chen Dr. Shijian Zhang Dr. Joseph Sodroski Dr. Zhongqiang Yang Dr. Dongsheng Liu Dr. Youdong Mao 《Angewandte Chemie (International ed. in English)》2018,57(8):2072-2076
Building upon DNA origami technology, we introduce a method to reconstitute a single membrane protein into a self‐assembled DNA nanobarrel that scaffolds a nanodisc‐like lipid environment. Compared with the membrane‐scaffolding‐protein nanodisc technique, our approach gives rise to defined stoichiometry, controlled sizes, as well as enhanced stability and homogeneity in membrane protein reconstitution. We further demonstrate potential applications of the DNA nanobarrels in the structural analysis of membrane proteins. 相似文献
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Yiyuan Han Zhixing Lin Jiajing Zhou Gyeongwon Yun Rui Guo Joseph J. Richardson Frank Caruso 《Angewandte Chemie (International ed. in English)》2020,59(36):15618-15625
Functional materials composed of proteins have attracted much interest owing to the inherent and diverse functionality of proteins. However, establishing general techniques for assembling proteins into nanomaterials is challenging owing to the complex physicochemical nature and potential denaturation of proteins. Here, a simple, versatile strategy is introduced to fabricate functional protein assemblies through the interfacial assembly of proteins and polyphenols (e.g., tannic acid) on various substrates (organic, inorganic, and biological). The dominant interactions (hydrogen‐bonding, hydrophobic, and ionic) between the proteins and tannic acid were elucidated; most proteins undergo multiple noncovalent stabilizing interactions with polyphenols, which can be used to engineer responsiveness into the assemblies. The proteins retain their structure and function within the assemblies, thereby enabling their use in various applications (e.g., catalysis, fluorescence imaging, and cell targeting). 相似文献
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Dr. Dorothee Wasserberg Dr. Christian Haase Dr. Hoang D. Nguyen Jan Hendrik Schenkel Prof. Dr. Jurriaan Huskens Prof. Dr. Bart Jan Ravoo Dr. Pascal Jonkheijm Prof. Dr. Luc Brunsveld 《Chemistry (Weinheim an der Bergstrasse, Germany)》2012,18(22):6788-6794
Supramolecular assembly of proteins on surfaces and vesicles was investigated by site‐selective incorporation of a supramolecular guest element on proteins. Fluorescent proteins were site‐selectively labeled with bisadamantane by SNAP‐tag technology. The assembly of the bisadamantane functionalized SNAP‐fusion proteins on cyclodextrin‐coated surfaces yielded stable monolayers. The binding of the fusion proteins is specific and occurs with an affinity in the order of 106 M ?1 as determined by surface plasmon resonance. Reversible micropatterns of the fusion proteins on micropatterned cyclodextrin surfaces were visualized by using fluorescence microscopy. Furthermore, the guest‐functionalized proteins could be assembled out of solution specifically onto the surface of cyclodextrin vesicles. The SNAP‐tag labeling of proteins thus allows for assembly of modified proteins through a host–guest interaction on different surfaces. This provides a new strategy in fabricating protein patterns on surfaces and takes advantage of the high labeling efficiency of the SNAP‐tag with designed supramolecular elements. 相似文献
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Yang-Jin Cho So-Yoen Kim Jie-Won Lee Prof. Won-Sik Han Prof. Chul Hoon Kim Prof. Ho-Jin Son Prof. Sang Ook Kang 《Chemistry (Weinheim an der Bergstrasse, Germany)》2019,25(34):8149-8156
A new type of solid-state photochromism was observed in an AB2-type molecular assembly comprising a central silole and two peripheral o-carborane units, and in this assembly, depending on the assembling positions of those units at the adjoining benzene ring, two different regioisomers were formed: Si-m-Cb and Si-p-Cb . Each isomer showed different solid-state photochromism depending on its solid-state molecular conformation and was either in the crystalline or amorphous state. The crystals of each meta- or para-isomer, CSi-m-Cb or CSi-p-Cb, showed yellow or blue emission, and mechanically grinding those crystals into amorphous powders of ASi-m-Cb and ASi-p-Cb, switched their emissions to blue and yellow, respectively. Photophysical studies revealed that the electronic interaction between silole and o-carborane units determined the emission color. The crystal and DFT-optimized structures each account for the crystalline and amorphous structures, respectively, and are correlated well with the electronic interactions in the molecular assembly in the solid state, thus enabling the prediction of the solid-state molecular conformational change. 相似文献
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Reinhard Wolf Masumi Asakawa Peter R. Ashton Marcos Gmez-Lpez Christoph Hamers Stephan Menzer Ian W. Parsons Neil Spencer J. Fraser Stoddart Malcolm S. Tolley David J. Williams 《Angewandte Chemie (International ed. in English)》1998,37(7):975-979
A color change from purple to green takes place on addition of tetrathiafulvalene (TTF) to the macrobicyclic receptor 1 4+, which is composed of a cyclobis(paraquat-p-phenylene) tetracation that shares one of its paraphenylene rings with a 1,5-naphthoparaphenylene-[36]crown-10 macrocycle. The TTF molecule forces the macrobicycle to turn inside out (see schematic drawing below) and displaces the self-complexed 1,5-dioxynaphthalene ring system from the center of the tetracationic cyclophane. 相似文献