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张希院士Acc. Chem. Res.最新综述：基于多功能生物界面的主客体作用的界面超分子化学
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超分子化学的发展不仅与大环化学（冠醚、穴醚、环糊精、杯芳烃、碳60等）的发展密切相连，而且与分子自组装（双分子膜、胶束、DNA双螺旋等）、分子器件和新兴有机材料的研究息息相关。到目前为止，尽管超分子化学还没有一个完整、精确的定义和范畴，但它的诞生和成长却是生机勃勃、充满活力 Supramolecular Chemistry at Interfaces: Host − Guest Interactions for Fabricating Multifunctional Biointerfaces 共10页 引文48篇 Hui Yang, Bin Yuan, and Xi Zhang* The Key Lab of Organic Optoelectronics & Molecular Engineering, Department of Chemistry, Tsinghua University, Beijing 100084, P. R. China Oren A. Scherman* Melville Laboratory for Polymer Synthesis, Department of Chemistry, University of Cambridge, Cambridge CB21EW, United Kingdom *E-mail: xi@mail.tsinghua.edu.cn (X.Z.)., *E-mail: oas23@cam.ac.uk (O.A.S.). Conspectus Host–guest chemistry can greatly improve the selectivity of biomolecule–ligand binding on account of recognition-directed interactions. In addition, functional structures and the actuation of supramolecular assemblies in molecular systems can be controlled efficiently through various host–guest chemistry. Together, these highly selective, strong yet dynamic interactions can be exploited as an alternative methodology for applications in the field of programmable and controllable engineering of supramolecular soft materials through the reversible binding between complementary components. Many processes in living systems such as biotransformation, transportation of matter, and energy transduction begin with interfacial molecular recognition, which is greatly influenced by various external stimuli at biointerfaces. Detailed investigations about the molecular recognition at interfaces can result in a better understanding of life science, and further guide us in developing new biomaterials and medicines. In order to mimic complicated molecular-recognition systems observed in nature that adapt to changes in their environment, combining host–guest chemistry and surface science is critical for fabricating the next generation of multifunctional biointerfaces with efficient stimuli-responsiveness and good biocompatibility. In this Account, we will summarize some recent progress on multifunctional stimuli-responsive biointerfaces and biosurfaces fabricated by cyclodextrin- or cucurbituril-based host–guest chemistry and highlight their potential applications including drug delivery, bioelectrocatalysis, and reversible adsorption and resistance of peptides, proteins, and cells. In addition, these biointerfaces and biosurfaces demonstrate efficient response toward various external stimuli, such as UV light, pH, redox chemistry, and competitive guests. All of these external stimuli can aid in mimicking the biological stimuli evident in complex biological environments. We begin by reviewing the current state of stimuli-responsive supramolecular assemblies formed by host–guest interactions, discussing how to transfer host–guest chemistry from solution onto surfaces required for fabricating multifunctional biosurfaces and biointerfaces. Then, we present different stimuli-responsive biosurfaces and biointerfaces, which have been prepared through a combination of cyclodextrin- or cucurbituril-based host–guest chemistry and various surface technologies such as self-assembled monolayers or layer-by-layer assembly. Moreover, we discuss the applications of these biointerfaces and biosurfaces in the fields of drug release, reversible adsorption and release of some organic molecules, peptides, proteins, and cells, and photoswitchable bioelectrocatalysis. In addition, we summarize the merits and current limitations of these methods for fabricating multifunctional stimuli-responsive biointerfaces in a dynamic noncovalent manner. Finally, we present possible strategies for future designs of stimuli-responsive multifunctional biointerfaces and biosurfaces by combining host–guest chemistry with surface science, which will lead to further critical development of supramolecular chemistry at interfaces. Biography Hui Yang got his Ph.D. in the School of Chemistry and Chemical Engineering, Shandong University under the guidance of Professor Yebang Tan. In 2012, he joined Prof. Xi Zhang’s group as a postdoctor in Department of Chemistry at Tsinghua University. Currently, he is working on fabricating functional supramolecular polymer materials. Biography Bin Yuan got his B.S. in Department of Chemistry, Tsinghua University in 2012. Now he is a Ph.D. student in Prof. Xi Zhang’s group. He is working on the supramolecular assembly at the interface. Biography Xi Zhang is a full professor of the Department of Chemistry, Dean of School of Science, Tsinghua University. His research interests are focused on supra-amphiphiles, supramolecular polymers, selenium-containing polymers, layer-by-layer assembly, and single-molecule force spectroscopy of polymers. He serves as a Senior Editor of Langmuir and is a member of the Advisory Board of several journals, including Accounts of Chemical Research, Chemical Communications, Chemistry—A European Journal, Polymer, and Polymer Chemistry. He was elected Member of Chinese Academy of Sciences in 2007, and fellow of Royal Society of Chemistry, U.K. in 2008. Currently, he is the vice president of the Chinese Chemical Society. Biography Oren A. Scherman is the Director of the Melville Laboratory for Polymer Synthesis in the Department of Chemistry and the University of Cambridge. His research group is interested in dynamic supramolecular self-assembly at interfaces. Oren’s current research projects include the application of macrocyclic host–guest chemistry using cucurbit[n]urils in the development of novel supramolecular hydrogels, drug-delivery systems based on dynamic hydrogels, the conservation and restoration of important historical artifacts through the exploitation of supramolecular polymer chemistry and sensing, and catalysis using self-assembled nanophotonic systems. Oren is also a cofounder of the recent spin-out company “aqdot” from Cambridge University working in the area of encapsulation. He is currently on sabbatical as the Xuetang Visiting Professor of Chemistry at Tsinghua University in Beijing, China.  |
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