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| Open AccessUsing antibodies to control DNA-templated chemical reactions
DNA-templated synthesis takes advantage of sequence-specific hybridization to accelerate chemical reactions. Here, the authors present templated synthesis controlled through antibody-antigen interactions.
- Lorena Baranda Pellejero
- , Malihe Mahdifar
- & Francesco Ricci
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Article
| Open AccessStructural order enhances charge carrier transport in self-assembled Au-nanoclusters
The collective properties of atomically precise nanoclusters bear vast potential for electronic materials by design. Here, the authors describe the self-assembly of Au32 nanoclusters into micro-crystals, which improves the electric conductivity and invokes new optical transitions caused by the high structural order.
- Florian Fetzer
- , Andre Maier
- & Marcus Scheele
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Article
| Open AccessThree host peculiarities of a cycloalkane-based micelle toward large metal-complex guests
Typical micelles are molecular assemblies composed of amphiphiles bearing linear alkyl chains. Herein, the authors present an uncommon type of cycloalkane-based bent amphiphile and its micelle which encapsulates large metal- complexes with high uptake efficiency, selectivity, and emissivity in water.
- Mamiko Hanafusa
- , Yamato Tsuchida
- & Michito Yoshizawa
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Article
| Open AccessPhotosynthetic hydrogen production by droplet-based microbial micro-reactors under aerobic conditions
The development of techniques capable of orchestrating the assembly of living cells into multicellular ensembles with synergistic and function is challenge. Here, the authors construct algal or algal/bacterial cells-based core shell-like structure based on aqueous two-phase system for synergic photosynthetic H2 production.
- Zhijun Xu
- , Shengliang Wang
- & Stephen Mann
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Article
| Open AccessSynthesis and X-ray characterization of 15- and 16-vertex closo-carboranes
The synthesis of closo-carboranes with more than 14 vertexes is challenging, and no examples have been reported to date. Herein, the authors present the long-sought 15- and 16-vertex closo-carboranes, in which the introduction of silyl groups to the two cage carbons is crucial; this finding might enable the synthesis of even larger carborane analogs in the future.
- Fangrui Zheng
- , Tsz Hin Yui
- & Zuowei Xie
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Article
| Open AccessSelf-assembled Möbius strips with controlled helicity
Different to exploring molecular topology, the development of supramolecular topology has been limited due to a lack of reliable synthetic methods. Here, the authors describe a supramolecular strategy to access Möbius strips through bending and cyclization of twisted nanofibers self-assembled from chiral glutamate amphiphiles.
- Guanghui Ouyang
- , Lukang Ji
- & Minghua Liu
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Article
| Open AccessHighly efficient synthesis of non-planar macrocycles possessing intriguing self-assembling behaviors and ethene/ethyne capture properties
The design of covalent macrocycles which show characteristic self-assembly behaviour and host-guest properties is challenging. Here, the authors demonstrate the synthesis of diphenylamine[n]arenes through a one-pot synthesis and demonstrate the π-π pi stacking of the non-planar rings as well as ethane/ethyne host-guest interactions.
- Lijun Mao
- , Yang Hu
- & Xueliang Shi
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Article
| Open AccessControl of self-assembly pathways toward conglomerate and racemic supramolecular polymers
Homo- and heterochiral aggregation is a process of interest to prebiotic and chiral separation chemistry. Here, the authors analyze the self-assembly of a racemic mixture into 1D supramolecular polymers and find homochiral aggregation into conglomerates under kinetic control, while under thermodynamic control a racemic polymer is formed.
- Marius Wehner
- , Merle Insa Silja Röhr
- & Frank Würthner
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Article
| Open AccessTwisted-Planar-Twisted expanded porphyrinoid dimer as a rudimentary reaction-based methanol indicator
Directly linked porphyrin dimers show intriguing electronic features but emphasis has been placed on planar monomeric units. Here, the authors report a Twisted-Planar-Twisted framework which can undergo a cis-trans transformation accompanied by a colour change in presence of methanol, making this framework applicable as a methanol sensor.
- Qizhao Li
- , Chengjie Li
- & Yongshu Xie
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Article
| Open AccessMolecular motor-functionalized porphyrin macrocycles
Molecular motors and switches change conformation under the influence of an external stimulus and can be incorporated into functional systems, allowing the construction of adaptive materials and switchable catalysts. Here, the authors present two molecular motor-functionalized porphyrin macrocycles for future photo-switchable catalysis.
- Pieter J. Gilissen
- , Paul B. White
- & Roeland J. M. Nolte
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Article
| Open AccessActive coacervate droplets as a model for membraneless organelles and protocells
Membraneless organelles are liquid-liquid phase-separated droplets whose behaviour can be regulated by chemical reactions, but this process is poorly understood. Here, the authors report model membraneless organelles based on coacervate droplets that show fuel-driven dynamic behaviour and concentrate functional RNA.
- Carsten Donau
- , Fabian Späth
- & Job Boekhoven
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Article
| Open AccessHomopolymer self-assembly of poly(propylene sulfone) hydrogels via dynamic noncovalent sulfone–sulfone bonding
Natural biomolecules such as peptides and DNA can dynamically self-organize into diverse hierarchical structures. Here the authors report experiments and simulations on the dynamic network self-assembly and subsequent collapse of the synthetic homopolymer poly(propylene sulfone).
- Fanfan Du
- , Baofu Qiao
- & Evan Alexander Scott
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Article
| Open AccessAutonomous mesoscale positioning emerging from myelin filament self-organization and Marangoni flows
Buckling instabilities in amphiphile-based lamellar systems can lead to the formation of tubular fingers. Van der Weijden et al. show how to shepherd their growth and destination by using drain droplets that help establishing stable interconnected mesoscale droplet networks.
- Arno van der Weijden
- , Mitch Winkens
- & Peter A. Korevaar
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Article
| Open AccessAbsolute configuration and host-guest binding of chiral porphyrin-cages by a combined chiroptical and theoretical approach
Vibrational circular dichroism (VCD) spectroscopy can be useful for determining the absolute configuration of chiral molecules, as long as the signal intensities are high enough. Here, the authors establish the absolute configurations of two large chiral porphyrin cages and, notably, discover that host-guest binding enhances their VCD intensities.
- Jiangkun Ouyang
- , Anne Swartjes
- & Roeland J. M. Nolte
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Article
| Open AccessGraphene transistors for real-time monitoring molecular self-assembly dynamics
Molecular self-assembly provides the desired functions to substrates, but investigation and control of its dynamics is challenging for the large area over which it must be detected. Here the authors report the use of graphene field effect devices to monitor with sub-second time resolution the photoinduced supramolecular assembly of a spiropyran derivative on graphene, covering an area of 100 × 100 μm2.
- Marco Gobbi
- , Agostino Galanti
- & Paolo Samorì
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Article
| Open AccessUltralong purely organic aqueous phosphorescence supramolecular polymer for targeted tumor cell imaging
Room-temperature phosphorescence has attracted attention for bioimaging, but quenching in aqueous systems is an issue. Here, the authors report on the synthesis of a water soluble organic phosphorescent polymer and demonstrate application is cancer cell targeting and imaging.
- Wei-Lei Zhou
- , Yong Chen
- & Yu Liu
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Article
| Open AccessWide range zero-thermal-quenching ultralong phosphorescence from zero-dimensional metal halide hybrids
Molecular luminescence is generally significantly quenched at high temperature. Here the authors report a zero-dimensional metal halide hybrid that exhibits zero-thermal-quenching ultralong phosphorescence over a wide temperature range of 220 K, and demonstrate use for Morse code encryption and logic gates.
- Shuya Liu
- , Xiaoyu Fang
- & Dongpeng Yan
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Article
| Open AccessTwo-photon excited deep-red and near-infrared emissive organic co-crystals
Two-photon excited near-infrared fluorescence materials have garnered considerable attention because of their superior optical properties compared with other optical materials. Here, the authors use a convenient and efficient supramolecular approach to synthesize a two-photon excited near-infrared emissive co-crystalline material.
- Yu Wang
- , Huang Wu
- & J. Fraser Stoddart
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Article
| Open AccessA molecular assembler that produces polymers
The feasibility of molecular assemblers as a device to control chemical reactions by positioning molecules with atomic precision is a matter of debate in the literature. Here the authors describe of a rudimentary synthetic molecular assembler, supramolecular aggregate of bifunctional surfactants produced by the reaction of two phase-separated reactants that produces polymers.
- Anthonius H. J. Engwerda
- & Stephen P. Fletcher
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Article
| Open AccessControl of seed formation allows two distinct self-sorting patterns of supramolecular nanofibers
Regulation of self-sorted nanofiber network patterns in double network hydrogels comprising supramolecular nanofibers is considered as key for potential applications. Here, the authors describe a selective construction of two distinct self-sorting network patterns, by controlling the kinetics of seed formation with dynamic covalent chemistry.
- Ryou Kubota
- , Kazutoshi Nagao
- & Itaru Hamachi
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Article
| Open AccessEqui–size nesting of Platonic and Archimedean metal–organic polyhedra into a twin capsid
Supramolecular constructs that mimic complex biological assemblies are synthetically challenging. Here, the authors present a double-shell cage wherein two independent metal-organic polyhedra are nested together in a manner analogous to that found in double-shell virus capsids.
- Hongmei Gan
- , Na Xu
- & Zhongmin Su
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Article
| Open AccessTransient dormant monomer states for supramolecular polymers with low dispersity
Monodisperse and well-defined self-assembled materials can be obtained by fuel-driven temporally controlled supramolecular polymerization via the buffered release of monomers. Here the authors show that a redox-responsive transient dormant state of monomer generated by redox reaction can lead to supramolecular polymers with low dispersity.
- Krishnendu Jalani
- , Anjali Devi Das
- & Subi J. George
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Article
| Open AccessSynthesis and assembly of extended quintulene
Quintulene, a quintuple non-graphitic cycloarene, is challenging to synthesize. Here, the authors synthesize and characterize the cone-shaped extended quintulene and its bilayer dimer, and disclose its dimerization as an entropy-driven, second-order reaction with a substantial activation energy.
- Hao Hou
- , Xin-Jing Zhao
- & Yuan-Zhi Tan
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Article
| Open AccessProtein-responsive protein release of supramolecular/polymer hydrogel composite integrating enzyme activation systems
Responsive hydrogels are of interest for diagnostic and controlled drug release applications. Here, the authors report on the design of a hydrogel with protein triggered release of an embedded protein through recovery of enzyme activity and subsequent degradation of supramolecular fibers.
- Hajime Shigemitsu
- , Ryou Kubota
- & Itaru Hamachi
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Article
| Open AccessSupramolecular double-stranded Archimedean spirals and concentric toroids
Connecting molecular-level phenomena to larger scales and molecular systems that resemble living systems remains a considerable challenge in supramolecular chemistry. Here, the authors report different self-assembly patterns in a porphyrin structure which can form – depending on the concentration - spirals or toroids.
- Norihiko Sasaki
- , Mathijs F. J. Mabesoone
- & Kazunori Sugiyasu
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Article
| Open AccessStructurally divergent dynamic combinatorial chemistry on racemic mixtures
Structurally divergent reactions on racemic mixtures, which produce distinct chemical species from an enantiomeric mixture, are extremely rare in the literature. Here, the authors are able to use a dynamic combinatorial approach to yield structurally divergent, non-isomeric [2]catenanes from an enantiomeric mixture.
- Tiberiu-M. Gianga
- & G. Dan Pantoș
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Article
| Open AccessForce generation by a propagating wave of supramolecular nanofibers
The rational design of spatiotemporal patterns in artificial molecular systems remains at an early stage of development. Here, the authors design a reaction network to control the formation and degradation of nanofibers by orthogonal chemical stimuli and describe force generation by a propagating wave of supramolecular nanofibers.
- Ryou Kubota
- , Masahiro Makuta
- & Itaru Hamachi
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Article
| Open AccessHeteroatom-bridged molecular belts as containers
Heteroatom-bearing molecular loops and belts are fascinating but generally difficult to synthesize. Here, the authors demonstrate that O,S-bridged double-stranded molecular belts—cyclophenoxathiins—can be successfully constructed and employed as versatile supramolecular hosts.
- Jialin Xie
- , Xia Li
- & Kelong Zhu
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Article
| Open Accessπ covalency in the halogen bond
Current models of halogen bonding describe the σ-symmetric component of this interaction but do not contemplate the possibility of π-covalency. Here the authors provide experimental and computational evidence of π-covalency in halogen bonds involving radical cation halogen bond donors.
- Cameron W. Kellett
- , Pierre Kennepohl
- & Curtis P. Berlinguette
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Article
| Open AccessEfficient self-assembly of heterometallic triangular necklace with strong antibacterial activity
Precise assembly of heterometallic complexes is a challenge. Here, the authors design a heterometallic triangular necklace through a highly efficient threading-and-ring-closing approach driven by metal-ligand coordination, which shows strong bacterium-binding and cell wall/plasma membrane-disrupting capacity for killing bacterial cells.
- Gui-Yuan Wu
- , Xueliang Shi
- & Hai-Bo Yang
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Article
| Open AccessCapturing transient antibody conformations with DNA origami epitopes
Understanding antibody-antigen interactions is important to deepen the understanding of immunology. Here, the authors report on the application of DNA origami structures for the controlled presentation of antigens to study antibody binding behaviours at room temperature.
- Ping Zhang
- , Xiaoguo Liu
- & Chunhai Fan
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Article
| Open AccessThe halogen bond with isocyano carbon reduces isocyanide odor
Carbon atoms of various species typically function as acceptors of noncovalent interactions when they are part of a π-system. Here, the authors report their discovery of a noncovalent halogen bond involving the isocyano carbon lone pair, which results in adducts with strongly reduced isocyanide odor.
- Alexander S. Mikherdov
- , Alexander S. Novikov
- & Vadim Yu. Kukushkin
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Article
| Open AccessA synthetic ion channel with anisotropic ligand response
Transmembrane proteins are important for cellular functions and synthetic analogues are of interest. Here the authors report on the design and testing of a synthetic multipass transmembrane channel which shows anisotropic responses to agonistic and antagonistic ligands.
- Takahiro Muraoka
- , Daiki Noguchi
- & Kazushi Kinbara
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Article
| Open AccessA host–guest approach to combining enzymatic and artificial catalysis for catalyzing biomimetic monooxygenation
Combining artificial and natural enzymes is a strategy to mimic biocatalytic processes with high efficiency and selectivity. This study reports a dual catalytic system composed of flavin adenine dinucleotide model and NADH mimics to catalyze the monooxygenation of cyclobutanones and thioethers.
- Liang Zhao
- , Junkai Cai
- & Chunying Duan
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Article
| Open AccessA nanomaterials discovery robot for the Darwinian evolution of shape programmable gold nanoparticles
The ability to discover and optimise the synthesis of inorganic nanomaterials has significant impact on various fields, from sensing to medicine. Here, the authors use a genetic algorithm to drive a robotic platform toward a pre-defined, spectroscopic goal in order to discover and optimise the conditions for several nanoparticle shapes.
- Daniel Salley
- , Graham Keenan
- & Leroy Cronin
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Article
| Open AccessA supramolecular system that strictly follows the binding mechanism of conformational selection
Conformational selection is one of the two dominant binding mechanisms in biology, but has rarely been studied in synthetic systems. Here, the authors report a supramolecular system that strictly follows the binding mechanism of conformational selection.
- Liu-Pan Yang
- , Li Zhang
- & Wei Jiang
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Article
| Open AccessA cyclic bis[2]catenane metallacage
Catenated cages are challenging synthetic targets in chemistry. Here, the authors employ a multi-component coordination strategy using a Pt(II) heteroligation to construct a cyclic bis[2]catenane metallacage, which could be reversibly transformed between the catenated structure and the bis-metallacage.
- Yiliang Wang
- , Yicheng Zhang
- & Peter J. Stang
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Article
| Open AccessHelical supramolecular polymers with rationally designed binding sites for chiral guest recognition
Since various helical supramolecular polymers became available, their application in molecular chirality recognition have been anticipated but not extensively studied. Here, the authors report the application of a helical supramolecular polymer for the enantio separation of chiral guest molecules.
- Krishnachary Salikolimi
- , Vakayil K. Praveen
- & Yasuhiro Ishida
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Article
| Open AccessCombining high-resolution scanning tunnelling microscopy and first-principles simulations to identify halogen bonding
Scanning tunnelling microscopy (STM) is commonly used to study 2D molecular self-assembly but is not always enough to fully solve a supramolecular structure. Here, the authors combine a high-resolution version of STM with first-principles simulations to precisely identify halogen bonding in polycyclic aromatic molecules.
- James Lawrence
- , Gabriele C. Sosso
- & Giovanni Costantini
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Article
| Open AccessUniversally autonomous self-healing elastomer with high stretchability
Developing autonomous self-healing materials for application under extreme conditions is challenging. Here, the authors design a highly stretchable elastomer by incorporation of H-bonds and disulphide methathesis, which shows efficient self-healing under extreme conditions.
- Hongshuang Guo
- , Yi Han
- & Lei Zhang
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Article
| Open AccessDynamic wrinkling pattern exhibiting tunable fluorescence for anticounterfeiting applications
Dynamic surface patterns are widely used in information security and anticounterfeiting technologies. Here, the authors demonstrated a dynamic wrinkled and fluorescent pattern using a supramolecular network in which both the wrinkle morphology and fluorescence color can be regulated by pH or light.
- Tianjiao Ma
- , Tiantian Li
- & Xuesong Jiang
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Article
| Open AccessIn situ supramolecular polymerization-enhanced self-assembly of polymer vesicles for highly efficient photothermal therapy
Photothermal therapy (PTT) has recently emerged as a promising approach for cancer therapy. Here, the authors report a hyperbranched polymer vesicle with favorable photothermal stability and high photothermal efficiency for PTT through a supramolecular polymerization-enhanced self-assembly strategy.
- Yannan Liu
- , Hao Wang
- & Yongfeng Zhou
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Article
| Open AccessIntercellular communication between artificial cells by allosteric amplification of a molecular signal
The principles of intercellular communication in multicellular organisms can be explored using artificial cells. Here, the authors report on giant vesicles which can recognize diffused chemical signals and amplify the signal by synthetic enzymatic cascades to allow signal propagation over long distances.
- Bastiaan C. Buddingh’
- , Janneke Elzinga
- & Jan C. M. van Hest
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Article
| Open AccessSingle crystal of a one-dimensional metallo-covalent organic framework
Although polymers have been studied for well over a century, there are few examples of covalently linked polymer crystals synthesized directly from solution. Here, the authors demonstrate a strategy to synthesize single crystalline 1D metallo-covalent organic frameworks by combining dynamic covalent chemistry and metal-ligand coordination.
- Hai-Sen Xu
- , Yi Luo
- & Kian Ping Loh
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Article
| Open AccessDecorating bacteria with self-assembled synthetic receptors
Cell surface proteins mediate the interactions between cells and their extracellular environment. Here the authors design synthetic biomemetic receptor-like sensors that facilitate programmable interactions between bacteria and their target.
- Naama Lahav-Mankovski
- , Pragati Kishore Prasad
- & David Margulies
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Article
| Open AccessMechanochemical synthesis of pillar[5]quinone derived multi-microporous organic polymers for radioactive organic iodide capture and storage
Incorporation of supramolecular macrocycles into porous organic polymers can increase uptake of guest molecules through host−guest interactions. Here the authors report a pillar[5]quinone derived multi-microporous organic polymer, which show a superior performance in radioactive iodomethane capture and storage.
- Kecheng Jie
- , Yujuan Zhou
- & Sheng Dai
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Article
| Open AccessColor-tunable ultralong organic room temperature phosphorescence from a multicomponent copolymer
Functional materials displaying tunable emission and long-lived luminescence are a powerful tool in information encryption, organic electronics and bioelectronics. Here the authors design a color-tunable ultralong organic room temperature phosphorescence polymer through radical multiple component cross-linked copolymerization.
- Long Gu
- , Hongwei Wu
- & Yanli Zhao
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Article
| Open AccessSelf-assembled conjoined-cages
Developing simple routes for construction of multi-compartmental cages is a compelling and challenging task. Here, the authors report modular construction of multi-3D-cavity cages featuring one, two or three units of a [Pd2L4] entity conjoined with a [Pd3L6] core.
- Sagarika Samantray
- , Shobhana Krishnaswamy
- & Dillip K. Chand
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Article
| Open AccessWeak functional group interactions revealed through metal-free active template rotaxane synthesis
Weak interactions between functional groups are often difficult to characterize in host–guest complexes. Here, the authors report the metal-free active template synthesis of a series of rotaxanes that permit a range of kinetically stabilized, weak crown ether-axle interactions to be characterized in solution and the solid state.
- Chong Tian
- , Stephen D. P. Fielden
- & David A. Leigh