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| Open AccessOne-pot universal initiation-growth methods from a liquid crystalline block copolymer
Construction of hierarchical nanostructures is important in material science, but precise morphological control remains a challenge. Here, the authors report a one-pot in-situ initiation-growth process from a liquid crystalline block copolymer to precisely control the morphology and dimensions of hierarchical nanostructures.
- Bixin Jin
- , Koki Sano
- & Xiaoyu Li
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Article
| Open AccessSuperlattice by charged block copolymer self-assembly
Understanding the phase behavior of charged block copolymers may potentially lead to unexplored self-assembled morphologies. Here, the authors report the preparation of ion-containing diblock copolymers featuring a superlattice state varying between disordered and lamellar morphologies depending on the charge density.
- Jimin Shim
- , Frank S. Bates
- & Timothy P. Lodge
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| Open AccessCoordination-driven self-assembly of a molecular figure-eight knot and other topologically complex architectures
Molecular knots and links continue to fascinate synthetic chemists. Here, the authors use stacking and hydrogen-bonding interactions between a set of similar building blocks to construct several complex molecular topologies, including a figure-eight knot and a trefoil knot.
- Li-Long Dang
- , Zhen-Bo Sun
- & Guo-Xin Jin
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Article
| Open AccessPolyaromatic nanocapsules as photoresponsive hosts in water
Photoresponsive molecular capsules that can be used in water are rare. Here, the authors construct polyaromatic nanocapsules via self-assembly from photoswitch-bearing amphiphilic molecules in water. Light induces a structural change in the amphiphiles, triggering the capsule to disassemble into monomers and release encapsulated guests.
- Lorenzo Catti
- , Natsuki Kishida
- & Michito Yoshizawa
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| Open AccessEnzyme-responsive progelator cyclic peptides for minimally invasive delivery to the heart post-myocardial infarction
Injectable hydrogels have gained significant interest; yet, due to high viscosity, many are unsuitable for catheter delivery. Here, the authors report on cyclic peptides with low viscosity for catheter delivery, which form self-assembled peptide hydrogels following enzymatic cleavage and demonstrated delivery in vivo.
- Andrea S. Carlini
- , Roberto Gaetani
- & Nathan C. Gianneschi
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| Open AccessPlant leaves inspired sunlight-driven purifier for high-efficiency clean water production
Natural leaves can purify water under sunlight through a combination of osmotic pressure, transpiration, and guttation effects. Here the authors design a composite material mimicking these combined effects, achieving sunlight-driven pure water production from brine with high collection rate.
- Hongya Geng
- , Qiang Xu
- & Chun Li
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Article
| Open AccessTemperature-controlled repeatable scrambling and induced-sorting of building blocks between cubic assemblies
In this paper, the authors study the temperature-controlled dynamic behavior of a system of nanocubes self-assembled from two different building blocks. Non-intuitively, the disordered, equilibrium state (a mixture of heteroleptic cubes) and the ordered, out-of-equilibrium state (a mixture of homoleptic cubes) are cycled by heating and subsequent rapid cooling.
- Yi-Yang Zhan
- , Tatsuo Kojima
- & Shuichi Hiraoka
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| Open AccessWater-mediated deracemization of a bisporphyrin helicate assisted by diastereoselective encapsulation of chiral guests
Deracemization is a powerful method which allows transformation of racemic mixtures into excess enantiomer, but was applied only to small chiral molecular systems so far. Here the authors report deracemization of a kinetically stable bisporphyrin helicate upon encapsulation of chiral aromatic guests.
- Naoki Ousaka
- , Shinya Yamamoto
- & Eiji Yashima
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| Open AccessControllable hierarchical self-assembly of porphyrin-derived supra-amphiphiles
The supra-amphiphiles spontaneously assemble to well-defined nanostructures but control of shape and size of supramolecular nanostructures is still a great challenge. Here the authors demonstrate control over shape and size of self-assemblies by using the recognition motifs of an amphiphilic porphyrin
- Shu-Ping Wang
- , Wei Lin
- & Shijun Li
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| Open AccessScalable preparation of alternating block copolymer particles with inverse bicontinuous mesophases
Block copolymer particles with controlled morphologies play a vital role in materials science and nanotechnology. Here the authors show a scalable preparation of amphiphilic alternating block polymer particles with inverse bicontinuous mesophases via polymerization-induced self-assembly.
- Fei Lv
- , Zesheng An
- & Peiyi Wu
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Article
| Open AccessAutonomous helical propagation of active toroids with mechanical action
Self-assembly in nature is dynamic and exists in out-of-equilibrium state and thus systems have the ability to autonomously respond to environmental changes. Here the authors report that input of thermal energy can trigger fixed, artificial toroids to spontaneously nucleate helical growth.
- Bowen Shen
- , Youliang Zhu
- & Myongsoo Lee
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Article
| Open AccessHarnessing liquid-in-liquid printing and micropatterned substrates to fabricate 3-dimensional all-liquid fluidic devices
Non-equilibrium systems of immiscible liquids have significant potential to advance different technologies, but control over morphology or functionality remains unexplored. Here, the authors demonstrate an all-liquid fluidic device by exploiting surfactant assemblies to produce a semi-permeable membrane between the liquids.
- Wenqian Feng
- , Yu Chai
- & Brett A. Helms
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Article
| Open AccessSites of high local frustration in DNA origami
Self-assembly of DNA origami is a complex folding problem without a unified view of the energetic factors involved. Here the authors analyse identical structures that differ by nucleotide sequence and identify how mechanical stress at nucleation sites shapes the energy landscape.
- Richard Kosinski
- , Ann Mukhortava
- & Barbara Saccà
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Article
| Open AccessA chemically fuelled self-replicator
Understanding how simple chemical mixtures transition into truly emergent systems is essential to create new lifelike materials. Here, the authors show a self-replicating system that can be maintained out-of-equilibrium by an oxidant fuel in analogy to simple metabolic cycles.
- Sarah M. Morrow
- , Ignacio Colomer
- & Stephen P. Fletcher
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| Open AccessProgramming chain-growth copolymerization of DNA hairpin tiles for in-vitro hierarchical supramolecular organization
Formation of biological filaments via intracellular supramolecular polymerization of proteins occurs under programmable and spatiotemporal control to maintain integrity. Here the authors devise a bioinspired isothermal chain-growth approach to programmably copolymerize DNA hairpin tiles into 1D nanofilaments.
- Honglu Zhang
- , Yu Wang
- & Chunhai Fan
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Article
| Open AccessMultimodal switching of a redox-active macrocycle
Molecules that can switch between multiple stable states in response to stimuli are promising for many applications, but are challenging to construct. Here, the authors design a resorcinarene switching manifold with multiple oxidation states and coupled charge-transfer states, which can access up to five distinct switch-states with unique optical outputs.
- Daniel T. Payne
- , Whitney A. Webre
- & Jonathan P. Hill
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Article
| Open AccessMetal–peptide rings form highly entangled topologically inequivalent frameworks with the same ring- and crossing-numbers
For interlocking ring structures, knot theory predicts that the number of topologically different links increases with ring and crossing number. Here, the authors use a peptide folding-and-assembly strategy to selectively realize two highly entangled catenanes with 4 rings and 12 crossings, representing two of the 100 predicted topologies with this complexity.
- Tomohisa Sawada
- , Ami Saito
- & Makoto Fujita
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| Open AccessHalogen bonding as a supramolecular dynamics catalyst
The halogen bond is well known for its ability to assemble supramolecules. Here, using NMR experiments, the authors reveal the role of these bonds in dynamic processes, finding that the halogen bond directly catalyzes dynamical rotation in solid cocrystals by reducing the associated energy barrier.
- Patrick M. J. Szell
- , Scott Zablotny
- & David L. Bryce
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| Open AccessDouble helical conformation and extreme rigidity in a rodlike polyelectrolyte
Double helix structures appear widely in nature, but only rarely in synthetic non-chiral macromolecules. Here the authors describe a double helix in a densely charged aromatic polyamide, which exhibits an axial rigidity persistence length of ~ 1 μm, much higher than that of DNA (~ 50 nm).
- Ying Wang
- , Yadong He
- & Louis A. Madsen
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| Open AccessStable radical anions generated from a porous perylenediimide metal-organic framework for boosting near-infrared photothermal conversion
Perylenediimide (PDI) radical anions show promise as photothermal agents for phototherapy, but are typically very unstable. Here the authors fabricate a PDI-based metal-organic framework where the PDI units become stable radical anions upon incorporation of amine vapors.
- Baozhong Lü
- , Yifa Chen
- & Meizhen Yin
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| Open AccessPermanent porous hydrogen-bonded frameworks with two types of Brønsted acid sites for heterogeneous asymmetric catalysis
The search for porous materials with strong Brønsted acid sites for challenging chemical reactions has been of significant interest, but remains challenging. Here the authors report a cage extension strategy to construct chiral permanent porous hydrogen-bonded frameworks with strong Brønsted acid groups for heterogeneous asymmetric catalysis.
- Wei Gong
- , Dandan Chu
- & Yan Liu
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Article
| Open AccessFlexible decapyrrylcorannulene hosts
The structures of fullerenes, or buckyballs, are often very difficult to resolve. Here, the authors describe a decapyrrylcorannulene host with ten flexible pyrryl groups that can efficiently co-crystallize with diverse fullerene derivatives in a ‘hand-ball-hand’ fashion, allowing crystallographic identification of commonly known types of fullerenes.
- Yun-Yan Xu
- , Han-Rui Tian
- & Lan-Sun Zheng
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Article
| Open AccessMolecular weight fractionation by confinement of polymer in one-dimensional pillar[5]arene channels
Confinement of polymers in nano-spaces can induce unique molecular dynamics and properties. Here the authors show high mass fractionation by the confinement of single polymer chains of poly(ethylene oxide) in the one-dimensional channels of crystalline pillar[5]arene.
- Tomoki Ogoshi
- , Ryuta Sueto
- & Motohiro Mizuno
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| Open AccessChemical fuel-driven living and transient supramolecular polymerization
Temporal control over self-assembly processes is a desirable trait for discovering adaptable and controllable materials. Here the authors show that a chemical fuel driven system can not only self-assemble in a controlled manner, but can also result in precise control over the assembly and disassembly kinetics.
- Ankit Jain
- , Shikha Dhiman
- & Subi J. George
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| Open AccessMolecular memory with downstream logic processing exemplified by switchable and self-indicating guest capture and release
While many processes in biological cells can be understood in terms of molecular logic gates that process information sequentially and combinationally, the design and construction of such devices in the laboratory are unknown. Here the authors achieve this by the reversibly-controlled capture and release of guest molecules from host containers.
- Brian Daly
- , Thomas S. Moody
- & A. Prasanna de Silva
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| Open AccessHalogen-bonded cocrystallization with phosphorus, arsenic and antimony acceptors
Halogen bonding can be exploited for the design of functional supramolecular materials, but heavier elements that are known to accept a halogen bond remain limited. Here, the authors demonstrate the formation of two-component cocrystals based on halogen bonds with phosphorus, arsenic and antimony.
- Katarina Lisac
- , Filip Topić
- & Dominik Cinčić
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Article
| Open AccessMolecular Russian dolls
Hierarchical non-intertwined ring-in-ring complexes are intriguing but challenging supramolecular targets. Here, the authors describe a box-in-box assembly based on radical-pairing interactions between two rigid diradical dicationic cyclophanes; the inner box can further accommodate guests to form Russian doll-like assemblies.
- Kang Cai
- , Mark C. Lipke
- & J. Fraser Stoddart
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Article
| Open AccessManipulating and monitoring nanoparticles in micellar thin film superstructures
Understanding how nanoparticle superstructures respond to external stimuli is of importance to their potential application. Here, the authors demonstrate the use of cryo-transmission electron microscopy for monitoring and manipulating movement within nanoparticle-loaded dendrimicelle superstructure thin films upon irradiation with an electron beam.
- Jan Bart ten Hove
- , Fijs W. B. van Leeuwen
- & Aldrik H. Velders
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| Open AccessNanoribbons self-assembled from short peptides demonstrate the formation of polar zippers between β-sheets
Peptide self-assembly is a hierarchical process which includes forming β-sheets but the formation of high ordered structures remains largely unexplored. Here the authors report on a super-secondary structural template, based on well-defined hydrogen bonds by rational design and assembly of short peptides
- Meng Wang
- , Jiqian Wang
- & Hai Xu
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Article
| Open AccessInterconvertible vanadium-seamed hexameric pyrogallol[4]arene nanocapsules
Adapting the cavity of a coordination capsule generally involves the addition or removal of subcomponents. Here, the authors report two vanadium-organic coordination nanocapsules with the same number of components but variable cavity sizes—an expanded ball and contracted octahedron—whose solvent-controlled interconversion is attributed to the versatile coordination geometry of the vanadium centers.
- Kongzhao Su
- , Mingyan Wu
- & Maochun Hong
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| Open AccessTwo-dimensional tessellation by molecular tiles constructed from halogen–halogen and halogen–metal networks
Molecular tessellations of complex tilings are difficult to design and construct. Here, the authors show that molecular tessellations can be formed from a single building block that gives rise to two distinct supramolecular phases, whose self-similar subdomains serve as tiles in the periodic tessellations.
- Fang Cheng
- , Xue-Jun Wu
- & Kian Ping Loh
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| Open AccessSelf-assembly of polycyclic supramolecules using linear metal-organic ligands
Coordination-driven supramolecular assembly provides the ability to build molecular architectures of impressive complexity. Here, the authors use a series of linear metal-organic ligands with specific sequences to construct multiple generations of precisely-controlled, 2D fractal polycyclic supramolecules.
- Bo Song
- , Sneha Kandapal
- & Xiaopeng Li
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Article
| Open AccessInduced-fit expansion and contraction of a self-assembled nanocube finely responding to neutral and anionic guests
Induced-fit binding, common in biological systems, is still relatively rare in artificial hosts. Here, the authors assemble a molecular cube from six gear-shaped faces, whose interdigitated design allows the cube to expand and contract in response to the size, shape, and charge of a guest molecule.
- Yi-Yang Zhan
- , Tatsuo Kojima
- & Shuichi Hiraoka
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Article
| Open AccessDynamics of individual molecular shuttles under mechanical force
Molecular shuttles are bi-stable and stimuli-responsive systems that are considered potential elements for molecular machinery. Here, the authors use optical tweezers to measure the force dependent real-time kinetics of individual molecular shuttles under aqueous conditions.
- Teresa Naranjo
- , Kateryna M. Lemishko
- & Borja Ibarra
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Article
| Open AccessRewriting the phase diagram of a diamagnetic liquid crystal by a magnetic field
Magnetically induced phase behaviour in a soft matter system is of potential interest for magneto-responsive compounds. Here the authors fabricate a discotic ionic liquid crystalline hybrid material which can be switched from orthorhombic to cubic phase in the absence or presence of a strong magnetic field.
- Fatin Hajjaj
- , Takashi Kajitani
- & Takanori Fukushima
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| Open AccessDesign and self-assembly of hexahedral coordination cages for cascade reactions
Supramolecular containers are promising enzyme mimics, but they currently accommodate only a limited range of chemical transformations. Here, the authors describe coordination cages that catalyze two-component cascade reactions without relying on an external or encapsulated catalytic species.
- Jingjing Jiao
- , Zijian Li
- & Yong Cui
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Article
| Open AccessCramming versus threading of long amphiphilic oligomers into a polyaromatic capsule
Molecular capsules typically bind only guests with volumes smaller than their cavities. Here, the authors find that a polyaromatic capsule accommodates linear amphiphilic oligomers in a length-dependent manner, whereas short chains are fully crammed into the cavity, long chains can be incorporated into the capsule in a threaded fashion.
- Masahiro Yamashina
- , Shunsuke Kusaba
- & Michito Yoshizawa
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| Open AccessCooperative supramolecular polymers with anthracene‒endoperoxide photo-switching for fluorescent anti-counterfeiting
There is a continual pursuit for different ways to detect counterfeiting in today’s society. Here the authors show photo-responsive supramolecular polymers can be used in fluorescent anti-counterfeit applications, by taking advantage of multicycle anthracene‒endoperoxide switching properties.
- Zhao Gao
- , Yifei Han
- & Feng Wang
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Article
| Open AccessChiral self-sorted multifunctional supramolecular biocoordination polymers and their applications in sensors
Chiral supramolecules may be used in chiral recognition, sensing and catalysis. Here the authors selectively synthesized homochiral and heterochiral supramolecular biocoordination polymers of naphthalene diimide ligands with alanine termini and Zn ions.
- Xiaobo Shang
- , Inho Song
- & Joon Hak Oh
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Article
| Open AccessModulating the hierarchical fibrous assembly of Au nanoparticles with atomic precision
Constructing nanoparticle assemblies with atomic precision remains a major challenge in nanoscience. Here, the authors realize atomic‐level control over the 1D, 2D and hierarchical 3D assembly of Au nanoparticles by modulating the site‐specific surface ligands and associated counterions.
- Qi Li
- , Jake C. Russell
- & Rongchao Jin
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Article
| Open AccessMacroscopic helical chirality and self-motion of hierarchical self-assemblies induced by enantiomeric small molecules
Chirality transfer by chemical self-assembly has been studied intensively for years but chirality transfers along the same path remains elusive. Here the authors use a multiscale chemo-mechanical model to elucidate the mechanism underlying the chirality transfer via self-assembly in hierarchical camphorsulfonic acid doped polyaniline.
- Yang Yang
- , Jie Liang
- & Zhixiang Wei
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Article
| Open AccessConcyclic CH-π arrays for single-axis rotations of a bowl in a tube
The weak and directional CH-π hydrogen bond has rarely been exploited in the design of supramolecular complexes and molecular machinery. Here, the authors construct a bowl-in-tube complex stabilized solely by concyclic CH-π hydrogen bonds, and show that the guest exhibits single-axis rotational motion despite tight association with the host.
- Taisuke Matsuno
- , Masahiro Fujita
- & Hiroyuki Isobe
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Article
| Open AccessBinder driven self-assembly of metal-organic cubes towards functional hydrogels
A possible route to producing processable soft materials is by assembling metal organic cubes into hydrogels. Here the authors show charge-assisted H-bond driven self-assembly of Ga3+-based anionic metal organic cubes and suitable molecular binders towards multi-functional hydrogels.
- Papri Sutar
- , Venkata M. Suresh
- & Tapas Kumar Maji
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Article
| Open AccessAmplification of chirality in surface-confined supramolecular bilayers
One of the most dramatic effects of supramolecular assembly is the generation of homochirality in near-racemic systems. Here the authors rationalize the chiral amplification mechanism with a combined scanning tunneling microscopy and modelling study of surface-grown enantiomerically unbalanced supramolecular bilayers.
- Hai Cao
- & Steven De Feyter
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Article
| Open AccessQuantum confined peptide assemblies with tunable visible to near-infrared spectral range
Quantum confined (QC) materials have favorable photoluminescent properties, yet are less bioavailable. Here, the authors developed aromatic cyclo-dipeptides that assemble into quantum dots and organize into biocompatible QC supramolecular structures suitable for in vivo imaging and optoelectronics.
- Kai Tao
- , Zhen Fan
- & Junbai Li
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Article
| Open AccessDual stimuli-responsive rotaxane-branched dendrimers with reversible dimension modulation
Mechanically interlocked molecules are extensively applied as artificial molecular machines but rotaxane-branched dendrimers are rarely explored because of synthetic challenges. Here the authors present the construction of dual stimuli-responsive rotaxane-branched dendrimer which can be stimulated by DMSO or acetate ions.
- Xu-Qing Wang
- , Wei Wang
- & Hai-Bo Yang
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Article
| Open AccessMapping the energy landscapes of supramolecular assembly by thermal hysteresis
Complex assembly pathways often involve transient, partly-formed intermediates that are challenging to characterize. Here, the authors present a simple and rapid spectroscopic thermal hysteresis method for mapping the energy landscapes of supramolecular assembly.
- Robert W. Harkness V
- , Nicole Avakyan
- & Anthony K. Mittermaier
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| Open AccessDiscovering privileged topologies of molecular knots with self-assembling models
Only a few different types of supramolecular knots have been synthesized so far. Here the authors use Monte Carlo sampling, molecular dynamics and combinatorics to discover new knot types made of identical templates.
- Mattia Marenda
- , Enzo Orlandini
- & Cristian Micheletti
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| Open AccessAn isolable catenane consisting of two Möbius conjugated nanohoops
Molecules exhibiting Möbius topology are fascinating but challenging synthetic targets. Here, the authors report the elegant synthesis and crystal structure of a catenane formed from two fully conjugated, interlocked Möbius nanohoops, and use theoretical calculations to understand its conformational stability and aromaticity.
- Yang-Yang Fan
- , Dandan Chen
- & Huan Cong