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Article
| Open AccessPropagating wave in a fluid by coherent motion of 2D colloids
Tiny movable components could generate macroscopic mechanical motion if precise coherent operation can be exerted simultaneously. Here, the authors demonstrate this by using 10^10 pieces of colloidally dispersed nanosheets to generate wave under non-equilibrium state.
- Koki Sano
- , Xiang Wang
- & Takuzo Aida
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Article
| Open AccessSupramolecular fibrillation of peptide amphiphiles induces environmental responses in aqueous droplets
One-dimensional (1D) supramolecular polymers are commonly found in natural and synthetic systems but very little is currently known about the physico-chemical consequences and functional role of 1D supramolecular polymerisation confined in aqueous compartments. Here, the authors describe the different phenomena that resulted from the chemically triggered supramolecular fibrillation of synthetic peptide amphiphiles inside water microdroplets.
- Richard Booth
- , Ignacio Insua
- & Javier Montenegro
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Article
| Open AccessSupramolecular tessellations by the exo-wall interactions of pagoda[4]arene
Supramolecular tessellation has gained increasing interest in supramolecular chemistry for its structural aesthetics and potential applications in optics, magnetics and catalysis. Here, the authors expand the examples of molecular building blocks for supramolecular tessellation and fabricate supramolecular tessellations using the exo-wall interactions of pagoda[4]arene.
- Xiao-Ni Han
- , Ying Han
- & Chuan-Feng Chen
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Article
| Open AccessA chemosensor-based chiral coassembly with switchable circularly polarized luminescence
‘Fluorescent chemisensors with fast response time and pronounced luminescence variation are important but have not been well investigated for self-assembled chiral systems. Here, the authors present a coassembled multiple component system that responds to SO2 derivatives, giving rise to dynamic aggregation behaviors and switchable luminescence as well as circularly polarized luminescence.
- Qiuhong Cheng
- , Aiyou Hao
- & Pengyao Xing
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Article
| Open AccessTuneable separation of gold by selective precipitation using a simple and recyclable diamide
The separation of metals from electronic waste is an enduring technological and societal challenge, and new metal extraction, refining and recycling solutions are needed. Here the authors report a recyclable and tuneable chemical reagent that separates valuable metals such as gold by direct and selective precipitation from various acidic, mixed-metal solutions of relevance to extraction and recycling industries.
- Luke M. M. Kinsman
- , Bryne T. Ngwenya
- & Jason B. Love
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Article
| Open AccessTopology-transformable block copolymers based on a rotaxane structure: change in bulk properties with same composition
The topology of a polymer is normally a fixed property of the material, derived from the characteristic of the monomers and their linkages. Here the authors present a method to transform the topology of block copolymers containing rotaxane linkages via acetylation.
- Hiroki Sato
- , Daisuke Aoki
- & Toshikazu Takata
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Article
| Open AccessA class of organic cages featuring twin cavities
The preparation of nanocages with unprecedented architectures may lead to new functions. Here the authors report the self-assembly of organic cages featuring twin cavities; the geometry and pocket size determine the molecular packing and the proton conductivity performance.
- Zhenyu Yang
- , Chunyang Yu
- & Shaodong Zhang
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Matters Arising
| Open AccessThe mechanism of bending in co-crystals of caffeine and 4-chloro-3-nitrobenzoic acid
- Amy J. Thompson
- , Jason R. Price
- & Jack K. Clegg
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Article
| Open AccessCoupling complementary strategy to flexible graph neural network for quick discovery of coformer in diverse co-crystal materials
Experimental determination of new cocrystals remains challenging due to the need of a systematic screening with a large range of coformers. Here the authors develop a flexible deep learning framework based on graph neural network demonstrated to quickly predict the formation of co-crystals.
- Yuanyuan Jiang
- , Zongwei Yang
- & Xuemei Pu
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Article
| Open AccessProliferating coacervate droplets as the missing link between chemistry and biology in the origins of life
Coacervate droplets (CDs) are a model for protocells formed by liquid-liquid phase separation (LLPS), but protocell models able to proliferate remain undeveloped. Here, the authors report a proliferating peptide-based CD using synthesised amino acid thioesters as monomers, which could concentrate RNA and lipids, enabling RNA to protect the droplet from dissolution by lipids.
- Muneyuki Matsuo
- & Kensuke Kurihara
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Article
| Open AccessA contorted nanographene shelter
Encapsulating large and contorted nanographenes inside artificial receptors remain challenging. This work reports the synthesis, characterization and binding properties of a trigonal prismatic cage compound that can serve as a receptor for contorted nanographene derivatives.
- Huang Wu
- , Yu Wang
- & J. Fraser Stoddart
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Article
| Open AccessA hybrid molecular peapod of sp2- and sp3-nanocarbons enabling ultrafast terahertz rotations
Mechanical motions in hybrid sp2/sp3 -hybrid nanocarbon peapods might lead to promising materials applications, but have been insufficiently explored. Here the authors demonstrate that a diamondoid molecule trapped inside a carbonaceous cylinder undergoes solid-state rotations at terahertz frequencies.
- Taisuke Matsuno
- , Seiya Terasaki
- & Hiroyuki Isobe
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Article
| Open AccessA host–guest semibiological photosynthesis system coupling artificial and natural enzymes for solar alcohol splitting
Abiotic–biotic hybrid systems are promising to trap light for fuel and chemical transformation with high efficacy and selectivity. This study reports a coenzyme-mediated supramolecular host-guest semibiological system combining supramolecular catalyst and enzymes for solar alcohol splitting.
- Junkai Cai
- , Liang Zhao
- & Chunying Duan
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Article
| Open AccessMethyl groups as widespread Lewis bases in noncovalent interactions
Tetrel bonds are noncovalent interactions between electron donors and group 14 elements; in these situations, C(sp3) atoms can act as Lewis acids, accepting electron density. Here, the authors show that methyl groups, when bound to atoms less electronegative than carbon, can participate in noncovalent interactions as electron density donors.
- Oliver Loveday
- & Jorge EcheverrÃa
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Article
| Open AccessLight-fueled transient supramolecular assemblies in water as fluorescence modulators
Dissipative self-assembly, which requires a continuous supply of fuel to maintain the assembled states far from equilibrium, is the foundation of biological systems but it remains a challenge to introduce light as fuel into artificial dissipative self-assemblies. Here, the authors report an artificial dissipative self-assembly system that is constructed from light-induced amphiphiles.
- Xu-Man Chen
- , Xiao-Fang Hou
- & Quan Li
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Article
| Open AccessRapid discovery of self-assembling peptides with one-bead one-compound peptide library
Self-assembling peptides have a range of potential applications but developing self-assembling sequences can be challenging. Here, the authors report on a one-bead one-compound combinatorial library where fluorescence is used to detect the potential for self-assembly and identified candidates are evaluated.
- Pei-Pei Yang
- , Yi-Jing Li
- & Kit S. Lam
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Article
| Open AccessAstral hydrogels mimic tissue mechanics by aster-aster interpenetration
The development of tissue-like materials which replicate the mechanical properties of tissue is of interest for a range of applications. Here, the authors report on the development of radial asters that form a gel network to stiffen in compression and soften in extension, resembling tissue mechanics.
- Qingqiao Xie
- , Yuandi Zhuang
- & Lingxiang Jiang
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Article
| Open AccessIntegration of photocatalytic and dark-operating catalytic biomimetic transformations through DNA-based constitutional dynamic networks
Nucleic acid-based constitutional dynamic networks (CDNs) enable control of various catalytic processes, but it is challenging to achieve intercommunication between different CDNs and by that mimic complex cell biology networks. Here, the authors report two CDNs that control the integration of photochemical and dark-operating processes, and show their intercommunication afforded by environmental components.
- Chen Wang
- , Michael P. O’Hagan
- & Itamar Willner
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Article
| Open AccessSelf-assembly using a retro Diels-Alder reaction
Despite their great utility in synthetic and materials chemistry, Diels-Alder and retro Diels-Alder reactions have been vastly unexplored in promoting self-assembly processes. Here the authors show the release of steric bulkiness associated with a bridged bicyclic Diels Alder adduct by the retro Diels-Alder reaction that allowed generation of two building blocks that spontaneously self-assembled to form a supramolecular polymer.
- Jaeyoung Park
- , Jung-Moo Heo
- & Jong-Man Kim
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Article
| Open AccessA curved host and second guest cooperatively inhibit the dynamic motion of corannulene
The preparation of artificial host–guest systems that display dynamic adaptation during guest binding is challenging. Here the authors report a chiral self-assembled tetrahedral cage featuring curved walls that reconfigures stereochemically to fit fullerene guests, regulates corannulene inversion, and enables the determination of co-guest enantiomeric excess by NMR spectroscopy.
- Yang Yang
- , Tanya K. Ronson
- & Jonathan R. Nitschke
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Article
| Open AccessPolymer cyclization for the emergence of hierarchical nanostructures
Synthetic polymer nano-objects with well-defined hierarchical structures are important for a wide range of applications such as nanomaterial synthesis, catalysis, and therapeutics. Here the authors demonstrate the strategy of fabricating controlled hierarchical structures through self-assembly of folded synthetic polymers.
- Chaojian Chen
- , Manjesh Kumar Singh
- & Tanja Weil
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Article
| Open AccessHigh-pressure reversibility in a plastically flexible coordination polymer crystal
Mechanically flexible single crystals are promising materials for advanced technological applications. Here, the authors study the high pressure response of a plastically flexible coordination polymer and provide indication of an overall disparate mechanical response of bulk flexibility and quasi-hydrostatic compression within the same crystal lattice.
- Xiaojiao Liu
- , Adam A. L. Michalchuk
- & Colin R. Pulham
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Article
| Open AccessSelf-assembly of an anion receptor with metal-dependent kinase inhibition and potent in vitro anti-cancer properties
Artificial self-assembling systems such as anion receptors or ‘binders’ are largely unexplored for therapeutic applications. Here, the authors report self-assembling trimetallic cryptands containing copper, zinc or manganese that encapsulate a range of anions, are highly toxic to human cancer cell lines and show metal-dependent selectivity towards cancer vs. healthy cells linked to the selective inhibition of multiple kinases.
- Simon J. Allison
- , Jaroslaw Bryk
- & Craig R. Rice
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Article
| Open AccessActive coacervate droplets are protocells that grow and resist Ostwald ripening
Active coacervate droplets are droplets coupled to a chemical reaction that maintains them out of equilibrium, which can be used to drive active processes, but coacervates are still subject to passive processes that compete with or mask growth. Here, the authors present a nucleotide-based model for active coacervate droplets that form and grow by fuel-driven synthesis of ATP, and, importantly, do not undergo Ostwald ripening.
- Karina K. Nakashima
- , Merlijn H. I. van Haren
- & Evan Spruijt
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Article
| Open AccessEfficient ethylene purification by a robust ethane-trapping porous organic cage
The removal of ethane from ethylene is of importance in the petrochemical industry, but similar physicochemical properties of these molecules makes separation a challenging task. Here, the authors demonstrate that a robust octahedral calix[4]resorcinarene-based porous organic cage can separate high-purity ethylene from ethane/ethylene mixtures.
- Kongzhao Su
- , Wenjing Wang
- & Daqiang Yuan
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Article
| Open AccessOrder–disorder transition of a rigid cage cation embedded in a cubic perovskite
In hybrid perovskites, the driving forces of an order–disorder transition that arise from the organic cation and inorganic framework cannot be easily untangled. Here, the authors introduce a cage-in-framework structure in which reorientation of the cage cation does not alter the cubic symmetry of the perovskite lattice.
- Zhifang Shi
- , Zheng Fang
- & Qixi Mi
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Article
| Open AccessIntracellular artificial supramolecules based on de novo designed Y15 peptides
Self-assembling peptides (SAPs) can be used to build biomaterials, but genetically encoded SAPs have rarely been used as building blocks in cells. Here, the authors design a SAP that can be genetically fused to target proteins to induce their intracellular clustering and modulate their signaling functions.
- Takayuki Miki
- , Taichi Nakai
- & Hisakazu Mihara
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Article
| Open AccessMultimodal host–guest complexation for efficient and stable perovskite photovoltaics
It remains a challenge to achieve a balance between performance and stability, as well as addressing the environmental impact of perovskite solar cells. Here, the authors propose a multimodal host-guest complexation strategy enabling these shortcomings to be addressed simultaneously.
- Hong Zhang
- , Felix Thomas Eickemeyer
- & Michael Grätzel
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Article
| Open AccessLiving supramolecular polymerization of fluorinated cyclohexanes
Living supramolecular polymerization can produce precise covalent polymers, but the scope of monomers is still narrow. Here the authors show a molecular platform for living supramolecular polymerization that is based on the unique structure of all-cis 1,2,3,4,5,6- 22 hexafluorocyclohexane, the most polar aliphatic compound reported to date.
- Oleksandr Shyshov
- , Shyamkumar Vadakket Haridas
- & Max von Delius
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Article
| Open AccessVersatile non-luminescent color palette based on guest exchange dynamics in paramagnetic cavitands
Host-guest supramolecular chemistry can be used as a tool to develop multicolor displays. Here, the authors present a system based on lanthanide-cradled cyclodextrins that allows to construct MRI-readable and erasable artificial non-luminescent color palettes.
- Elad Goren
- , Liat Avram
- & Amnon Bar-Shir
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Article
| Open AccessAcceleration of lipid reproduction by emergence of microscopic motion
Artificial molecular systems can show complex kinetics of reproduction, however their integration into larger ensembles remains a challenge towards evolving higher order functionality. Here authors use show that self-reproducing lipids can initiate and accelerate octanol droplet movement and that reciprocally chemotactic movement of these droplets increases the rate of lipid reproduction substantially.
- Dhanya Babu
- , Robert J. H. Scanes
- & Nathalie Katsonis
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Article
| Open AccessHierarchical communication of chirality for aromatic oligoamide sequences
Communication of chirality at a molecular level is the fundamental for transmitting chirality information but one-step communication modes in many artificial systems limits further processing the chirality information. Here, the authors report chirality communication of aromatic oligoamide sequences within interpenetrated helicate architecture in a hierarchical manner.
- Jiajia Zhang
- , Dan Luo
- & Quan Gan
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Article
| Open AccessOriented arrangement of simple monomers enabled by confinement: towards living supramolecular polymerization
Using simple monomers in living supramolecular polymerization is difficult due to energy principles. Here the authors use confinement from a layered double hydroxide nanomaterial to successfully polymerise several simple monomers with length control and narrow dispersity.
- Yingtong Zong
- , Si-Min Xu
- & Chao Lu
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Article
| Open AccessOvertemperature-protection intelligent molecular chiroptical photoswitches
Realizing overtemperature protection with a molecular device is challenging. Here, the authors demonstrate an overtemperature protection function by integrating thermo- and photoresponsive functions into a pillar[6]arene based pseudocatanene.
- Jiabin Yao
- , Wanhua Wu
- & Cheng Yang
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Article
| Open AccessSemi-conducting 2D rectangles with tunable length via uniaxial living crystallization-driven self-assembly of homopolymer
Semi-conducting two-dimensional polymer nanoobjects are promising materials but examples of self-assembled 2D nanosheets with controlled dimensions has not been shown before. Here, the authors precisely tune the length of 2D sheets of conjugated polymers by using blending, heating, and seeded-growth strategies.
- Sanghee Yang
- , Sung-Yun Kang
- & Tae-Lim Choi
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Article
| Open AccessUltraviolet irradiation-responsive dynamic ultralong organic phosphorescence in polymeric systems
Efficient stimulus-responsive phosphorescence organic materials are attractive, but are extremely rare because of unclear design principles and intrinsically spin-forbidden intersystem crossing. Here, the authors present a facile strategy to achieve ultraviolet irradiation-responsive ultralong room-temperature phosphorescence in several simple amorphous polymer materials.
- Yongfeng Zhang
- , Liang Gao
- & Yanli Zhao
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Article
| Open AccessOrganic superstructure microwires with hierarchical spatial organisation
Rationally designing and precisely constructing the dimensions, configurations and compositions of organic micro- and nanomaterials are key issues in material chemistry, but remain challenging. Here, the authors realize the fine synthesis of organic superstructure microwires via a hierarchical epitaxial-growth approach.
- Ming-Peng Zhuo
- , Guang-Peng He
- & Liang-Sheng Liao
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Article
| Open AccessGenerating biomembrane-like local curvature in polymersomes via dynamic polymer insertion
Investigating biomembrane curvature formation is important for studying intracellular processes, but the instability of liposome models mimicking these membranes restricts exploration of membrane processes. Here, the authors demonstrate control over the curvature formation in polymersome membranes by insertion of PNIPAm as stimuli responsive polymer.
- Jiawei Sun
- , Sjoerd J. Rijpkema
- & Daniela A. Wilson
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Article
| Open AccessPhotoactivated nanomotors via aggregation induced emission for enhanced phototherapy
Induced motion has emerged as a method to increase the efficacy of delivery and therapeutic outcomes using nanomaterials. Here, the authors report on a Janus gold shell polymersome with aggregation-induced emission molecules for phototactic and photodynamic therapy applications.
- Shoupeng Cao
- , Jingxin Shao
- & Jan C. M. van Hest
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Matters Arising
| Open AccessOxalate production via oxidation of ascorbate rather than reduction of carbon dioxide
- Fatemeh Khamespanah
- , Maximilian Marx
- & Matthias Beller
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Article
| Open AccessStereoselectivity in spontaneous assembly of rolled incommensurate carbon bilayers
Incommensurate pairing is a type of stereoisomerism, observed in carbon bilayers, that arises from the twisted orientations of the graphitic layers. Here, the authors create a finite molecular version of an incommensurate carbon bilayer in the form of two concentrically assembled cylindrical molecules.
- Taisuke Matsuno
- , Yutaro Ohtomo
- & Hiroyuki Isobe
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Article
| Open AccessNear quantitative synthesis of urea macrocycles enabled by bulky N-substituent
Macrocycles are molecular structures extensively used in the design of catalysts, therapeutics and supramolecular assemblies but synthesis procedures that can produce macrocycles in high yield under high reaction concentrations are rare. Here the authors report the use of dynamic hindered urea bond for the construction of urea macrocycles with high efficiency.
- Yingfeng Yang
- , Hanze Ying
- & Jianjun Cheng
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Article
| Open AccessPhotoresponsive supramolecular coordination polyelectrolyte as smart anticounterfeiting inks
Photoluminescence printing is a widely applied anticounterfeiting technique but there are still challenges in developing new generation anticounterfeiting materials providing a high security level. Here, the authors demonstrate coordination dependent photochromic luminescence in a supramolecular coordination polyelectrolyte for multiple information authentication.
- Zhiqiang Li
- , Xiao Liu
- & Yanli Zhao
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Article
| Open AccessMolecular cannibalism: Sacrificial materials as precursors for hollow and multidomain single crystals
The coexistence of single-crystallinity with a multidomain morphology is a paradoxical crystallographic phenomenon. Here, the authors introduce a crystallographic morphology never reported before. The single-crystals with a curved and hollow morphology offer opportunities to generate a class of synthetic multidomain crystals.
- Maria Chiara di Gregorio
- , Merna Elsousou
- & Milko E. van der Boom
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Article
| Open AccessDigital navigation of energy–structure–function maps for hydrogen-bonded porous molecular crystals
Energy–structure–function (ESF) maps can facilitate functional materials discovery. Here the authors provide a protocol for the digital navigation of ESF maps, as demonstrated for hydrogen-bonded organic frameworks constructed from triptycene- and spiro-biphenyl-based molecular building block.
- Chengxi Zhao
- , Linjiang Chen
- & Andrew I. Cooper
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Article
| Open AccessFerroelectric columnar assemblies from the bowl-to-bowl inversion of aromatic cores
Organic ferroelectrics are of potential use in state-of-the-art ferroelectric devices but mechanistic insight in generating ferroelectricity remains limited. Here, the authors demonstrate that a bowl-to-bowl inversion of a bowl shaped organic molecule generates ferroelectric dipole relaxation, extending the concept of ferroelectricity in small organic molecules.
- Shunsuke Furukawa
- , Jianyun Wu
- & Tomoyuki Akutagawa
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Article
| Open AccessPhysical networks from entropy-driven non-covalent interactions
Physical networks typically employ enthalpy-dominated crosslinking interactions that become more dynamic at elevated temperatures. Here, the authors report an entropy-driven physical network based on polymer-nanoparticle interactions that exhibits mechanical properties that are invariant with temperature.
- Anthony C. Yu
- , Huada Lian
- & Eric A. Appel
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Article
| Open AccessEnantioselective preparation of mechanically planar chiral rotaxanes by kinetic resolution strategy
Since the discovery of mechanically planar chiral rotaxanes and topologically chiral catenanes, their asymmetric synthesis has been a long-standing challenge. Here, the authors report enantioselective preparation of mechanically planar chiral rotaxanes with up to 99.9% ee in 29% yield.
- Ayumi Imayoshi
- , Bhatraju Vasantha Lakshmi
- & Takeo Kawabata
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Article
| Open AccessA DNA origami-based aptamer nanoarray for potent and reversible anticoagulation in hemodialysis
Safe haemodialysis is essential for patients with acute kidney injury and renal failure. Here the authors present a DNA origami-based approach with high affinity and specificity to thrombin, inhibiting coagulation.
- Shuai Zhao
- , Run Tian
- & Baoquan Ding