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| Open AccessDual enzyme-powered chemotactic cross β amyloid based functional nanomotors
Nanomotor chassis constructed from biological precursors and powered by biocatalytic transformations can offer important applications in the future. Here, the authors prepare short-peptide-based cross β amyloid nanomotors which can host dedicated enzymes with orthogonal substrates for motility and navigation.
- Chandranath Ghosh
- , Souvik Ghosh
- & Dibyendu Das
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| Open AccessHistidine modulates amyloid-like assembly of peptide nanomaterials and confers enzyme-like activity
In this work, the authors report that Histidine residues play a critical role in modulating amyloid-like assembly and building active sites for Fmoc–F–F and Aβ aggregates. Aβ1-42 filaments were found to perform peroxidase-like activity to enhance oxidative stress, which might also be ascribed to the interaction mode of His and F-F.
- Ye Yuan
- , Lei Chen
- & Lizeng Gao
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| Open AccessNongenetic surface engineering of mesenchymal stromal cells with polyvalent antibodies to enhance targeting efficiency
Limited delivery of therapeutic cells to diseased tissue hampers the effective application of mesenchymal stromal cells (MSCs). Here, authors modify the cell surface with polyvalent antibodies using DNA-templated assembly, and show that polyvalent interactions can be used to improve the targeting efficiency of MSCs.
- Tenghui Ye
- , Xi Liu
- & Peng Shi
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Article
| Open AccessChiral recognition of neutral guests by chiral naphthotubes with a bis-thiourea endo-functionalized cavity
Chiral receptors with an endo-functionalized cavity for chiral recognition are of interest in the field of molecular recognition. Here, the authors develop chiral naphthotubes containing a bis-thiourea endo-functionalized cavity to effectively recognize neutral chiral molecules with high enantioselectivity.
- Song-Meng Wang
- , Yan-Fang Wang
- & Liu-Pan Yang
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Article
| Open AccessDual hypoxia-responsive supramolecular complex for cancer target therapy
The natural product BE-43547A2 (BE) could potentially serve as a template of hypoxia target strategy for treating pancreatic cancer, but the unsatisfactory pharmacokinetics profile and severe toxicity impeded the application of BE or its derivatives. Here the authors report a supramolecular dual hypoxia-responsive BE-based complex for achieving efficient drug delivery within tumors.
- Jian-Shuang Guo
- , Juan-Juan Li
- & Yue Chen
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| Open AccessCoupled reaction equilibria enable the light-driven formation of metal-functionalized molecular vanadium oxides
The introduction of metal sites into polyoxometalates is key for tuning their structure and reactivity but the complex mechanisms which govern metal functionalization of polyoxometalates are still poorly understood. Here, the authors report a coupled set of light-dependent and light-independent reaction equilibria controlling the mono- and di- metal-functionalization of a prototype molecular vanadium oxide cluster
- Stefan Repp
- , Moritz Remmers
- & Carsten Streb
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Article
| Open AccessNonporous amorphous superadsorbents for highly effective and selective adsorption of iodine in water
Porous or crystalline materials are generally employed as adsorbents for environmental remediation. Here the authors employ nonporous and amorphous covalent organic superphane cages for aqueous iodine adsorption achieving good selectivity, high adsorption capability and fast kinetics.
- Wei Zhou
- , Aimin Li
- & Qing He
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| Open AccessIntegration of AIEgens into covalent organic frameworks for pyroptosis and ferroptosis primed cancer immunotherapy
Pyroptosis and ferroptosis are typically induced by metal species or chemotherapeutic drugs, and able to boost a robust antitumor immunity, however their therapeutic uses have been hindered by the risks arising from metal species or chemotherapeutic drugs. Here the authors report a pyroptosis and ferroptosis dual-inducer based on non-metallic AIEgen-based covalent organic frameworks.
- Liang Zhang
- , An Song
- & Zhi-Jun Sun
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Article
| Open AccessStimuli-responsive rotaxane-branched dendronized polymers with tunable thermal and rheological properties
Enriching the toolbox of polymers, the design and construction of novel polymers with desired properties and functions remains an attractive topic in polymer chemistry. Here the authors demonstrate rotaxane-branched dendronized polymers with rotaxane-branched dendrons attached onto the polymer chains as polymers with attractive dynamic properties.
- Yu Zhu
- , Hanqiu Jiang
- & Hai-Bo Yang
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Article
| Open AccessA route to metalloligands consolidated silver nanoclusters by grafting thiacalix[4]arene onto polyoxovanadates
Metalloligands provide a potent strategy for manipulating the surface metal arrangements of metal nanoclusters (NCs), but their synthesis and subsequent installation onto metal NCs remains a significant challenge. Here, the authors demonstrate the synthesis of two atomically precise silver NCs by controlling reaction temperature and demonstrate thermal induced structure transformation between the clusters during a temperature-dependent assembly process.
- Zhi Wang
- , Yan-Jie Zhu
- & Di Sun
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Article
| Open AccessDual donor-acceptor covalent organic frameworks for hydrogen peroxide photosynthesis
In this study, benzotrithiophene-based covalent organic frameworks with spatially separated oxidative and reductive reaction centers are rationally designed for photocatalytic production of H2O2 from water and oxygen without sacrificial agents.
- Chencheng Qin
- , Xiaodong Wu
- & Hou Wang
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| Open AccessA cage-on-MOF strategy to coordinatively functionalize mesoporous MOFs for manipulating selectivity in adsorption and catalysis
Functionalising porous materials is a route to enhancing properties of hybrid materials. Here authors present a “Cage-on-MOF” strategy to modify the surface of mesoporous MOFs by using molecular cages to achieve selective dyes adsorption behavior and heterogeneous catalysis.
- Yu Liang
- , Xiaoxin Yang
- & Yu Fang
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Article
| Open AccessData-mining unveils structure–property–activity correlation of viral infectivity enhancing self-assembling peptides
Certain peptides can boost viral infectivity. However, the requirements for their activity remain unclear. Here, the authors demonstrate that peptides are efficient viral enhancers if they form hydrophobic β-sheet-rich, positively charged μm-sized aggregates.
- Kübra Kaygisiz
- , Lena Rauch-Wirth
- & Tanja Weil
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| Open AccessAllosteric control of olefin isomerization kinetics via remote metal binding and its mechanochemical analysis
The mechanisms by which changes in local geometries of receptor sites lower activation reaction barriers in electronically uncoupled, remote reaction moieties remain relatively unexplored. Here, the authors demonstrate allosteric acceleration in the thermal isomerization of an alkene triggered by the binding of a metal ion to a remote receptor site.
- Yichen Yu
- , Robert T. O’Neill
- & Stephen L. Craig
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Article
| Open AccessProgrammable supramolecular chirality in non-equilibrium systems affording a multistate chiroptical switch
The dynamic regulation of supramolecular chirality in non-equilibrium systems can provide valuable insights into molecular self-assembly in living systems. Here, the authors demonstrate the use of chemical fuels for regulating self-assembly pathway, which thereby controls the supramolecular chirality of a non-equilibrium assembled system.
- Jingjing Li
- , Yihan Cui
- & Chun-Sen Liu
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| Open AccessCe-mediated molecular tailoring on gigantic polyoxometalate {Mo132} into half-closed {Ce11Mo96} for high proton conduction
Polyoxometalates (POMs) are molecular clusters with diverse structures. Here authors present the synthesis of POMs by Ce-mediated molecular tailoring from gigantic {Mo132} into half-closed {Ce11Mo96}, with proton conductivity nearly two orders of magnitude higher than {Mo132}.
- Xue-Xin Li
- , Cai-Hong Li
- & Zhong-Min Su
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| Open AccessPillararene incorporated metal–organic frameworks for supramolecular recognition and selective separation
Frameworks containing flexible macrocycle units provide opportunities in molecular recognition and separation. Here authors present MOFs with uniformly embedded pillar[5]arene that can recognise paraquat and 1,2,4,5-tetracyanobenzene in solution and selectively remove trace pyridine from toluene.
- Yitao Wu
- , Meiqi Tang
- & Feihe Huang
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| Open AccessEffector-dependent structural transformation of a crystalline framework with allosteric effects on molecular recognition ability
Porous crystals with molecular recognition sites in the inner pores are promising for achieving functional control, where the local binding of effectors triggers a distortion which propagates throughout the structure. Here the authors report that the structure of a porous molecular crystal can be allosterically controlled by local adsorption of effectors within low-symmetry nanochannels with multiple molecular recognition sites.
- Ryunosuke Hayashi
- , Shohei Tashiro
- & Mitsuhiko Shionoya
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| Open AccessSaddles as rotational locks within shape-assisted self-assembled nanosheets
Self-assembly in the formation of two dimensional materials typically relies upon strong, directional interactions instead of covalent bonds but control over less directional forces remains challenging. Here, the authors show the process of shape-assisted self-assembly to be consistent across a range of derivatives that highlights the restriction of rotational motion.
- Joseph F. Woods
- , Lucía Gallego
- & Michel Rickhaus
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| Open AccessA stretchable, mechanically robust polymer exhibiting shape-memory-assisted self-healing and clustering-triggered emission
Polymers formed with non-covalent bonds are increasingly being developed, but often show inferior mechanical properties. Here, the authors report the development of high performances polyurethane-urea elastomer with shape-memory assisted self-healing behaviour
- Xiaoyue Wang
- , Jing Xu
- & Xinrui Zhang
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| Open AccessThe sharp structural switch of covalent cages mediated by subtle variation of directing groups
Controlling the self-assembly on noncovalent components is possible by suppressing entropy loss with templates but this is challenging for covalent components. Here the authors employed directing groups to endow purely covalent molecular building blocks with different conformations which favor the formation of specific self-assembled products.
- Qiong Chen
- , Zhaoyong Li
- & Hao Li
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Article
| Open AccessThe host–guest inclusion driven by host-stabilized charge transfer for construction of sequentially red-shifted mechanochromic system
The understanding of the structure-property relationship of mechanochromic luminescent molecules remains challenging. Here, the authors elucidate the effect of host-guest interactions on the mechanochromic properties of organic molecules.
- Dongdong Sun
- , Yong Wu
- & Simin Liu
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| Open AccessA supramolecular metalloenzyme possessing robust oxidase-mimetic catalytic function
The de novo synthesis of enzyme-like active sites remains a challenge, due to the difficulties in imitating the spatial arrangement of the functional groups. Here, the authors report the construction of a supramolecular mimetic enzyme possessing catechol oxidase-like copper-cluster active sites.
- Shichao Xu
- , Haifeng Wu
- & Zhen-Gang Wang
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| Open AccessPhotoswitchable dynamic conjugate addition-elimination reactions as a tool for light-mediated click and clip chemistry
Photoinduced dynamic covalent bonds have the advantage of light-mediated bond making and breaking. Here, the authors report photoswitchable dynamic conjugate addition-elimination reactions with a broad scope and demonstrate diverse applications.
- Hanwei Lu
- , Hebo Ye
- & Lei You
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Article
| Open AccessAssembly drives regioselective azide-alkyne cycloaddition reaction
Metal-free versions of azide–alkyne cycloadditions could find widespread applications in biomedical contexts. Here, the authors report an assembly-driven, regioselective azide–alkyne cycloaddition.
- Qiaochu Jiang
- , Wenjun Zhan
- & Gaolin Liang
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Article
| Open AccessCucurbit[8]uril-based water-dispersible assemblies with enhanced optoacoustic performance for multispectral optoacoustic imaging
The applications of organic small-molecule contrast agents for multispectral optoacoustic imaging have been restrained by several challenges including relatively low extinction coefficient, poor water solubility and weak optoacoustic performance. Here, the authors address these limitations by constructing water-dispersible supramolecular optoacoustic assemblies based on cucurbit[8]uril.
- Yinglong Wu
- , Lihe Sun
- & Yanli Zhao
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| Open AccessAccelerating the prediction and discovery of peptide hydrogels with human-in-the-loop
Accurate prediction of peptidic hydrogels could prove useful for diverse biomedical applications. Here, the authors develop a “human-in-the-loop” approach that integrates coarse-grained molecular dynamics, machine learning, and experimentation to design natural peptide hydrogels.
- Tengyan Xu
- , Jiaqi Wang
- & Huaimin Wang
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Article
| Open AccessRapid and reversible optical switching of cell membrane area by an amphiphilic azobenzene
The surface area of living cells is tightly regulated. Here, authors show that the surface area and shape of cells can be reversibly manipulated with light using amphiphilic molecular photoswitches that enter and leave the membrane.
- Fabian Höglsperger
- , Bart E. Vos
- & Bart Jan Ravoo
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| Open AccessAn approach to MOFaxanes by threading ultralong polymers through metal–organic framework microcrystals
Mechanically interlocked architectures inspired the fabrication of numerous molecular systems, but the topological design of such architectures has not been fully explored from the nano- to the macroscopic scale. Here, the authors propose a MOFaxane, comprised of long chain molecules penetrating a microcrystal of metal– organic framework.
- Tomoya Iizuka
- , Hiroyuki Sano
- & Takashi Uemura
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| Open AccessMulti-chiral materials comprising metallosupramolecular and covalent helical polymers containing five axial motifs within a helix
The axial helical structure of supramolecular and covalent polymers provides communication mechanisms among monomer repeating units. Here, the authors present multi-helical materials comprising five axial motifs that combine information from both metallosupramolecular and covalent helical polymers
- Francisco Rey- Tarrío
- , Emilio Quiñoá
- & Félix Freire
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| Open AccessMechanosensitive non-equilibrium supramolecular polymerization in closed chemical systems
Chemical fuel-driven supramolecular systems have been developed showing out of-equilibrium functions such as transient gelation and oscillations but these systems suffer from undesired waste accumulation and they function only in open systems. Here, the authors we report non-equilibrium supramolecular polymerizations in a closed system, which is built by viologens and pyranine in the presence of hydrazine hydrate.
- Xianhua Lang
- , Yingjie Huang
- & Hui Zhao
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| Open AccessMagnetic control of self-assembly and disassembly in organic materials
Organic molecules and materials are generally insensitive or weakly sensitive to magnetic fields due to their small diamagnetic force. Here, the authors show a strategy to amplify the magnetic responsiveness of self-assembled peptide nanostructures by synergistically combining the concepts of perfect α-helix and rod-coil supramolecular building blocks
- You-jin Jung
- , Hyoseok Kim
- & Yong-beom Lim
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| Open Access[2,2] Paracyclophanes-based double helicates for constructing artificial light-harvesting systems and white LED device
The construction of efficient artificial lightharvesting (ALH) systems is of vital importance in utilizing solar energy. Here, the authors report the non-covalent syntheses of double helicates by metalcoordination interaction and their applications in ALHSs and white LED device
- Zhe Lian
- , Jing He
- & Hua Jiang
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| Open AccessSwitching imidazole reactivity by dynamic control of tautomer state in an allosteric foldamer
Molecular biology achieves control over complex reaction networks by means of molecular systems that translate a chemical input into an orthogonal chemical output but the application of dynamic foldamers has been limited by the restriction to stereochemical changes that produce spectroscopic signals. Here, the authors present an artificial molecular translation device that converts a chemical input into an unrelated chemical output.
- David P. Tilly
- , Jean-Paul Heeb
- & Jonathan Clayden
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| Open AccessHierarchical porous photosensitizers with efficient photooxidation
Photosensitizers (PS) with nano- or micro-sized pore provide a great promise in the conversion of light energy into chemical fuel but pore deformation and blocking often decreases the catalytic efficiency. Here, the authors prepare an ordered porous PSs by cross-linking hierarchical porous assemblies of hydrogen donating PSs and functionalized acceptors.
- Yajun Fang
- , Yuntian Yang
- & Zhegang Huang
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Article
| Open AccessChemically routed interpore molecular diffusion in metal-organic framework thin films
In heterogeneous porous systems diffusion rate is controlled by pore window sizes and concentration gradient. Here authors show that in a porous metal-organic framework system, the diffusion direction can be orthogonal to the concentration gradient.
- Tanmoy Maity
- , Pratibha Malik
- & Ritesh Haldar
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| Open AccessRepurposing host-guest chemistry to sequester virulence and eradicate biofilms in multidrug resistant Pseudomonas aeruginosa and Acinetobacter baumannii
Rapid antibiotic resistance in bacteria is putting pressure on both existing therapies as well as the development pipeline. Here, the authors present a dual-acting anti-virulence treatment that evades antibiotic resistance mechanisms and remains effective against Top Priority pathogens.
- Christopher Jonkergouw
- , Ngong Kodiah Beyeh
- & Markus B. Linder
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Article
| Open AccessA supramolecular gel-elastomer system for soft iontronic adhesives
Electroadhesion in soft robotics provides controllable interfacial attraction for robotic functionalities but materials selection is limited. Here, Gao et. al. present an iontronic adhesive to design a soft iontronic gripper with self-healability, tunable adhesion at reduced voltages and rapid release.
- Dace Gao
- , Gurunathan Thangavel
- & Pooi See Lee
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Article
| Open AccessAnomalous deep-red luminescence of perylene black analogues with strong π-π interactions
Perylene bisimide dyes are high-performance pigments that have red, maroon or black colors, but with typically only weak fluorescence in the solid state. Here, the authors report a series of π-stacked PBI derivatives that show highly efficient deep-red fluorescence in the solid state.
- Ningning Tang
- , Jiadong Zhou
- & Zengqi Xie
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Article
| Open AccessAmyloid-polysaccharide interfacial coacervates as therapeutic materials
Liquid-liquid phase separation offer a strategy for targeting biomaterial scaffolds, but controlling assembly to form functional materials is challenging. Here, the authors transform native proteins into amyloid fibres for assembly, and use the materials as a gastric ulcer protective agent.
- Mohammad Peydayesh
- , Sabrina Kistler
- & Raffaele Mezzenga
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Article
| Open AccessHigh-entropy alloy nanopatterns by prescribed metallization of DNA origami templates
Morphology, composition, and uniformity of highly entropic nanoalloys are critical to their properties and applications. Here, the authors develop a DNA origami-based metallization reaction concept for the precise synthesis of multimetallic nanopatterns.
- Mo Xie
- , Weina Fang
- & Huajie Liu
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Article
| Open AccessFour distinct network patterns of supramolecular/polymer composite hydrogels controlled by formation kinetics and interfiber interactions
Synthetic hydrogels composed of covalent polymers and supramolecular fibers have been investigated for controlled delivery of biopharmaceuticals, but characterisation of the structures and properties can be challenging. Here, the authors report an imaging study for the composite network, categorizing into four distinct patterns controlled by network formation kinetics and interactions between
- Keisuke Nakamura
- , Ryou Kubota
- & Itaru Hamachi
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Article
| Open AccessPhotothermally induced natural vibration for versatile and high-speed actuation of crystals
Soft robotics is a growing field, and requires versatile actuation methodology. Here, the authors report high-speed bending of anisole crystals due to natural vibration, induced and amplified by photothermal effect.
- Yuki Hagiwara
- , Shodai Hasebe
- & Hideko Koshima
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Article
| Open AccessPolymerizable rotaxane hydrogels for three-dimensional printing fabrication of wearable sensors
While hydrogels find applications in wearable sensors and electronic skins, they are prone to fatigue fractures upon deformation cycling. Xiong et al. report the synthesis of conductive polymerizable rotaxane hydrogels, exhibiting large fatigue resistance, for 3D printable flexible sensors.
- Xueru Xiong
- , Yunhua Chen
- & Yanli Zhao
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Article
| Open AccessHigh-efficiency gold recovery by additive-induced supramolecular polymerization of β-cyclodextrin
Eco-friendly, efficient, and selective gold recovery technologies are urgently desired to satisfy the increasing demand for gold. Here, the authors report one such technology based on the supramolecular polymerization of second-sphere coordinated adducts formed between β-cyclodextrin and tetrabromoaurate anions.
- Huang Wu
- , Yu Wang
- & J. Fraser Stoddart
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Article
| Open AccessBioinspired crowding directs supramolecular polymerisation
Crowding effects have long been established as powerful guiding forces in natural assembly processes. Here the authors report a bioinspired approach translating this phenomenon to artificial supramolecular polymers.
- Nils Bäumer
- , Eduardo Castellanos
- & Gustavo Fernández
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| Open AccessSupramolecular framework membrane for precise sieving of small molecules, nanoparticles and proteins
Synthetic framework materials are appealing candidates for the fabrication of separation membranes but realizing precise control of aperture distribution and separation threshold remains challenging. Here, the authors show a two-dimensional processible supramolecular framework which can be used in the fabrication of separation membranes by integrating directional organic host-guest motifs and inorganic functional polyanionic clusters.
- Guohua Zhang
- , Xinyue Li
- & Lixin Wu
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Article
| Open AccessEnzyme-like polyene cyclizations catalyzed by dynamic, self-assembled, supramolecular fluoro alcohol-amine clusters
Terpene cyclases enable the synthesis of (poly)cyclic carbon frameworks via ring closure of linear polyenes. Here, the authors report in-situ formed fluorinated-alcohol-amine supramolecular clusters that mimic terpene cyclases for shape-controlled polyene cyclizations.
- Andreas M. Arnold
- , Philipp Dullinger
- & Tanja Gulder
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Article
| Open AccessSpatially non-uniform condensates emerge from dynamically arrested phase separation
Biomolecular condensates with internal structure allow cells to further organise their processes. In this work the authors investigate how condensates can obtain an internal structure with droplets of dilute phase inside via kinetic, rather than purely thermodynamic driving forces.
- Nadia A. Erkamp
- , Tomas Sneideris
- & Tuomas P. J. Knowles