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| Open AccessAnionic ring-opening polymerization of functional epoxide monomers in the solid state
Despite recent advancements in mechanochemical polymerization, understanding the unique mechanochemical reactivity during the ball milling polymerization process still requires extensive investigations. Here the authors use solid-state anionic ring-opening polymerization to synthesize polyethers from various functional epoxide monomers.
- Jihye Park
- , Ahyun Kim
- & Byeong-Su Kim
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Article
| Open AccessSmart dynamic hybrid membranes with self-cleaning capability
The performance of membrane desalination of seawater is hampered by fouling. Here the authors develop smart gating hybrid membranes by surface coating with polymer-embedded thermosalient crystals. These membranes enhance pure water flux by over 40% in saltwater desalination by osmotic distillation.
- Elvira Pantuso
- , Ejaz Ahmed
- & Gianluca Di Profio
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Article
| Open AccessA nanoscale MOF-based heterogeneous catalytic system for the polymerization of N-carboxyanhydrides enables direct routes toward both polypeptides and related hybrid materials
Metal-based heterogeneous catalysts are widely employed in ring-opening polymerization (ROP) but up to now the exploration of metal-organic frameworks (MOF) as catalysts in ROP remains underdeveloped. Here, the authors report a MOF heterogeneous catalytic system for fast, controllable, air- and moisture-insensitive ring-opening polymerization of α-amino acid N-carboxyanhydrides, and its seamless integration with hybrid material preparation.
- Ying Liu
- , Zhongwu Ren
- & Yugang Bai
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Article
| Open AccessRecyclable photoresins for light-mediated additive manufacturing towards Loop 3D printing
Among additive manufacturing methods vat photopolymerization (VP) is desired owing to improved efficiency, excellent surface finish, and printing resolution at the micron-scale but the major portion of resins available for VP are based on systems with limited or negligible recyclability. Here, the authors describe an approach that enables the printing of a resin that is amenable to re-printing with retained properties and appearance.
- Xabier Lopez de Pariza
- , Oihane Varela
- & Haritz Sardon
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Article
| Open AccessOrganic laser power converter for efficient wireless micro power transfer
Due to the adjustable bandgap, flexibility, absence of heavy metals and high power per weight, organic laser converters have unique advantages in wireless power transfer. Here, authors integrate organic laser power converters exhibiting efficiency over 36% at 660 nm with photon flux of 9.5 mW/cm2.
- Yafei Wang
- , Zhong Zheng
- & Jianhui Hou
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Article
| Open AccessA recyclable polyester library from reversible alternating copolymerization of aldehyde and cyclic anhydride
Alternating copolymerization of cyclic anhydrides and epoxides is an interesting platform for the synthesis of polyesters from renewable resources, but the near irreversibility of the copolymerization makes it challenging to develop chemically recyclable polyesters with easy-to-tune structure. Here, the authors develop a recyclable polyester library from alternating copolymerization of aldehyde and cyclic anhydride.
- Xun Zhang
- , Wenqi Guo
- & Xinghong Zhang
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Article
| Open AccessProtein fibers with self-recoverable mechanical properties via dynamic imine chemistry
Manipulating the internal interactions within biological fibers to tune macroscopic properties is important but challenging, and can limit applications. Here, the authors report the use of dynamic imine chemistry for engineering molecular interactions and forming strong and tough protein fibers.
- Jing Sun
- , Haonan He
- & Kai Liu
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Article
| Open AccessNanocompartment-confined polymerization in living systems
Polymerizations in living systems can effectively regulate cell functions and behaviors, but their uses have been hindered by the existence of complicated intracorporal interferences, the needs of high concentration of monomers and extra stimulates. Here, the authors address these issues by developing a nanocompartment-confined strategy to achieve broad-spectrum polymerizations in living systems.
- Yun Chen
- , Mengxuan Zuo
- & Yanli Zhao
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Article
| Open AccessStable trapping of multiple proteins at physiological conditions using nanoscale chambers with macromolecular gates
The possibility to trap biomolecules is important for analysing them by optical methods. Here we show how nanoscale chambers with macromolecular gates can be used to trap hundreds of proteins in a volume of one attoliter at physiological conditions without exposing them to any direct forces.
- Justas Svirelis
- , Zeynep Adali
- & Andreas Dahlin
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Article
| Open AccessToughening self-healing elastomer crosslinked by metal–ligand coordination through mixed counter anion dynamics
The trade-off relationship between mechanical robustness and viscoelasticity limits the strategies to produce mechanically tough self-healing polymers. Here the authors, introduce a strengthening strategy for self-healing polymers cross-linked by metal-ligand coordination using mixed counter anion dynamics.
- Hyunchang Park
- , Taewon Kang
- & Jiheong Kang
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Perspective
| Open AccessApplied machine learning as a driver for polymeric biomaterials design
The design of polymers for regenerative medicine could be accelerated with the help of machine learning. Here the authors note that machine learning has been applied successfully in other areas of polymer chemistry, while highlighting that data limitations must be overcome to enable widespread adoption within polymeric biomaterials.
- Samantha M. McDonald
- , Emily K. Augustine
- & Matthew L. Becker
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Article
| Open AccessHeterogenous electromediated depolymerization of highly crystalline polyoxymethylene
Post-consumer plastic waste in the environment has driven the scientific community to develop deconstruction methods that yield valued substances from these synthetic macromolecules but depolymerization of highly crystalline engineering thermoplastics remains challenging. Here, the authors demonstrate that electrocatalysis can be used to depolymerize polyoxymethylene into repolymerizable monomer under ambient conditions.
- Yuting Zhou
- , Joaquín Rodríguez-López
- & Jeffrey S. Moore
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Article
| Open AccessUnderstanding catalytic synergy in dinuclear polymerization catalysts for sustainable polymers
Understanding the intermetallic synergy and the structure-performances relationships of catalysts remains challenging. Here, the authors demonstrate a relationship between both the rates, selectivity and the s-block metal acidity in a series of heterodinuclear catalysts based on Co(III) in combination with alkali and alkaline earth metals for three different polymerization reactios.
- Francesca Fiorentini
- , Wilfred T. Diment
- & Charlotte K. Williams
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Article
| Open AccessPrecise cooperative sulfur placement leads to semi-crystallinity and selective depolymerisability in CS2/oxetane copolymers
CS2 promises easy access to degradable sulfur-rich polymers, but ring-opening copolymerisation using CS2 is challenging due to low linkage selectivity and small-molecule by-products. Here, the authors report a cooperative Cr(III)/K catalyst which selectively delivers poly(dithiocarbonates) from CS2 and oxetanes.
- Christoph Fornacon-Wood
- , Bhargav R. Manjunatha
- & Alex J. Plajer
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Article
| Open AccessMesitylated trityl radicals, a platform for doublet emission: symmetry breaking, charge-transfer states and conjugated polymers
Neutral π-radicals are potential emitters for optoelectronic devices due to the absence of energetically low-lying non-emissive states. Here, the authors report mesityl-substituted tris(2,4,6-trichlorophenyl)methyl radicals and achieve maximum device efficiency of 28% at a wavelength of 689 nm.
- Petri Murto
- , Rituparno Chowdhury
- & Hugo Bronstein
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Article
| Open AccessChalcogen-bridged coordination polymer for the photocatalytic activation of aryl halides
Chalcogen-bridged naphthalene diimide coordination polymers are designed and synthesised as potent excited state reductants for the activation of inert bonds in a series of aryl halides.
- Le Zeng
- , Tiexin Zhang
- & Chunying Duan
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Article
| Open AccessLean-water hydrogel electrolyte for zinc ion batteries
Excess water in hydrogel-based zinc ion batteries causes side reactions, but reduced water content results in low conductivities. Here, authors develop a lean-water hydrogel based on molecular lubrication mechanism for fast ion transportation, extended stability, and reversible Zinc plating/stripping.
- Yanbo Wang
- , Qing Li
- & Chunyi Zhi
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Article
| Open AccessHierarchical conductive metal-organic framework films enabling efficient interfacial mass transfer
Heterogeneous reactions associated with porous films are vital in nature and industry. A hierarchical-structure-accelerated interfacial dynamic strategy is reported to improve interfacial gas transfer on conductive metal-organic framework films.
- Chuanhui Huang
- , Xinglong Shang
- & Renhao Dong
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Article
| Open AccessThermally trainable dual network hydrogels
Trainable responsive materials have received research interests for future adaptive and intelligent material systems but to date trainable responsive materials only allow one direction of functionality change. Here, the authors demonstrate thermally trainable hydrogel systems consisting of two thermoresponsive polymers, where the volumetric response of the system upon phase transitions enhances or decreases through a training process above a certain threshold temperature.
- Shanming Hu
- , Yuhuang Fang
- & Hang Zhang
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Article
| Open AccessArtificial intelligence driven design of catalysts and materials for ring opening polymerization using a domain-specific language
Developing accessible polymeric materials is a challenging task for generative AI models. Here, the authors show that a domain-specific language enables the use of historical data to tune generative models to produce experimentally achievable material designs.
- Nathaniel H. Park
- , Matteo Manica
- & Pedro L. Arrechea
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Article
| Open AccessUpconversion particle-assisted NIR polymerization enables microdomain gradient photopolymerization at inter-particulate length scale
High crosslinking and low shrinkage stress are difficult to reconcile in the preparation of performance-enhancing photopolymer materials. Here the authors report the mechanism of upconversion particles-assisted NIR polymerization in reducing shrinkage stress and enhancing mechanical properties of cured materials
- Peng Hu
- , Hang Xu
- & Ren Liu
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Article
| Open AccessBayesian-optimization-assisted discovery of stereoselective aluminum complexes for ring-opening polymerization of racemic lactide
Stereoselective catalysts impact polymer’s properties, but discovering such catalysts is expensive and based on trial-and-error. Here, the authors develop a machine-learning tool to guide catalyst discovery and reveal mechanistic features affecting stereoselectivity.
- Xiaoqian Wang
- , Yang Huang
- & Rong Tong
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Article
| Open AccessA single-domain green fluorescent protein catenane
Natural proteins exhibit rich structural diversity based on the folds of an invariably linear chain. Here the authors design a single-domain GFP catenane as the counterpart of conventional linear GFP with enhanced thermal resilience and to provide a robust scaffold for making fusion protein catenanes.
- Zhiyu Qu
- , Jing Fang
- & Wen-Bin Zhang
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Article
| Open AccessUpper critical solution temperature polymer assemblies via variable temperature liquid phase transmission electron microscopy and liquid resonant soft X-ray scattering
The inclusion of an upper critical solution temperature (UCST) block in multiblock copolymer amphiphiles can enable temperature triggered nanoscale morphological transitions, but there are limited studies probing the actual UCST transition. Here, the authors couple variable temperature liquid-cell transmission electron microscopy and variable temperature liquid resonant soft X-ray scattering to study UCST polymeric nanostructures.
- Joanna Korpanty
- , Cheng Wang
- & Nathan C. Gianneschi
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Article
| Open AccessSolution-processable polymers of intrinsic microporosity for gas-phase carbon dioxide photoreduction
This works presents a series of solution processable, conjugated polymers of intrinsic microporosity, which are used as photocatalysts for carbon dioxide reduction to carbon monoxide in the presence of hydrogen.
- Floriana Moruzzi
- , Weimin Zhang
- & Iain McCulloch
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Article
| 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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Article
| 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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Article
| Open AccessVisualizing the multi-level assembly structures of conjugated molecular systems with chain-length dependent behavior
A deep understanding of multi-level assembly structures of conjugated polymers is crucial for developing high performance conjugated polymers and optoelectronic devices, however, it remains a challenge. Here, the authors report the morphological evolution of multi-level assembly of a model system of isoindigo-based conjugated polymer.
- Yang-Yang Zhou
- , Yu-Chun Xu
- & Jian Pei
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Article
| Open AccessSelf-healable polymer complex with a giant ionic thermoelectric effect
Thermoelectric devices have received significant attention for energy generation owing to their unique advantages over traditional heat engines. Here, the authors developed a well performing stretchable and self-healable iono thermoelectric material by optimizing the thermophoresis of protons in a polymer complex PEDOT:PAAMPSA:PA polymer.
- Dong-Hu Kim
- , Zico Alaia Akbar
- & Sung-Yeon Jang
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Article
| Open AccessInsights into substitution strategy towards thermodynamic and property regulation of chemically recyclable polymers
The global plastic pollution crisis can be mitigated by developing chemically recyclable polymers following the monomer design principle. Here, the authors evaluate substitution effects and structure−property relationships in the ɛ-caprolactone system to guide the design of monomers for the preparation of chemically recyclable polymers.
- Yi-Min Tu
- , Fu-Long Gong
- & Jian-Bo Zhu
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Article
| Open AccessFacile conversion of water to functional molecules and cross-linked polymeric films with efficient clusteroluminescence
Synthetic approaches that employ water to produce functional molecules and polymers with clusteroluminescence properties are highly desirable but not yet reported. Here, the authors apply a water-involved reaction and interfacial polymerization strategy to synthesize nonaromatic molecules and cross-linked polymer films that emit visible light.
- Bo Song
- , Jianyu Zhang
- & Ben Zhong Tang
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Article
| 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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Article
| Open AccessConjugated cross-linked phosphine as broadband light or sunlight-driven photocatalyst for large-scale atom transfer radical polymerization
The application for large-scale production of polymers using photocatalyzed reversible deactivation radical polymerization remains challenging. Here, the authors report the development of a phosphine-based conjugated hypercrosslinked polymer as photocatalyst for an efficient photoinduced and oxygen tolerant copper-catalyzed atom transfer radical polymerization.
- Wei-Wei Fang
- , Gui-Yu Yang
- & Bi-En Tan
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Article
| Open AccessLong-wave infrared transparent sulfur polymers enabled by symmetric thiol cross-linker
Infrared (IR) transmissive polymeric materials for optical elements require a balance between their optical and thermal properties but achieving simultaneously a high refractive index and IR transparency in the long wavelength infrared region in polymer materials is challenging. Here the authors demonstrate inverse vulcanization of 1,3,5-benzenetrithiol (BTT) to achieve a long wavelength IR transparent material without sacrificing on the thermal properties.
- Miyeon Lee
- , Yuna Oh
- & Nam-Ho You
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Article
| Open AccessUpscaled production of an ultramicroporous anion-exchange membrane enables long-term operation in electrochemical energy devices
The design of highly selective yet robust anion exchange membranes remains a challenge. Here, the authors prepare a stable polymer membrane composed of terphenyl isomers, demonstrate roll-to-roll manufacturing, and assess its properties in redox flow batteries, water electrolyzers and fuel cells.
- Wanjie Song
- , Kang Peng
- & Tongwen Xu
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Article
| Open AccessImproved photovoltaic performance and robustness of all-polymer solar cells enabled by a polyfullerene guest acceptor
Fullerene acceptors typically suffer from undesirable segregation and dimerization. Here, the authors report a poly(fullerene-alt-xylene) acceptor as guest component to facilitate charge transfer and suppress charge recombination, achieving efficiency of 18% for ternary all-polymer solar cells.
- Han Yu
- , Yan Wang
- & Shangshang Chen
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Article
| Open AccessA non-Newtonian fluid quasi-solid electrolyte designed for long life and high safety Li-O2 batteries
Lithium dendrite growth and liquid electrolyte volatilization limit the further development of lithium-oxygen batteries. Here, authors report a non-Newtonian fluid quasi-solid electrolyte to address those issues, which improve the life duration of the lithium-oxygen batteries.
- Guangli Zheng
- , Tong Yan
- & Huiyu Song
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Article
| Open AccessAdaptable covalently cross-linked fibers
Covalent cross-linking can be used to improve the mechanical properties of fibers, but can be complicated to prepare and process. Here, the authors report fibers prepared with dynamic covalent bonds, which can reversibly dissociate to enable processing, while maintaining improved mechanical properties in the final material.
- Hui Tan
- , Luzhi Zhang
- & Zhengwei You
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Article
| Open AccessScrew sense excess and reversals of helical polymers in solution
Reversals are structural motifs found in helical polymers that are difficult to determine experimentally. Here, the authors turn to photochemical electrocyclization as a tool to establish their presence and estimate excess screw sense in solution.
- Francisco Rey-Tarrío
- , Rafael Rodríguez
- & Félix Freire
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Article
| Open AccessOne-pot synthesis of hyperbranched polymers via visible light regulated switchable catalysis
Switchable catalysis promises exceptional efficiency in synthesizing polymers with increasing structural complexity but current achievements in such attempts are limited to constructing linear block copolymers. Here the authors report a visible light regulated switchable catalytic system capable of synthesizing hyperbranched polymers in a one-pot/two-stage procedure with commercial glycidyl acrylate as a heterofunctional monomer.
- Shuaishuai Zhu
- , Maoji Zhao
- & Xiaolin Xie
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Article
| Open AccessA co-anchoring strategy for the synthesis of polar bimodal polyethylene
Polar functional groups can improve the polymer properties of polyolefins but also poison the metal catalyst used during the polymerization reaction. Here, the authors show that functionalized bimodal polyolefins in which the high-molecular-weight fraction bears few functional groups and possesses high mechanical and melt properties can be used to implement both polarity and processability
- Chen Zou
- , Quan Wang
- & Changle Chen
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Article
| Open Access3D printing of dynamic covalent polymer network with on-demand geometric and mechanical reprogrammability
3D printing allows preparation of versatile polymer materials for device applications, but properties are often fixed following printing. Here, the authors report a photo-printable dynamic covalent network that allows modification of properties following printing.
- Zizheng Fang
- , Yunpeng Shi
- & Tao Xie
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Article
| Open AccessSingle-vat single-cure grayscale digital light processing 3D printing of materials with large property difference and high stretchability
Despite recent progress in additive
manufacturing of organic materials, multimaterial additive manufacturing remains
challenging. Here, the authors design a resin design that can be used for singlevat
single-cure grayscale digital light processing 3D printing where light intensity
can locally control the conversion of monomers to form from a highly stretchable
soft organogel to a stiff thermoset within in a single layer of printing
- Liang Yue
- , S. Macrae Montgomery
- & H. Jerry Qi
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Article
| Open AccessIn-situ forming dynamic covalently crosslinked nanofibers with one-pot closed-loop recyclability
Polymeric nanofibers are attractive nanomaterials owing to their high surfacearea- to-volume ratio and superior flexibility but designing durable and recyclable polymer nanofibers is challenging. Here, the authors integrate the concept of covalent adaptable networks to produce dynamic covalently crosslinked nanofibers via electrospinning.
- Sheng Wang
- , Nannan Wang
- & Zibiao Li
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Article
| Open AccessMetal-coordinated polybenzimidazole membranes with preferential K+ transport
Membranes with fast and selective ion transport are essential for electrochemical processes. Here the authors provide mechanistic insights into the structures of metal-ion coordinated polybenzimidazole membranes and the preferential K+ transport, and their application in an alkaline zinc-iron flow battery.
- Jine Wu
- , Chenyi Liao
- & Xianfeng Li
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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
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Article
| Open AccessNew insights in polydopamine formation via surface adsorption
Polydopamine is a biomimetic self-adherent polymer, which can be easily deposited on a wide variety of materials but the polymerization mechanism and the key intermediate species formed during the deposition process are still controversial. Here, the authors report a systematic investigation of polydopamine formation on halloysite nanotubes.
- Hamoon Hemmatpour
- , Oreste De Luca
- & Petra Rudolf
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Article
| Open AccessSelf-spinning filaments for autonomously linked microfibers
Bio-inspired assembly of mesoscale materials presents a unique challenge due to complex machinery or labor-intensive processing involved in engineering. Barber et al. report chiral filaments self-assembled into free-standing, anisotropic bundles through pre-programmed, light-mediated structural deformations.
- Dylan M. Barber
- , Todd Emrick
- & Alfred J. Crosby
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Article
| Open AccessAchiral organoiodine-functionalized helical polyisocyanides for multiple asymmetric dearomative oxidations
Immobilizing organocatalysts onto helical polymers can facilitate catalyst recycling and boost enantioselectivity. Here, the authors prepare achiral organoiodine-functionalized single left- and right-handed helical polyisocyanides from the same monomers and demonstrate their use in three asymmetric oxidations.
- Zong-Quan Wu
- , Xue Song
- & Na Liu