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| Open AccessHarmonic amide bond density as a game-changer for deciphering the crosslinking puzzle of polyamide
Relating the degree of network crosslinking as a descriptor to the desalination performance of crosslinked polymer membranes remains challenging. Here, the authors introduce a parameter based on distinct amide bonds per unit mass of polyamide, to unravel the relationship between the crosslinked networks of polyamide membranes and their desalination performance.
- Yu-Ren Xue
- , Chang Liu
- & Zhi-Kang Xu
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Article
| Open AccessUnraveling the rheology of inverse vulcanized polymers
Polymers typically exhibit rheology with multiple relaxation times to fully capture stress relaxation processes to terminal flow. Here, the authors use inverse vulcanization to synthesize polymers that exhibit a single relaxation time due to dynamic covalent disulfide bond reorganization that dominate the rheological properties of these materials.
- Derek J. Bischoff
- , Taeheon Lee
- & Michael E. Mackay
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Article
| Open AccessCatalyst switch strategy enabled a single polymer with five different crystalline phases
Well-defined multicrystalline multiblock polymers are essential model polymers for advancing the physics of crystallization but due to the different chain properties and incompatible synthetic methodologies, multicrystalline multiblock polymers with more than two crystallites are rarely reported. Here the authors combine polyhomologation, ring-opening polymerization and a catalyst switch strategy to synthesize a pentacrystalline pentablock quintopolymer.
- Pengfei Zhang
- , Viko Ladelta
- & Nikos Hadjichristidis
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Article
| Open AccessPolymer architecture dictates multiple relaxation processes in soft networks with two orthogonal dynamic bonds
Materials with tunable modulus, viscosity, and complex viscoelastic spectra are crucial in various applications but it remains challenging to design polymer networks with predicted hierarchical relaxation processes. Here, the authors synthesize networks with both pendant and telechelic architectures using mixed orthogonal dynamic bonds to understand how the network connectivity and bond exchange mechanisms govern the overall relaxation spectrum.
- Sirui Ge
- , Yu-Hsuan Tsao
- & Christopher M. Evans
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Article
| Open AccessApparent symmetry rising induced by crystallization inhibition in ternary co-crystallization-driven self-assembly
The concept of apparent symmetry rising, opposite to symmetry breaking, was proposed to illustrate the unusual phenomenon that the symmetry of the apparent morphology of the multiply twinned particle is higher than that of its crystal structure. Here the authors develop a strategy of co-crystallization-driven self-assembly of amphiphilic block copolymers and the inorganic clusters to achieve apparent symmetry rising of nanoparticles under mild conditions
- Siyu Xie
- , Wenjia Sun
- & Jie 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 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 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 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 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 AccessPhosphorescent extensophores expose elastic nonuniformity in polymer networks
The macroscopic mechanical response in cross-linked polymer networks has been well investigated but an understanding of pre-failure local mechanical responses at the level of individual crosslinks is still lacking. Here, using an extensophore concept, the authors show that the crosslinks in an elastic polymer network extend, fluctuate, and deform with a wide range of molecular individuality
- Kaikai Zheng
- , Yifan Zhang
- & Steve Granick
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Article
| Open AccessForce-triggered rapid microstructure growth on hydrogel surface for on-demand functions
Living organisms are able to grow structures on their surface for specific applications. Here, the authors report on a force-triggered polymerisation mechanism of double-network hydrogels which allows for the growth of structures on polymer surfaces within seconds and demonstrate the creation of different functionalities.
- Qifeng Mu
- , Kunpeng Cui
- & Jian Ping Gong
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Article
| Open AccessThe molecular mechanism of constructive remodeling of a mechanically-loaded polymer
Large mechanical loads usually degrade polymers by accelerating fragmentation of their backbones but rarely, they can cause new backbone bonds to form leading to arrested or reversed degradation when new bonds are formed faster than the original bonds break.Here, the authors report the molecular mechanism and analysis of constructive remodeling driven by the macroradical products of mechanochemical fragmentation of a hydrocarbon backbone.
- Chenxu Wang
- , Sergey Akbulatov
- & Roman Boulatov
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Article
| Open AccessCompetition between crystal growth and intracrystalline chain diffusion determines the lamellar thickness in semicrystalline polymers
The mechanism of crystal thickness selection in semi-crystalline polymers is unclear but intracrystalline chain diffusion has been shown to have a role. Here, the authors report on observations related to poly(oxymethylene) with slow intra-crystalline chain diffusion to fill the knowledge gaps between fast and absent diffusion systems
- Martha Schulz
- , Mareen Schäfer
- & Thomas Thurn-Albrecht
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Article
| Open AccessSolution-processable and functionalizable ultra-high molecular weight polymers via topochemical synthesis
Topochemical polymerization reactions produce ultra-high molecular weight crystalline polymers. Here the authors show a family of para-azaquinodimethane compounds that undergo facile visible light and thermally initiated polymerization in the solid state and the crystal structure has been resolved via cryoelectron microscopy.
- Christopher L. Anderson
- , He Li
- & Yi Liu
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Article
| Open AccessAsymmetrizing an icosahedral virus capsid by hierarchical assembly of subunits with designed asymmetry
Viruses have been re-engineered for many applications but the ability to build asymmetric capsids in vitro has been lacking. Here, the authors report the design of asymmetric subunits with different growth rates leading to capsids with discrete patches and potential for distinct surface chemistries.
- Zhongchao Zhao
- , Joseph Che-Yen Wang
- & Adam Zlotnick
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Article
| Open AccessCrystallization-induced mechanofluorescence for visualization of polymer crystallization
Residual stress in crystalline polymers can lead to material failure, but currently methods which can quantify residual stress in such materials are lacking. Here, by using fluorescent-type mechanochromophores, the authors develop a method to visualize and quantify low degrees of stress that arises from micro-mechanical forces during polymer crystallization.
- Sota Kato
- , Shigeki Furukawa
- & Hideyuki Otsuka
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Article
| Open AccessWater accelerated self-healing of hydrophobic copolymers
Self-healing of polymers became a vivid research area, but self-healing under water and its mechanistic concepts are less investigated. Here, the authors report water accelerated self-healing in a pMMA/nBA copolymer and demonstrate that perturbation of ubiquitous van der Walls forces upon mechanical damage in hydrophobic polymers in the presence of water is energetically unfavorable and accelerates self-healing.
- Dmitriy Davydovich
- & Marek W. Urban
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Article
| Open AccessEnhanced polymer mechanical degradation through mechanochemically unveiled lactonization
The mechanical degradation of polymers is typically limited to a single chain scission event and the loss of stress transfer during the scission process limits the extent of degradation achieved. Here, the authors report a mechanically triggered, delayed scission strategy that allows many eventual scission events to be initiated within a single polymer chain.
- Yangju Lin
- , Tatiana B. Kouznetsova
- & Stephen L. Craig
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Article
| Open AccessPhotodegradable branched polyethylenes from carbon monoxide copolymerization under benign conditions
Small amounts of in-chain keto groups render polyethylene (PE) photodegradable, a desirable feature in view of environmental plastics pollution. Here the authors introduce low ketone content by copolymerization in organic solvent or under aqueous conditions at moderate pressures.
- Tobias O. Morgen
- , Maximilian Baur
- & Stefan Mecking
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Article
| Open AccessRhodanine-based Knoevenagel reaction and ring-opening polymerization for efficiently constructing multicyclic polymers
Cyclic polymers have a number of unique physical properties compared to their linear counterparts but their synthesis is very limited. Here, the authors show a method to form a wide variety of multicyclic polymers by a rhodanine˗based Knoevenagel reaction and ring-opening polymerization.
- Ze Zhang
- , Xuan Nie
- & Ye-Zi You
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Article
| Open AccessFlow-induced crystallisation of polymers from aqueous solution
With the rise in polymer consumption, energy efficient techniques for polymer processing become more important. Using poly(ethylene oxide) aqueous solutions, the authors show that flow can causes a change of polymer solubility resulting in polymer crystallisation at ambient conditions.
- Gary J. Dunderdale
- , Sarah J. Davidson
- & Oleksandr O. Mykhaylyk
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Article
| Open AccessGeneral route to design polymer molecular weight distributions through flow chemistry
The properties of a polymer are known to be intrinsically related to its molecular weight distribution. Here the authors use a design to synthesis protocol for producing a targeted molecular weight distribution with a computer controlled tubular flow reactor.
- Dylan J. Walsh
- , Devin A. Schinski
- & Damien Guironnet
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Article
| Open AccessBreaking translational symmetry via polymer chain overcrowding in molecular bottlebrush crystallization
One of the fundamental laws in crystallization is translational symmetry but breaking translational symmetry can be used as a general route towards the design of nanostructures. Here the authors show that overcrowding in molecular bottlebrush polymers allows for spontaneous formation of spherical hollow crystals with broken translational symmetry.
- Hao Qi
- , Xiting Liu
- & Christopher Y. Li
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Article
| Open AccessOrigin of micro-scale heterogeneity in polymerisation of photo-activated resin composites
Resin-based-composites are widely used in industry and medicine but the influence of the filler particles on the reactive group conversion in photocurable resins is yet to be elucidated. Here the authors observe reduced local conversion and chemical bond strain in silica filler acrylate composite using synchrotron-based wide-field IR imaging.
- Slobodan Sirovica
- , Johanne H. Solheim
- & Owen Addison
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Article
| Open AccessBiobased chiral semi-crystalline or amorphous high-performance polyamides and their scalable stereoselective synthesis
Bio‐based compounds often suffer from high production cost and low performance when used to synthesise macromolecules. Here the authors show the conversion of (+)‐3‐ carene, a by‐product of the cellulose industry, into its ε‐lactams and then to polyamides with high‐performance thermal properties.
- Paul N. Stockmann
- , Daniel Van Opdenbosch
- & Volker Sieber
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Article
| Open AccessDecoupling of mechanical properties and ionic conductivity in supramolecular lithium ion conductors
Typically, ion conducting polymers exhibit a trade-off between mechanical robustness and ionic conducting performance. Here, the authors utilize supramolecular chemistry obtaining extremely tough electrolytes with high ionic conductivity and enabling stretchable lithium-ion batteries.
- David G. Mackanic
- , Xuzhou Yan
- & Zhenan Bao
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Article
| Open AccessPhoto-editable macromolecular information
Light-induced alteration of macromolecular information plays a central role in biology and is known to influence health and aging. Here the authors show that light can trigger sequence variations in abiotic information-containing polymers that possess photo-sensitive monomers
- Niklas Felix König
- , Abdelaziz Al Ouahabi
- & Jean-François Lutz
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Article
| Open AccessVisualization and design of the functional group distribution during statistical copolymerization
Understanding the functional group distribution in a polymer chain has been difficult, but this information can be very useful. Here the authors visualize the monomer distribution in individual polymer chains by combining experimental and theoretical analysis of the construction of functionality-chain length distributions.
- Paul H. M. Van Steenberge
- , Ondrej Sedlacek
- & Dagmar R. D’hooge
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Article
| Open AccessPackaging materials with desired mechanical and barrier properties and full chemical recyclability
Biodegradable plastics usually have poorer mechanical or transport properties compared to conventional plastics. Here the authors show a class of biorenewable and chemically recyclable plastics based on copolymers of γ-butyrolactone and its ring-fused derivative, with competitive properties compared to conventional plastics.
- Ainara Sangroniz
- , Jian-Bo Zhu
- & Haritz Sardon
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Article
| Open AccessDetecting topology freezing transition temperature of vitrimers by AIE luminogens
Detecting and understanding the topology freezing transition temperature of vitrimers has been very limited in the past. Here the authors use a sensitive and universal method by doping or swelling aggregation-induced-emission luminogens into vitrimers as probes to monitor the topology freezing transition temperature
- Yang Yang
- , Shuai Zhang
- & Yan Ji
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Article
| Open AccessTuning the permselectivity of polymeric desalination membranes via control of polymer crystallite size
Increasing the selectivity of desalination membranes is of crucial importance for advancing membrane desalination technologies. Here the authors demonstrate a plasticizing-extracting process for tuning the permselectivity of polymeric membranes and achieving desired desalination performance.
- Xinglin Lu
- , Xunda Feng
- & Menachem Elimelech
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Article
| Open AccessBinary tree-inspired digital dendrimer
Digital polymers with precisely ordered units for next-generation data storage media are continually investigated for higher storage capacity. Here the authors show the synthesis of information-coded 2D digital dendrimers and the generated data matrix barcode can be read by a common hand-held device.
- Zhihao Huang
- , Qiunan Shi
- & Xiulin Zhu
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Article
| Open AccessEffect of molecular architecture on ring polymer dynamics in semidilute linear polymer solutions
Understanding the dynamics of ring polymers is challenging are despite recent progress, understanding of the nonequilibrium behavior of ring polymers has not yet been achieved. Here, the authors directly observe the flow dynamics of DNA-based rings in semidilute linear polymer solutions using single molecule techniques.
- Yuecheng Zhou
- , Kai-Wen Hsiao
- & Charles M. Schroeder
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Article
| Open AccessExploring the colloid-to-polymer transition for ultra-low crosslinked microgels from three to two dimensions
Microgels combine the properties of flexible polymers and colloids, but effects which influence the individual properties are less known. Here the authors show that the properties of a microgel can change from colloidal-like in three dimensions to a flexible polymer under a confined environment.
- A. Scotti
- , S. Bochenek
- & W. Richtering
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Article
| Open AccessElectroactive materials with tunable response based on block copolymer self-assembly
Ferroelectric polymers are key building blocks for flexible electronic devices, but lack functionality and ability to tune their ferroelectric response. Here the authors show a method to introduce functionality in ferroelectric polymers while preserving ferroelectricity and tune the ferroelectric response by incorporating insulating polymer chains.
- Ivan Terzic
- , Niels L. Meereboer
- & Katja Loos
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Article
| Open AccessBlocking-cyclization technique for precise synthesis of cyclic polymers with regulated topology
Cyclic polymers can be usually accessed by ring-expansion and ring-closure approaches. Here, the authors report an alternative blocking-cyclization technique which enables the tunable synthesis of multicyclic polymers via commercial Ru-based Grubbs catalysts and conventional ring-opening metathesis polymerisation.
- Jie Chen
- , Hongfei Li
- & Meiran Xie
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Article
| Open AccessMacromolecular-clustered facial amphiphilic antimicrobials
Bacterial infections and antibiotic resistance are an increasing concern for the world. Here the authors report a class of cationic antimicrobial polymers that cluster local facial amphiphilicity from repeating units to enhance interactions with bacterial membranes without requiring a high unfavorable entropic loss.
- Md Anisur Rahman
- , Marpe Bam
- & Chuanbing Tang
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Article
| Open AccessDissymmetry enhancement in enantioselective synthesis of helical polydiacetylene by application of superchiral light
Superchiral light can be utilized to promote asymmetric photochemical reactions. Here the authors show that superchiral light imparts greater chiral bias to trigger asymmetric photo-polymerization reactions from initially achiral diacetylene monomers and enhanced optical dissymmetry in polydiacetylene films.
- Chenlu He
- , Guang Yang
- & Gang Zou
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Article
| Open AccessEntangled polymer dynamics beyond reptation
Polymer dynamics at entangled conditions has generally been simplified as motions governed by the two ends of each polymer chain. Abadi et al. characterize linear and cyclic dsDNA molecules with high resolution, revealing position-dependent chain motions which cannot be described by the reptation theory.
- Maram Abadi
- , Maged F. Serag
- & Satoshi Habuchi
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Article
| Open AccessTuning anhydrous proton conduction in single-ion polymers by crystalline ion channels
High-conductivity solid-state electrolyte materials with minimal polarization loss are difficult to synthesize. Here the authors show single-ion block copolymers with crystalline protogenic channels having a promising potential to be used as efficient proton conductors.
- Onnuri Kim
- , Kyoungwook Kim
- & Moon Jeong Park
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Review Article
| Open AccessMetallo-polyelectrolytes as a class of ionic macromolecules for functional materials
Polyelectrolytes are a class of macromolecules containing charged groups. Here the authors review properties and functions of metallo-polyelectrolytes to shed light on how to harness fundamental physiochemical properties for applications in biomedical sciences and advanced materials.
- Tianyu Zhu
- , Ye Sha
- & Chuanbing Tang
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Article
| Open AccessPolymerization driven monomer passage through monolayer chemical vapour deposition graphene
Translocation of larger molecules through graphene holds potential for molecular sieving, however it is rarely observed. Here, the authors show the radical polymerization of vinyl monomers via their translocation through a single layer graphene to a monolayer initiator and additionally study the monomer-graphene interactions.
- Tao Zhang
- , Zhongquan Liao
- & Rainer Jordan
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Article
| Open AccessUniform doping of graphene close to the Dirac point by polymer-assisted assembly of molecular dopants
Incorporating dopants in the graphene lattice to tune its electronic properties is a challenging task. Here, the authors report a strategy to dope epitaxial large-area graphene on SiC by means of spin-coating deposition of F4TCNQ polymers in ambient conditions.
- Hans He
- , Kyung Ho Kim
- & Samuel Lara-Avila
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Article
| Open AccessLight-induced mechanical response in crosslinked liquid-crystalline polymers with photoswitchable glass transition temperatures
Energy conversion of light into mechanical work is of fundamental interest for a wide range of applications, but the development of efficient light responsive polymers is challenging. Here the authors demonstrate photoswitchable glass transition temperatures contribute to the photomechanical bending in a crosslinked azobenzene polymer.
- Youfeng Yue
- , Yasuo Norikane
- & Emiko Koyama
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Article
| Open AccessUnraveling substituent effects on the glass transition temperatures of biorenewable polyesters
Biorenewable feedstocks allow the design of polymers with targeted properties and functionalities. Here the authors report a series of high glass transition temperature sugar-based polyesters and investigate how substituents affect their thermal properties.
- Xiaopeng Yu
- , Junteng Jia
- & Robert A. DiStasio Jr.
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Article
| Open AccessCopolymer dielectrics with balanced chain-packing density and surface polarity for high-performance flexible organic electronics
Developing large-scale flexible display technologies calls for new gate dielectric materials balancing the insulating property and molecular packing of organic semiconductors. Ji et al. synthesize a dielectric copolymer contributing with charge mobility of 5 cm2 V−1 s−1 and low operating voltage of 3 V.
- Deyang Ji
- , Tao Li
- & Wenping Hu
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Article
| Open AccessMolecular understanding of polyelectrolyte binders that actively regulate ion transport in sulfur cathodes
Polymer binders in battery electrodes can affect their performance, however design rules are still lacking. Here, the authors reveal why polyelectrolyte binders outperform charge-neutral alternatives in lithium–sulfur batteries, showing how cationic polyelectrolytes can regulate ion transport selectively.
- Longjun Li
- , Tod A. Pascal
- & Brett A. Helms
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Article
| Open AccessThe introduction of the Barbier reaction into polymer chemistry
The Barbier reaction, a widely utilized reaction for carbon–carbon bond formation, has played important roles in modern organic chemistry. Here, the authors show a one-pot Barbier polyaddition reaction of monomers containing an organic halide and a benzoyl group to form a series of phenylmethanol group containing polymers.
- Xiao-Li Sun
- , Dong-Ming Liu
- & Wen-Ming Wan