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| Open AccessDouble cross-linked 3D layered PBI proton exchange membranes for stable fuel cell performance above 200 °C
Phosphoric acid (PA) doped proton exchange membranes (PEMs) often degrade above 200 °C due to membrane creeping, PA dehydration, and condensation. Here, the authors introduce gel-state polybenzimidazole PEMs with double cross-linked 3D layered structures, enabling efficient and stable fuel cell operation above 200 °C.
- Liang Zhang
- , Mengjiao Liu
- & Lixin Xue
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Article
| Open AccessIterative SuFEx approach for sequence-regulated oligosulfates and its extension to periodic copolymers
The synthesis of sequence-regulated oligosulfates has not yet been established due to the difficulties in precise reactivity control. Here, the authors report a multi-directional divergent iterative method to furnish oligosulfates based on a chain homologation approach, in which the fluorosulfate unit is regenerated.
- Min Pyeong Kim
- , Swatilekha Kayal
- & Sung You Hong
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Article
| Open AccessX-ray-activated polymerization expanding the frontiers of deep-tissue hydrogel formation
Photo-crosslinking polymerization facilitates precise control of hydrogel formation for various applications including tissue engineering, but most existing photo-crosslinking methods fail to achieve deep-tissue penetration, especially within bone structures. Here the authors report a strategy of low-dose X-ray-activated polymerization that enables deep-tissue hydrogel formation.
- Hailei Zhang
- , Boyan Tang
- & Gang Han
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Article
| Open AccessKinetically controlled metal-elastomer nanophases for environmentally resilient stretchable electronics
Metal-elastomer nanophases are critical for stretchable electronics but face mixing challenges. This study introduces a kinetic method for precise mixing, yielding gyrified nanophases with improved durability and strain-invariant conductivity, which holds promise for resilient stretchable devices.
- Soosang Chae
- , Won Jin Choi
- & Tae Il Lee
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Article
| Open AccessClosed-loop recycling of sulfur-rich polymers with tunable properties spanning thermoplastics, elastomers, and vitrimers
Sulfur-rich polymers are promising candidates for chemical recycling but lack efficient synthetic strategies for achieving diverse structures. Here, the authors report a synthesis strategy for polytrithiocarbonates which is compatible with a wide range of monomers enabling diverse structures via polycondensation of dithiols and dimethyl trithiocarbonate.
- Jin-Zhuo Zhao
- , Tian-Jun Yue
- & Wei-Min Ren
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Article
| Open AccessConvoluted micellar morphological transitions driven by tailorable mesogenic ordering effect from discotic mesogen-containing block copolymer
Assembly of block copolymers can be controlled to give varying morphologies and functionalities, but there are still aspects of the process that are not well understood. Here, the authors report convoluted self-assembly behaviours of block copolymers with discotic liquid crystalline moieties.
- Huanzhi Yang
- , Yunjun Luo
- & Xiaoyu Li
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Article
| Open AccessLong lifetimes white afterglow in slightly crosslinked polymer systems
It is challenging to achieve multicolor long-lived room temperature phosphorescence in intrinsic polymers, especially for white afterglow. Here, the authors report a strategy to obtain pure white afterglow micro-crosslinked polymers by covalently coupling different conjugated chromophores with precursors through a simple and rapid one-pot reaction.
- Qingao Chen
- , Lunjun Qu
- & Chaolong Yang
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Article
| Open AccessUltraviolet light blocking optically clear adhesives for foldable displays via highly efficient visible-light curing
The slow curing speed of UV-based methods to produce UV-blocking optically clear adhesive (OCA) for display panels poses a barrier to commercialization. Here, authors introduce a visible-light driven photo-initiating system for rapid production of OCAs, demonstrating efficient UV-blocking ability.
- Yonghwan Kwon
- , Seokju Lee
- & Min Sang Kwon
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Review Article
| Open AccessLight-driven polymer recycling to monomers and small molecules
Chemical recycling of plastic enables renewed production of pristine materials, but generally comes at a high energy cost. This review focuses on light-driven approaches for chemically recycling and upcycling plastic waste, with emphasis on reduced energy consumption and selective transformations of challenging to recycle backbone structures.
- Laura Wimberger
- , Gervase Ng
- & Cyrille Boyer
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Article
| Open AccessEncoding ordered structural complexity to covalent organic frameworks
Starting from simple building blocks with specific molecular packing geometries, here, the authors synthesized structurally complex covalent organic framework COF-305 with nine different stereoisomers of its constituents showing specific sequences on topologically equivalent sites.
- Lei Wei
- , Xinyue Hai
- & Yingbo Zhao
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Article
| Open AccessLight and matter co-confined multi-photon lithography
Mask-free multi-photon lithography allows the straightforward fabrication of nanostructures, but high precision and good resolution can be challenging to achieve. Here, the authors report a combination of photo-inhibition and chemical quenchers for improved lithography performance.
- Lingling Guan
- , Chun Cao
- & Xu Liu
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Article
| Open Access3D printing by stereolithography using thermal initiators
Common stereolithography-based 3D printing relies on photopolymerization using photoinitiators. Here, the authors replace the conventional photoinitiators with low-cost, widely used thermal initiators to achieve 3D-printed objects.
- Doron Kam
- , Omri Rulf
- & Shlomo Magdassi
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Article
| Open AccessTuning polymer-backbone coplanarity and conformational order to achieve high-performance printed all-polymer solar cells
All-polymer solar cells comprising both polymeric donors and acceptors offer better morphological and mechanical stability, and a broader processing window for printing. Here, the authors report a polymer acceptor based on bithiazole linker with more coplanar and ordered molecular conformation.
- Yilei Wu
- , Yue Yuan
- & Zhenan Bao
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Article
| Open AccessEffect of inorganic material surface chemistry on structures and fracture behaviours of epoxy resin
The mechanisms of adhesion between polymers and inorganic materials are not fully understood. Here, authors demonstrate the clear evidence that the surface chemistry impacts the crosslinked structures of resins near the interfaces, resulting in different fracture behaviours and adhesive strengths.
- Tomohiro Miyata
- , Yohei K. Sato
- & Hiroshi Jinnai
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Article
| Open AccessUltrafast underwater self-healing piezo-ionic elastomer via dynamic hydrophobic-hydrolytic domains
Elastomers capable of autonomous self-healing and mechanical stimulus sensing in aquatic environments are interesting for applications in underwater soft electronics. Here, the authors present a hydrophobic-hydrolytic molecularly engineered self-healing piezo-ionic elastomer with underwater self-healing properties and mechanosensitive ion channels.
- Zhengyang Kong
- , Elvis K. Boahen
- & Do Hwan Kim
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Article
| Open AccessWater-dispersible X-ray scintillators enabling coating and blending with polymer materials for multiple applications
Water dispersible X-ray scintillators are highly desirable for multiple application scenarios. Zhang et al report the synthesis of new X-ray scintillator nanocrystals anchored on the surface of water dispersible halloysite nanotubes, enabling radiation exposure monitoring, flexible scintillator screens, and information encryption.
- Hailei Zhang
- , Bo Zhang
- & Richard Hoogenboom
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Article
| Open AccessEndogenous stimuli-responsive separating microneedles to inhibit hypertrophic scar through remodeling the pathological microenvironment
The treatment of hypertrophic scar (HS) is hindered by the low bioavailability of drugs and the pathological microenvironment. Here the authors report a separating microneedle drug delivery system responsive to high reactive oxygen species levels and overexpression of matrix metalloproteinases to remodel the pathological microenvironment for HS treatment.
- Zhuo-Ran Yang
- , Huinan Suo
- & Jintao Zhu
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Article
| Open AccessPhotocured room temperature phosphorescent materials from lignosulfonate
It is elusive to manufacture room temperature phosphorescent (RTP) materials through effective and ambient processing approaches. Here the authors report the production of photocured RTP materials using lignosulfonate to act as RTP chromophore and photoinitiator, achieving easy preparation, low cost and good performance.
- Hongda Guo
- , Mengnan Cao
- & Zhijun Chen
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Article
| 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 AccessReal-time monitoring polymerization degree of organic photovoltaic materials toward no batch-to-batch variations in device performance
Polymerization degree plays a vital role in controlling material properties and batch-to-batch variations in device performance of polymer solar cells. Here, authors develop in-situ photoluminescence system in tandem to track and estimate the polymerization degree of organic photovoltaic materials.
- Lin-Yong Xu
- , Wei Wang
- & Jie Min
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Article
| Open AccessNatural diversity screening, assay development, and characterization of nylon-6 enzymatic depolymerization
Polyamides (PAs) or nylons are types of plastics with wide applications, but due to their accumulation in the environment, strategies for their deconstruction are of interest. Here, the authors screen 40 potential nylon-hydrolyzing enzymes (nylonases) using a mass spectrometry-based approach and identify a thermostabilized N-terminal nucleophile hydrolase as the most promising for further development, as well as crucial targets for progressing PA6 enzymatic depolymerization.
- Elizabeth L. Bell
- , Gloria Rosetto
- & Gregg T. Beckham
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Article
| Open AccessCreating amphiphilic porosity in two-dimensional covalent organic frameworks via steric-hindrance-mediated precision hydrophilic-hydrophobic microphase separation
Creating different pore environments within a covalent organic framework (COF) leads to useful multicompartment structure and multiple functions. Here, the authors propose a strategy to construct amphiphilic COFs with separated hydrophilic and hydrophobic nanochannels by precisely controlling the distribution of hydrophilic and hydrophobic segments in two different kinds of pores.
- Shu-Yan Jiang
- , Zhi-Bei Zhou
- & Xin Zhao
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Article
| Open AccessOvercoming small-bandgap charge recombination in visible and NIR-light-driven hydrogen evolution by engineering the polymer photocatalyst structure
Designing an organic polymer photocatalyst for efficient hydrogen evolution in the near-infrared (NIR) light region is still a major challenge. The authors present here a series of polymer nanoparticles for a efficient hydrogen evolution under visible and NIR light irradiation, without combining or hybridizing with other materials.
- Mohamed Hammad Elsayed
- , Mohamed Abdellah
- & Ho-Hsiu Chou
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Article
| Open AccessCultured meat with enriched organoleptic properties by regulating cell differentiation
Achieving organoleptic properties of conventional meat is important for cultured meat production. Here, the authors demonstrate that the texture, flavor, and nutritional content of cultured meat can be significantly enhanced by regulating cell differentiation inside hydrogel scaffolds.
- Milae Lee
- , Sohyeon Park
- & Jinkee Hong
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Article
| Open AccessHighly stretchable polymer semiconductor thin films with multi-modal energy dissipation and high relative stretchability
Stretchable polymer semiconductors with high mechanical and electrical properties are challenging to develop. Wu et al. show that reversible molecular ordering under strain important for performance optimization and relative stretchability can be used to compare the relative strain tolerance of materials.
- Hung-Chin Wu
- , Shayla Nikzad
- & Zhenan Bao
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Article
| Open AccessHydrogen-bonding and π-π interaction promoted solution-processable covalent organic frameworks
Covalent organic frameworks are generally not dispersible in common solvents resulting in the poor processability which limits their practical application. Here, the authors develop a top-down process to produce solution-processable covalent organic frameworks based on the assistance of ionic liquids by means of intermolecular hydrogen bonding and π-π interactions.
- Lei Zhang
- , Qiu-Hong Zhu
- & Ling He
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Article
| Open AccessTough soldering for stretchable electronics by small-molecule modulated interfacial assemblies
“The interface mismatch of soft substrates and rigid silicon-based microelectronics frequently causes failures of integrated circuits. Here, the authors develop a stretchable solder based on liquid metal-polymer composites which enables seamless integration of electronic components with soft substrates, showcasing high conductivity and stretchability”.
- Liqing Ai
- , Weikang Lin
- & Xi Yao
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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 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 AccessResorbable barrier polymers for flexible bioelectronics
Resorbable bioelectronic devices have potential as tools for monitoring physiological parameters, but short functional lifetimes have slowed translation. Here, the authors report succinate-based copolyesters with barrier properties able to extend the functional lifetime of devices.
- Samantha M. McDonald
- , Quansan Yang
- & Matthew L. Becker
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Article
| Open AccessSite-selected in situ polymerization for living cell surface engineering
Constructing polymer-based mimics on the surface of cells has potential to manipulate cell behavior, but precise control of grafting sites is challenging. Here, the authors report a method for site selected radical polymerization on cell surfaces by metabolic labelling.
- Yihong Zhong
- , Lijia Xu
- & Huangxian Ju
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Article
| Open AccessThermo-responsive chiral micelles as recyclable organocatalyst for asymmetric Rauhut-Currier reaction in water
Developing eco-friendly chiral organocatalysts with the combined advantages of homogeneous catalysis and heterogeneous processes is challenging. Here, the authors present, a family of amphiphilic one handed helical polyisocyanides bearing phosphine pendants which self-assembled into well-defined chiral micelles in water and show thermo-responsiveness
- Lei Xu
- , Li Zhou
- & Zong-Quan Wu
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Article
| Open AccessStepwise taming of triplet excitons via multiple confinements in intrinsic polymers for long-lived room-temperature phosphorescence
Materials with room temperature phosphorescence have potential in a range of applications, but preparing the systems can still be challenging. Here, the authors report an intrinsically polymeric room temperature phosphorescent material, applied in crack detection.
- Liang Gao
- , Jiayue Huang
- & Chaolong Yang
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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 AccessCharge-altering releasable transporters enhance mRNA delivery in vitro and exhibit in vivo tropism
Polymers are promising for mRNA delivery, but can have limited efficacy in hard to transfect cells. Here, the authors report charge-altering releasable transporters for improved mRNA transfection in primary T-lymphocytes and enhanced and selective protein expression in vivo.
- Zhijian Li
- , Laura Amaya
- & Paul A. Wender
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Article
| Open AccessNear-infrared-II photoacoustic imaging and photo-triggered synergistic treatment of thrombosis via fibrin-specific homopolymer nanoparticles
The near-infrared-II (NIR-II) window has shown great promise for in vivo imaging and therapy. Here, the authors integrate a homopolymer and thermo-sensitive nitric oxide prodrug into nanoparticles for long-wavelength NIR-II photoacoustic imaging and synergistic treatment in preclinical thrombosis models.
- Jianwen Song
- , Xiaoying Kang
- & Ji Qi
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Article
| Open AccessUpcycling fish scales through heating for steganography and Rhodamine B adsorption application
Waste materials including fish scales are increasingly being developed for alternative applications, but simple processing is required. Here, the authors report the treatment of fish scales to give fluorescent materials suitable for dye absorption.
- Malcolm Miao Geng Sow
- , Zheng Zhang
- & Sharon Xiaodai Lim
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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 AccessPorphene and porphite as porphyrin analogs of graphene and graphite
Here the authors report Zn porphene, a member of a new organic metalloporphene family. Similar to graphene, these also are fully conjugated 2D polymers, but are composed of fused metalloporphyrin rings.
- Thomas F. Magnera
- , Paul I. Dron
- & Josef Michl
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Article
| Open AccessTunable backbone-degradable robust tissue adhesives via in situ radical ring-opening polymerization
Adhesives with both robust adhesion and tunable degradability are clinically and ecologically vital, but their fabrication remains a formidable challenge. Here, the authors report in situ radical ring-opening polymerization-based design and potential biomedical applications of a backbone degradable robust adhesive.
- Ran Yang
- , Xu Zhang
- & Shifang Luan
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Article
| Open AccessPromoting multiexciton interactions in singlet fission and triplet fusion upconversion dendrimers
The impact of multiexcitonic through-space interactions in macromolecular architectures is poorly investigated. Here the authors use dendritic macromolecules to study the effect of interchromophore interactions on the dynamics of multiexciton generation and decay as a function of dendrimer generation.
- Guiying He
- , Emily M. Churchill
- & Luis M. Campos
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Article
| 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