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| Open AccessStabilizing copper sites in coordination polymers toward efficient electrochemical C-C coupling
Typically, Cu catalysts agglomerate under electrochemical conditions. Here, the authors report a coordination polymer catalyst with neighboring Cu sites which remain isolated and reduce CO2 to C2H4 with high selectivity and stability
- Yongxiang Liang
- , Jiankang Zhao
- & Jie Zeng
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Article
| Open AccessMulticolor hyperafterglow from isolated fluorescence chromophores
The development of organic afterglow materials with sufficient color purity and high quantum efficiency for hyperafterglow is a great challenging. Here, the authors demonstrate an efficient strategy to achieve hyperafterglow emission through sensitizing and stabilizing isolated fluorescence chromophores by integrating multiresonance fluorescence chromophores into afterglow host in a singlecomponent copolymer.
- Xiao Zhang
- , Mingjian Zeng
- & Wei Huang
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Article
| Open AccessEndosomal sorting results in a selective separation of the protein corona from nanoparticles
Protein corona formation on nanoparticles and the resultant effects on cellular interactions is well documented, where less is known about the fate of the corona in the cell. Here, the authors track the protein corona and nanoparticles in cells and describe the separation and different processing within different cellular compartments.
- Shen Han
- , Richard da Costa Marques
- & Ingo Lieberwirth
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Article
| Open AccessMechanochemically accessing a challenging-to-synthesize depolymerizable polymer
Polymers with low ceiling temperatures (Tc) are highly desirable as they can depolymerize under mild conditions, but they typically suffer from demanding synthetic conditions and poor stability. Here, the authors envision that this challenge can be addressed by developing high-Tc polymers that can be converted into low-Tc polymers on demand.
- Tze-Gang Hsu
- , Shiqi Liu
- & Junpeng Wang
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Article
| Open Access2D conjugated microporous polyacetylenes synthesized via halogen-bond-assisted radical solid-phase polymerization for high-performance metal-ion absorbents
Polyacetylenes are an important class of conjugated polymers but are generally synthesized via metal-catalyzed coordination polymerization leaving trace metals as impurities. Here the authors demonstrate a free radical polymerization of co-crystalized acetylene monomers without the need of a metal catalyst.
- Hong Tho Le
- , Chen-Gang Wang
- & Atsushi Goto
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Article
| Open AccessMachine learning models to accelerate the design of polymeric long-acting injectables
Polymer-based long-acting injectable drugs are a promising therapeutic strategy for chronic diseases. Here the authors use machine learning to inform the data-driven development of advanced drug formulations.
- Pauric Bannigan
- , Zeqing Bao
- & Christine Allen
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Article
| Open AccessThe effect of residual palladium on the performance of organic electrochemical transistors
The optimization of organic mixed ionic-electronic conductor is critical to realize high performance organic electrochemical transistors. Here, the authors demonstrate the removal of residual palladium impurities to be the key factor to achieving a figure-of-merit of [μC*] of over 2000 V−1 cm−1 s−1.
- Sophie Griggs
- , Adam Marks
- & Iain McCulloch
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Article
| Open AccessClosed-loop chemical recycling of cross-linked polymeric materials based on reversible amidation chemistry
Closed-loop chemical recycling provides a solution to the end-of-use problem of synthetic polymers but the design of dynamic bonds for preparing chemically recyclable cross-linked polymers remains challenging. Here, the authors report a dynamic reversible amidation reaction between maleic anhydrides and secondary amines.
- Bo Qin
- , Siyuan Liu
- & Xi Zhang
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Article
| Open AccessOvercoming the low reactivity of biobased, secondary diols in polyester synthesis
Glucose-derived isosorbide is a rigid polyester monomer with a low reactivity. Here, the authors report the synthesis of high molecular weight biobased polyesters with promising barrier and mechanical properties via in situ generation of reactive aryl ester groups.
- Daniel H. Weinland
- , Kevin van der Maas
- & Gert-Jan M. Gruter
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Article
| Open AccessModular stimuli-responsive hydrogel sealants for early gastrointestinal leak detection and containment
Digestive surgical leaks manifesting days after a successful surgery can lead to severe complications and affect healthcare worldwide. Here, the authors address the problem holistically with a hydrogel patch capable of sealing tissues, while detecting imminent leaks via a smartphone-operated ultrasound probe.
- Alexandre H. C. Anthis
- , Maria Paulene Abundo
- & Inge K. Herrmann
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Article
| Open AccessPrecise tuning of interlayer electronic coupling in layered conductive metal-organic frameworks
Layered metal-organic frameworks attract interests for optoelectronics and spintronics. Here, the authors report a strategy to tune interlayer charge transport and thermoelectric properties via side-chain induced control of the layer spacing.
- Yang Lu
- , Yingying Zhang
- & Renhao Dong
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Article
| Open AccessSpatially nanoconfined N-type polymer semiconductors for stretchable ultrasensitive X-ray detection
Wearable and skin-like X-ray detectors need intrinsic flexibility and high sensitivity. Here Guo et al. develop a stretchable n-type polymer semiconductor with aligned nanofiber networks which achieve photosensitivity of 1.52×10^4 μC Gyair^-1 cm^−2 and low detection limit of 37.7 nGyair s^-1.
- Yangshuang Bian
- , Kai Liu
- & Yunlong Guo
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Article
| Open AccessStereoisomeric engineering of aggregation-induced emission photosensitizers towards fungal killing
Fungal infections are often major causes of disease in immune compromised patients and photodynamic therapy offers and attractive treatment. Here, the authors develop stereoisomeric photosensitizers via supramolecular assembly and demonstrate aggregation-induced photodynamic action against fungi.
- Wenping Zhu
- , Ying Li
- & Ben Zhong Tang
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Article
| Open AccessAqueous synthesis of highly functional, hydrophobic, and chemically recyclable cellulose nanomaterials through oxime ligation
Water is a standing challenge in the chemical modification of cellulose nanofibrils. Here, authors employ oxime-ligation to solve this by direct covalent chemistry on dialdehyde-CNF in water and assess the material for potential applications in green electronics and triboelectric nanogenerators.
- Elena Subbotina
- , Farsa Ram
- & Peter Olsén
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Article
| Open AccessExplosive percolation yields highly-conductive polymer nanocomposites
Materials with correlated localisation of percolating particles and emergent conductive paths can realise sharp transitions and high conductivities characteristic of the explosively-grown network. Here the authors exploit explosive percolation to realize a low-loading composite material with enhanced electrical properties by in-situ reduction of graphene oxide.
- Manuela Meloni
- , Matthew J. Large
- & Alan B. Dalton
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Article
| Open AccessPeptide-enhanced tough, resilient and adhesive eutectogels for highly reliable strain/pressure sensing under extreme conditions
Biomimetic hydrogel materials show outstanding mechanical properties but water as solvent or carrier limits the possibility to apply these materials under extreme conditions. Here the authors report a peptide-enhanced eutectogel with excellent mechanical, anti-freezing and anti-drying properties and its application as sensor for monitoring human motion.
- Yan Zhang
- , Yafei Wang
- & Yongjun Zhang
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Article
| Open AccessTemporally programmed polymer – solvent interactions using a chemical reaction network
Out of equilibrium operation of chemical reaction networks. (CRNs) enables materials to autonomously respond to their environment by activation and deactivation of intermolecular interactions but the deactivation to noninteracting building blocks remains understudied. Here, the authors develop a new, modular CRN that enables control over the deactivation kinetics.
- Benjamin Klemm
- , Reece W. Lewis
- & Rienk Eelkema
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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 AccessUntangling the threads of cellulose mercerization
During mercerization, cellulose undergoes a conversion from form I to form II which involves change of the direction of every other cellulose chain but a clear understanding of how this change happens is lacking. Here, the authors use neutron diffraction on deuterium labelled cellulose to demonstrate that chains fold back on themselves in a zigzag pattern to form crystalline anti-parallel domains.
- Daisuke Sawada
- , Yoshiharu Nishiyama
- & Paul Langan
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| Open AccessMain-chain engineering of polymer photocatalysts with hydrophilic non-conjugated segments for visible-light-driven hydrogen evolution
The introduction of hydrophilic segments into the main-chain of polymer photocatalysts allows water to efficiently enter the interior through these hydrophilic segments, and results in effective water/polymer interfaces for hydrogen evolution.
- Chih-Li Chang
- , Wei-Cheng Lin
- & Ho-Hsiu Chou
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Article
| Open AccessSynthesis, properties, and material hybridization of bare aromatic polymers enabled by dendrimer support
Unsubstituted aromatic polymers are materials with multiple potential applications, but their preparation remains challenging. Here, the authors report a dendrimer-enabled synthesis of soluble bare aromatic polymers and explore their properties; these compounds can be further transformed into other materials.
- Shusei Fujiki
- , Kazuma Amaike
- & Kenichiro Itami
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Article
| Open AccessHigh performance polymerized small molecule acceptor by synergistic optimization on π-bridge linker and side chain
The modification of small molecule acceptor building block and π−bridge linker is effective to improve photovoltaic performance. Here, the authors replace linear with branched alkyl chains and introduce difluorene-substituted linker to realise all-polymer solar cells with efficiency of 17.24%.
- Guangpei Sun
- , Xin Jiang
- & Yongfang Li
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Article
| Open AccessControllable synthesis of conjugated microporous polymer films for ultrasensitive detection of chemical warfare agents
The high toxicity of nerve agents makes the development of fluorescence sensors with suitable limit of detection challenging. Here, the authors propose a sensor design based on a conjugated microporous polymer film for the detection of diethyl chlorophosphate, a substitute of Sarin, with low detection limit of 2.5 ppt.
- Wanqi Mo
- , Zihao Zhu
- & Bin Li
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Article
| Open AccessMicrospheres from light—a sustainable materials platform
Photopolymerization provides a safe and mild fabrication pathway towards polymeric particles but the implementation of photochemistry from solution to dispersed media to produce particles is far from trivial. Here, the authors demonstrate an additive-free step-growth photopolymerization with sunlight, exploiting the photoinduced Diels-Alder to fabricate micrometer sized polymeric particles.
- Laura Delafresnaye
- , Florian Feist
- & Christopher Barner-Kowollik
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Article
| Open AccessChemical zymogens for the protein cysteinome
Reversible on/off switches for enzyme activity are foundational in nature but are challenging to design using tools of synthetic chemistry. Here the authors design chemical zymogens amenable for activation via biomolecular interactions.
- Mireia Casanovas Montasell
- , Pere Monge
- & Alexander N. Zelikin
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Article
| Open AccessPhase-locked constructing dynamic supramolecular ionic conductive elastomers with superior toughness, autonomous self-healing and recyclability
Stretchable ionic conductors are attractive candidates for flexible ionotronics but combining high conductivity with excellent mechanical properties is challenging. Herein, the authors combine these properties in a dynamic supramolecular ionic conductive elastomer enabling lithium-ion transport in the soft phase and dynamic disulfide and supramolecular hydrogen bonding in the hard segments.
- Jing Chen
- , Yiyang Gao
- & Shujiang Ding
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Article
| Open AccessMechanochemical synthesis of inverse vulcanized polymers
Inverse vulcanization is a process that enables to convert sulfur, a by-product of the petroleum industry, into polymers. Here the authors report a synthetic method of inverse vulcanization via mechanochemical synthesis; compared to thermal routes, a broader range of monomers can be used, and the protocol yields materials with enhanced mercury capture capacity.
- Peiyao Yan
- , Wei Zhao
- & Tom Hasell
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Article
| Open AccessSynthesis of bioactive (1→6)-β-glucose branched poly-amido-saccharides that stimulate and induce M1 polarization in macrophages
Difficulty with purification, structural heterogenicity, and limited water solubility of β-glucans has significantly limited their therapeutic applications. Here, the authors report the synthesis of (1→6)-β-glucose-branched poly-amido-saccharides as glycan-mimetics and demonstrate macrophage stimulation and polarization.
- Ruiqing Xiao
- , Jialiu Zeng
- & Mark W. Grinstaff
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Article
| Open AccessReactive oxygen species-responsive and Raman-traceable hydrogel combining photodynamic and immune therapy for postsurgical cancer treatment
Combined immune checkpoint blockade (ICB) and photodynamic therapies have huge potential but suffer from possible damage of the antibodies. Here, the authors create a ROS-responsive hydrogel that protects the ICB antibodies and allows for sustained co-delivery and demonstrate restrained regrowth of tumours in vivo.
- Yiyi Zhang
- , Sidan Tian
- & Liang Luo
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Article
| Open AccessCopper-catalyzed Z-selective synthesis of acrylamides and polyacrylamides via alkylidene ketenimines
Alkylidene ketenimines are rarely reported, but synthetically useful, reactive intermediates. Here, the authors disclose a three-component reaction of alkyne, azide and water by cycloaddition, nitrogen extrusion, and carbene-assisted rearrangement, via in situ formation of alkylidene ketenimine.
- Xuelun Duan
- , Nan Zheng
- & Wangze Song
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Article
| Open AccessPrecision cancer sono-immunotherapy using deep-tissue activatable semiconducting polymer immunomodulatory nanoparticles
To improve the specificity of immunotherapy, here the authors report the design of a semiconducting polymer immunomodulatory nanoparticle with sonodynamic process to remotely release immune-modulators for deep-tissue precision cancer sono-immunotherapy.
- Jingchao Li
- , Yu Luo
- & Ruiping Zhang
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Article
| Open AccessSignal-processing and adaptive prototissue formation in metabolic DNA protocells
Signal processing for downstream functional and morphological adaptations is crucial for understanding and re-enacting features of living systems. Here, the authors show DNAzyme-containing, metabolic protocells that induce prototissue formation via chemical messenger communication due to in situ cleavage of upstream DNA signals.
- Avik Samanta
- , Maximilian Hörner
- & Andreas Walther
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Article
| Open AccessMulti-scale computer-aided design and photo-controlled macromolecular synthesis boosting uranium harvesting from seawater
Developing materials for uranium harvesting from seawater with high adsorption capacity remains challenging. Here, the authors develop a new protocol, by combining multi-scale computational simulations with the PET-RAFT polymerization, for rational design and precise synthesis of block copolymers with optimal architectures and atomic economy, achieving a capacity of 11.4 mg/g within 28 days.
- Zeyu Liu
- , Youshi Lan
- & Gang Ye
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Article
| Open AccessAnionic polymerization of nonaromatic maleimide to achieve full-color nonconventional luminescence
Nonconventional luminophores without extended π-conjugation is a rising star in the area of luminescent materials but continuously tuning the emission color within a broad visible region via rational molecular design remains challenging. Here, the authors present poly(maleimide)s as a new class of nonconventional luminophores with fully tunable room temperature color emission that can be regulated by anionic polymerization
- Xin Ji
- , Weiguo Tian
- & Jun Zhang
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Article
| Open AccessVisible light-controlled living cationic polymerization of methoxystyrene
Photo-controlled living polymerization has received great attention in recent years but the reports on photo-controlled living cationic polymerization are limited. Here, the authors demonstrate a metal-free and visible light-controlled living cationic polymerization using a photocatalyst and a phosphate as the chain transfer agent for the polymerization of 4-methoxystyrene.
- Lei Wang
- , Yupo Xu
- & Yongfeng Zhou
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Article
| Open AccessNano- to macro-scale control of 3D printed materials via polymerization induced microphase separation
3D printing allows the macroscopic structure of objects to be easily controlled but controlling the nanostructure of 3D printed materials has rarely been reported. Here, the authors report an efficient and versatile process for fabricating 3D printed materials with controlled nano-scale structural features.
- Valentin A. Bobrin
- , Yin Yao
- & Cyrille Boyer
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Article
| Open AccessAnomalous thermo-osmotic conversion performance of ionic covalent-organic-framework membranes in response to charge variations
The development of ionic membranes with a high charge population is critical for realizing efficient thermo-osmotic energy conversion. Here, the authors demonstrated that the thermo-osmotic energy conversion efficiency can be improved by increasing the membrane charge density but this enhancement only occurs within a narrow window.
- Weipeng Xian
- , Xiuhui Zuo
- & Qi Sun
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Article
| Open AccessForce–reversible chemical reaction at ambient temperature for designing toughened dynamic covalent polymer networks
Weak force-activated covalent bonds as crosslink points can increase mechanical strength and ductility in polymers but the bonds, once broken, cannot be reformed in real time under ambient conditions leading to irreversible damage. Here, the authors demonstrate that triazolinedione (TAD)-indole adducts acting as crosslink points enable materials to display already at ambient temperature reversible stress-responsiveness in real time.
- Mengqi Du
- , Hannes A. Houck
- & Guanjun Chang
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Article
| Open AccessEfficient aqueous remote loading of peptides in poly(lactic-co-glycolic acid)
Encapsulation of bioactive peptides in slow-release particles is complex and relies on organic solvents. Here, the authors absorb peptides in a polymer phase from water, creating a simple low-cost encapsulation process in a class of polymer depot.
- Morgan B. Giles
- , Justin K. Y. Hong
- & Steven P. Schwendeman
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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 AccessVinyl copolymers with faster hydrolytic degradation than aliphatic polyesters and tunable upper critical solution temperatures
The non-degradability of vinyl polymers has long limited their use in biomedical applications. In this article, the authors demonstrate a system based on acrylamide and cyclic ketene acetals to obtain copolymers with faster degradation rates for potential drug release and environmental applications.
- Amaury Bossion
- , Chen Zhu
- & Julien Nicolas
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Article
| Open AccessThioesters provide a plausible prebiotic path to proto-peptides
One of the early processes enabling the origins of life is thought to be the condensation of building blocks into oligomers and polymers. In this article, the authors report the synthesis of thiodepsipeptides and HS-peptides under mild temperatures and various pH, suggesting they could have formed on early prebiotic Earth.
- Moran Frenkel-Pinter
- , Marcos Bouza
- & Aikomari Guzman-Martinez
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Article
| Open AccessCovalent organic frameworks with high quantum efficiency in sacrificial photocatalytic hydrogen evolution
While organic semiconductors offer a tunable platform for photocatalysis, they often show worse performances. Here, authors examine how a donor-acceptor pair’s incorporation into a covalent organic framework boosts photocatalytic H2 evolution performances with a platinum co-catalyst.
- Chunzhi Li
- , Jiali Liu
- & Qihua Yang
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Article
| Open AccessSuperstretchable, yet stiff, fatigue-resistant ligament-like elastomers
Stiffness, toughness, and fatigue resistance are seemingly incompatible in materials design. Here the authors demonstrate a hierarchical crosslinking strategy using lithium ion oxygen interactions and PMMA nanoaggregates to enable energy dissipation in the network, leading to stiff yet tough polymer materials.
- Mengxue Li
- , Lili Chen
- & Chao Wang
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Article
| Open AccessHigh-mobility semiconducting polymers with different spin ground states
Semiconducting polymers with high-spin at their neutral ground state are rarely reported. Here the authors synthesize three semiconducting polymers with different spin ground states and high hole/electron mobility, by appropriate choice of the building blocks’ singlet-triplet energy gap, spin distributions and solid-state interchain interactions.
- Xiao-Xiang Chen
- , Jia-Tong Li
- & Ting Lei
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Article
| Open AccessToward azo-linked covalent organic frameworks by developing linkage chemistry via linker exchange
Exploring new linkage chemistry for covalent organic frameworks (COFs) provides a strong driving force to promote the development of this class porous materials. Here, the authors report a strategy to synthesize COFs with azo linkages based on an in situ linker exchange strategy which transforms imine-linked COFs into their azo-linked counterparts, and explore the unique properties of azo-linked COFs.
- Zhi-Bei Zhou
- , Peng-Ju Tian
- & Xin Zhao
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Article
| Open AccessLateral growth of cylinders
Precise control of the microstructure of nanomaterials is of interest but living lateral growth of cylinders is still very challenging. Here, the authors propose a crystallization-driven fusion-induced particle assembly strategy to prepare cylinders with growing diameters by controlled fusion of spherical micelles self-assembled from an amphiphilic homopolymer.
- Hui Sun
- , Shuai Chen
- & Jianzhong Du
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Article
| Open AccessNon-metallic T2-MRI agents based on conjugated polymers
The toxicity of heavy metals for MRI contrast agents is an issue. Here, the authors report on the development of conjugated polymers nanoparticles based on paramagnetic polypyrrole to generate T2 MRI contrast effects by changing the interactions between polarons and water protons.
- Qinrui Lin
- , Yuhong Yang
- & Zhengzhong Shao
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Article
| Open AccessUltrastrong underwater adhesion on diverse substrates using non-canonical phenolic groups
Realizing robust underwater adhesion is challenging because a hydration layer impedes the interaction between substrates and adhesives. Here, the authors report a class of ultrastrong underwater adhesives with molecular non-canonical phenolic groups in a polymer to realize strong adhesion on various substrates.
- Bohan Cheng
- , Jinhong Yu
- & Hirotaka Ejima