Article
|
Open Access
Featured
-
-
Article
| Open AccessSynthesis and structure of a non-van-der-Waals two-dimensional coordination polymer with superconductivity
Two-dimensional conjugated coordination polymers can show large electrical conductivity. Here, the authors synthesize high-quality single crystals of Cu3BHT to unveil the atomic structure and intrinsic superconducting properties.
- Zhichao Pan
- , Xing Huang
- & Jin-Hu Dou
-
Article
| Open AccessMechano-adaptive meta-gels through synergistic chemical and physical information-processing
‘Functional adaptation after local mechanical stimulation is ubiquitous in nature but remains elusive in artificial systems. Here, the authors describe metamaterial hydrogels to sense mechanical stimuli with sharp force threshold, transmit this information and induce mechanical strengthening by growing nanofibril networks or soft robotic actuation through competitive swelling.
- Brigitta Dúzs
- , Oliver Skarsetz
- & Andreas Walther
-
Article
| Open AccessBifunctional and recyclable polyesters by chemoselective ring-opening polymerization of a δ-lactone derived from CO2 and butadiene
The δ-lactone 3-ethylidene-6-vinyltetrahydro-2H-pyran-2-one (EVP), synthesized by telomerization of CO2 with 1,3-butadiene, is a promising monomer for the direct use of CO2 in the synthesis of polymers, but its ring-opening polymerization (ROP) remains challenging. Here the authors report its chemoselective ROP using a phosphazene/urea binary catalyst, affording exclusively a linear unsaturated polyester which can be recycled back to the pristine monomer.
- Jinbo Zhang
- , Lihang Jiang
- & Zhibo Li
-
Article
| Open AccessVitrimer-like elastomers with rapid stress-relaxation by high-speed carboxy exchange through conjugate substitution reaction
Fast bond exchange reactions is critical for the design of vitrimer and vitrimer-like materials but are not sufficiently explored. Here, the authors use fast bond exchange between α-(acyloxymethyl)acrylate and carboxylic acid resulting in rapid stress relaxation and excellent processability owing to the highly efficient network rearrangement.
- Natsumi Nishiie
- , Ryo Kawatani
- & Yasuhiro Kohsaka
-
Article
| Open AccessChemically recyclable polyvinyl chloride-like plastics
The development of PVC-like plastics that can be depolymerized back to monomer contributes to a circular plastic economy but remains understudied. Here, the authors develop a series of chemically recyclable plastics from the reversible copolymerization of cyclic anhydride with chloral.
- Xun Zhang
- , Ximin Feng
- & Xinghong Zhang
-
Article
| Open AccessBiorenewable and circular polyolefin thermoplastic elastomers
Polymers capable of depolymerizing back to their own monomers offer a promising solution to address the challenges in polymer sustainability but chemical recycling of thermoplastic elastomers is relatively less studied. Here, the authors propose a chemically recyclable, semicrystalline and tough thermoplastic elastomer prepared via ring-opening metathesis polymerization of a fully biobased cyclic olefin.
- Ye Sha
- , Xiaofan Chen
- & Puyou Jia
-
Article
| Open AccessInverse ceria-nickel catalyst for enhanced C–O bond hydrogenolysis of biomass and polyether
Selective C-O bond scission is a challenging process for the transformation of biomass or plastic waste. This study reports an inverse ceria nickel catalyst showcasing enhanced hydrogenolysis activity and selectivity.
- Zelun Zhao
- , Guang Gao
- & Fuwei Li
-
Article
| Open Access{Co4O4} Cubanes in a conducting polymer matrix as bio-inspired molecular oxygen evolution catalysts
Cuboidal {Co4O4} complexes are attractive molecular water oxidation catalysts as they combine features of both heterogeneous and homogeneous catalysis with bio-inspired motifs, but their application requires stabilization strategies. Here, the authors introduce a conductive polymer-hybrid approach to covalently immobilize {Co4O4} clusters.
- Shangkun Li
- , Zeyi Zhang
- & Greta R. Patzke
-
Article
| Open AccessFluoropolymer sorbent for efficient and selective capturing of per- and polyfluorinated compounds
It is challenging to remove Per- and polyfluoroalkyl substances (PFAS) from water. Here, authors developed a polymer sorbent capable of selectively and efficiently removing PFAS from contaminated water sources to levels below detection limits.
- Zhuojing Yang
- , Yutong Zhu
- & Cheng Zhang
-
Article
| Open AccessThermal runaway prevention through scalable fabrication of safety reinforced layer in practical Li-ion batteries
The authors present a scalable method for implementing a thermo-responsive safety reinforced layer (SRL) in batteries, which enables immediate shutdown during internal short circuits and reduces the risk of overheating and explosions.
- In Taek Song
- , Joonkoo Kang
- & Kihwan Kim
-
Article
| Open AccessStereospecific supramolecular polymerization of nanoclusters into ultra-long helical chains and enantiomer separation
Understanding the mechanism for supramolecular polymer assembly from nanoclusters bearing hierarchy and homochirality is challenging. Here, the authors report a cooperative self-assembly strategy using ionic complexes with chiral surfactants through a nucleation-elongation growth mechanism with chiral self-sorting and prepare a permeable membrane for the separation of histidine derivatives.
- Zexi Zhu
- , Guohua Zhang
- & Lixin Wu
-
Article
| Open AccessFully recyclable and tough thermoplastic elastomers from simple bio-sourced δ-valerolactones
While a large number of chemically recyclable thermoplastics have been developed in recent years, technologically bio-based and fully recyclable thermoplastic elastomers (TPEs) with excellent mechanical properties are lacking. Here the authors demonstrate an all δvalerolactone-based polyester tri-BCP TPEs, which exhibit not only closed-loop chemical recyclability but also exceptional toughness.
- Kai Ma
- , Hai-Yan An
- & Tie-Qi Xu
-
Article
| Open AccessMaglev-fabricated long and biodegradable stent for interventional treatment of peripheral vessels
The interventional treatment of limb-threatening ischemia calls for a medical stent. Herein, a long and biodegradable stent appropriate for below-the-knee artery is developed based on a metal-polymer composite material, where a magnetic levitation is employed to achieve a homogeneous coating.
- Wanqian Zhang
- , Xian Gao
- & Jiandong Ding
-
Article
| Open AccessPolyphosphonate covalent organic frameworks
Covalent organic frameworks (COFs) can be synthesized through a wide range of reactions but phosphonate-COFs remained elusive. Here the authors report a polyphosphonate-COFs constructed via P-O-P linkages with good water and exceptional electrochemical stability.
- Ke Xu
- , Robert Oestreich
- & Gündoğ Yücesan
-
Article
| Open AccessResponsive circularly polarized ultralong room temperature phosphorescence materials with easy-to-scale and chiral-sensing performance
Circularly polarised room temperature materials have promising applications, but colour control is still challenging. Here, the authors report the development of these materials with full colour based on anionic cellulose derivatives and achiral luminophores.
- Jingxuan You
- , Chunchun Yin
- & Jinming Zhang
-
Article
| Open AccessAn anionic two dimensional covalent organic framework from tetratopic borate centres pillared by lithium ions
Non-covalent interactions facilitate the stacking of framework layers in two dimensional covalent organic frameworks playing an important role for the framework formation. Here, the authors describe a covalent organic framework with tetratopic borate linkages whose counter cations promote the framework layer interaction.
- Darosch Asgari
- , Julia Grüneberg
- & Arne Thomas
-
Article
| Open AccessMolecular control via dynamic bonding enables material responsiveness in additively manufactured metallo-polyelectrolytes
Metallopolyelectrolytes are versatile materials for various applications, utilizing dynamic, reversible electrostatic interactions. However, the knowledge gap between molecular-level chemistry and material properties persists. Here, the authors present a framework combining theoretical and experimental insights, highlighting the interplay of molecular parameters in governing material properties.
- Seola Lee
- , Pierre J. Walker
- & Julia R. Greer
-
Article
| Open AccessPrinted polymer platform empowering machine-assisted chemical synthesis in stacked droplets
Existing platforms for machine assistant synthetic workflows compatible with multiple liquid phases lack the possibility of easy customization and throughput increasement. Here, the authors report a droplet-based chip that allows self-organization of various liquid phases into stacked layers for conducting chemical transformations.
- Yingxue Sun
- , Yuanyi Zhao
- & Wenqian Feng
-
Article
| Open AccessRevealing and reconstructing the 3D Li-ion transportation network for superionic poly(ethylene) oxide conductor
The sluggish ionic conductivity of polymer electrolytes has been a long-standing concern. Here, authors present a multiscale study of the lithium ion conduction network of poly(ethylene) oxide-based electrolytes and elucidate how aluminium-oxo molecular clusters improve the transport properties.
- Cheng-Dong Fang
- , Ying Huang
- & Jia-Jia Chen
-
Article
| Open AccessSequence-encoded bioactive protein-multiblock polymer conjugates via quantitative one-pot iterative living polymerization
Protein therapeutics are useful but instability limits the range of applications for which they are viable. Here, the authors report the development of a one-pot method for the preparation of protein-polymer conjugates with defined sequences.
- Ziying Li
- , Kaiyuan Song
- & Ruijiao Dong
-
Article
| Open AccessHolographic direct sound printing
Within the field of additive manufacturing, direct sound printing is limited to a voxel-by-voxel printing. Here, the authors overcome this limitation with a holographic direct sound printing technique in which the information printed part is stored in an acoustic hologram and the printing material polymerizes instantly therefore improving the printing speed and allowing to print multimaterial objects even behind optically non-transparent media.
- Mahdi Derayatifar
- , Mohsen Habibi
- & Muthukumaran Packirisamy
-
Article
| Open AccessSimultaneous and in situ syntheses of an enantiomeric pair of homochiral polymers as their perfect stereocomplex in a crystal
Stereocomplexation is a powerful strategy for improving polymer properties but inefficient complexation remains a major challenge in stereocomplex formation. Here, the authors circumvent the difficulties of conventional stereocomplexation of preformed polymers and, synthesize two enantiopure polymers of opposite chirality simultaneously and in situ as their stereocomplex via topochemical polymerization.
- Ravichandran Khazeber
- , Sourav Pathak
- & Kana M. Sureshan
-
Article
| Open AccessHierarchical single-crystal-to-single-crystal transformations of a monomer to a 1D-polymer and then to a 2D-polymer
The design and synthesis of two-dimensional polymers (2D-Ps) via molecular preorganization presents an intriguing yet challenging frontier in research. Here, the authors report the single-crystal-to-single-crystal synthesis of a 2D-P via thermally induced topochemical azide-alkyne cycloaddition reaction.
- Haripriya Balan
- & Kana M. Sureshan
-
Article
| Open AccessStabilizing hexagonally close-packed phase in single-component block copolymers through rational symmetry breaking
Although hexagonally close packed structures are predicted, obtaining direct experimental evidence has been a challenge. Here, the authors report direct evidence for this phaseby regulation of phase behaviour by deliberate breaking of molecular symmetry.
- Zhanhui Gan
- , Zhuoqi Xu
- & Xue-Hui Dong
-
Article
| Open AccessBridge-rich and loop-less hydrogel networks through suppressed micellization of multiblock polyelectrolytes
In the formation of physical hydrogels from triblock copolymers, formation of polymer loops can result in topological defects. Here, the authors report the development of hydrogels from oppositely charged copolymers which assembled to form branched and bridge-rich networks.
- Jihoon Han
- , Saeed Najafi
- & Youn Soo Kim
-
Article
| Open AccessQuantifying the conductivity of a single polyene chain by lifting with an STM tip
Polyene is a segment of polyacetylene, a conductive polymer. Here, the authors measured the conductance of single molecular chain of trans-polyene and found a high conductivity and low decay constant, attributed to the alignment of the energy levels.
- Sifan You
- , Cuiju Yu
- & Lifeng Chi
-
Article
| Open AccessElectrochemical on-surface synthesis of a strong electron-donating graphene nanoribbon catalyst
On-surface synthesis of edge-functionalized graphene nanoribbons (GNRs) has attracted much attention but producing such GNRs on a large scale under ultra-high vacuum on thermally activated metal surfaces remains challenging. Here the authors develop an on-surface electrochemical technique that utilizes redox reactions of asymmetric precursors at an electric double layer where a strong electric field is confined to the liquid-solid interface.
- Hiroshi Sakaguchi
- , Takahiro Kojima
- & Kazuhiro Fukami
-
Article
| Open AccessDirect synthesis of partially ethoxylated branched polyethylenimine from ethanolamine
The industrial process for the synthesis of branched polyethylenimine (PEI) and polyethylenimine ethoxylated (PEIE) uses highly toxic and mutagenic chemicals. Here the authors report a method to make a branched and partially ethoxylated polyethyleneimine derivative directly from ethanolamine using a pincer complex of Earth-abundant manganese, and producing water as the only byproduct.
- Claire N. Brodie
- , Alister S. Goodfellow
- & Amit Kumar
-
Article
| Open AccessAerobic mechanochemical reversible-deactivation radical polymerization
Polymer materials suffer mechano-oxidative deterioration or degradation in the presence of molecular oxygen and mechanical forces. Here the authors demonstrate a synthetic approach in which molecular oxygen and mechanical energy synergistically initiate polymerization and affords robustness in polymeric materials.
- Haoyang Feng
- , Zhe Chen
- & Zhenhua Wang
-
Article
| Open AccessHow molecular architecture defines quantum yields
Chemical topology is important in bond-forming reactions, but understanding the relationship between them is challenging. Here, the authors report a study considering photo-induced cyclisations for a series of monodisperse macromolecules with defined spacers and apply their findings to 3D printing.
- Fred Pashley-Johnson
- , Rangika Munaweera
- & Christopher Barner-Kowollik
-
Article
| Open AccessA strategy for tough and fatigue-resistant hydrogels via loose cross-linking and dense dehydration-induced entanglements
For use in a range of applications, hydrogel properties are vital, but it can be challenging to balance different aspects. Here, the authors report the use of a dehydration strategy to prepare hydrogels with desirable fracture toughness, fatigue threshold, and modulus.
- Danming Zhong
- , Zhicheng Wang
- & Wei Yang
-
Article
| Open AccessChemically tailored block copolymers for highly reliable sub-10-nm patterns by directed self-assembly
Printing features with half pitch size of less than 10 nm by block copolymer lithography is challenging. Here, the authors employ directed self-assembly on tailored block co-polymers and achieved line pattern of 15.1 nm which corresponds to 7.6 nm half pitch size.
- Shinsuke Maekawa
- , Takehiro Seshimo
- & Teruaki Hayakawa
-
Article
| Open AccessRecycling polyolefin plastic waste at short contact times via rapid joule heating
This manuscript demonstrates a single-step electrified approach using rapid joule heating over an H-ZSM-5 catalyst for effective deconstruction of polyolefin plastic waste into light olefins (C2–C4) in milliseconds.
- Esun Selvam
- , Kewei Yu
- & Dionisios G. Vlachos
-
Article
| Open AccessUnveiling the mechanism of triphos-Ru catalysed C–O bond disconnections in polymers
Ruthenium complexes with facially coordinating tripodal phosphine ligands are privileged catalysts for a broad range of (de-)hydrogenation-based transformations but the mechanism remains poorly understood. Here the authors present a detailed investigation on the triphos-Ru catalysed C–O bond scission on a molecular level.
- Alexander Ahrens
- , Gabriel Martins Ferreira Batista
- & Troels Skrydstrup
-
Article
| Open AccessStructural evolution during inverse vulcanization
Inverse vulcanization exploits elemental sulfur to synthesize versatile polysulfides but the mechanism of inverse vulcanization remains elusive. Herein, the authors use inverse vulcanization curves to describe the three-stage structural evolution during the inverse vulcanization process.
- Botuo Zheng
- , Liling Zhong
- & Huagui Zhang
-
Article
| Open AccessHighly efficient dual photoredox/copper catalyzed atom transfer radical polymerization achieved through mechanism-driven photocatalyst design
Atom transfer radical polymerization with dual photoredox/copper catalysis often requires high photocatalyst loadings. Herein the authors report a photocatalyst that functions at the sub-ppm level for controlled radical polymerizations, focusing on a design strategy aimed at photocatalyst regeneration.
- Woojin Jeon
- , Yonghwan Kwon
- & Min Sang Kwon
-
Article
| Open AccessControlled switching thiocarbonylthio end-groups enables interconvertible radical and cationic single-unit monomer insertions and RAFT polymerizations
To emulate the ordered arrangement of radically and cationically polymerizable monomers using single-unit monomer insertion (SUMI) remians challenging. Here the authors demonstrate sequence-defined vinyl polymers via SUMI by manipulating thiocarbonylthio end-groups.
- Wei He
- , Wei Tao
- & Ronghua Yang
-
Article
| Open AccessRapidly damping hydrogels engineered through molecular friction
Hydrogels capable of swift mechanical energy dissipation are desirable for various uses, but traditional energy absorption in hydrogels typically relies on viscoelastic mechanisms and often suffers from slow recovery. Here, the authors report a hydrogel design harnessing molecular friction to achieve efficient energy dissipation and rapid recovery.
- Zhengyu Xu
- , Jiajun Lu
- & Wei Wang
-
Article
| Open AccessClosed-loop recycling of tough epoxy supramolecular thermosets constructed with hyperbranched topological structure
The covalent crosslinked structure of epoxy thermosets difficult their reprocessability and recyclability. Here, the authors report a method for developing closed loop recycling of strong and tough epoxy supramolecular thermosets constructed with hyperbranched topological structure in an energy-saving and easy-to-conduct way.
- Junheng Zhang
- , Can Jiang
- & Daohong Zhang
-
Article
| Open AccessInternal water circulation mediated synergistic co-hydrolysis of PET/cotton textile blends in gamma-valerolactone
Recycling strategies for mixed plastics and textile blends currently aim for recycling only one of the components. Here the authors demonstrate a water coupling strategy to co-hydrolyze polyester/cotton textile blends into polymer monomers and platform chemicals.
- Shun Zhang
- , Wenhao Xu
- & Yu-Zhong Wang
-
Article
| Open AccessHeat-activated growth of metastable and length-defined DNA fibers expands traditional polymer assembly
The combination of dynamic, energy driven folding and growth with structural stiffness and length control is difficult to achieve in synthetic polymer self-assembly. Here the authors show that highly charged, monodisperse DNA oligomers assemble via seeded growth into length-controlled supramolecular fibers during heating.
- Michael D. Dore
- , Muhammad Ghufran Rafique
- & Hanadi F. Sleiman
-
Article
| Open AccessConcentration-induced spontaneous polymerization of protic ionic liquids for efficient in situ adhesion
Adhesives require a balance between cohesion and interfacial adhesion, which can be challenging to achieve. Here the authors report the polymerisation of a protic ionic liquid-based monomer, with internal and external non-covalent interactions contributing to both cohesion and adhesion.
- Jun Zhang
- , Xuan Zhou
- & Shiguo Zhang
-
Article
| Open AccessStretchable phosphorescent polymers by multiphase engineering
Stretchable phosphorescent materials have potential in applications such as wearable electronics, but achieving a suitable balance of emission and stretchability is challenging. Here, the authors report the use of microphase separation to show stretchability with emission lifetimes maintained.
- Nan Gan
- , Xin Zou
- & Wei Huang
-
Article
| Open AccessNested non-covalent interactions expand the functions of supramolecular polymer networks
Supramolecular polymer networks have unique and useful properties due to the reversible nature of their cross-links. Here, the authors show that when two distinct supramolecular interaction classes exist within a single cross-link, new functions can result.
- David J. Lundberg
- , Christopher M. Brown
- & Jeremiah A. Johnson
-
Article
| Open AccessConverting inorganic sulfur into degradable thermoplastics and adhesives by copolymerization with cyclic disulfides
The inherent instability of poly(sulfur) renders the conversion of elementary sulfur into sulfur-rich polymers challenging which limits the use of this industrial by-product. Here, the authors demonstrate that inorganic sulfur can be utilized by copolymerizing with cyclic disulfides, producing high-performance thermoplastic elastomers with self-healing ability and degradability.
- Yuanxin Deng
- , Zhengtie Huang
- & Da-Hui Qu
-
Article
| Open AccessCellulose nanofiber-mediated manifold dynamic synergy enabling adhesive and photo-detachable hydrogel for self-powered E-skin
Certain devices require rapid adhesion and detachment, but achieving both can be challenging. Here, the authors report the development of a supramolecular hydrogel with reversible tough adhesion and triggered photodetachment.
- Lei Zhang
- , Lu Chen
- & Chaoji Chen
-
Article
| Open AccessNoncovalent synthesis of homo and hetero-architectures of supramolecular polymers via secondary nucleation
Synthesis of supramolecular polymers with controlled architecture is desirable but challenging. Here, the authors use a secondary nucleation event to prepare a range of supramolecular polymer architectures.
- Srinu Kotha
- , Rahul Sahu
- & Kotagiri Venkata Rao
-
Article
| Open AccessProgramming viscoelastic properties in a complexation gel composite by utilizing entropy-driven topologically frustrated dynamical state
Tuning the physical interactions and structures to govern the viscoelastic properties in hydrogels without altering the chemistry is challenging. Here the authors design a complexation gel composite and utilize the physical principle of topologically frustrated dynamical state to tune the correlated structures between the guest polycation chains and negatively charged host gels.
- Gui Kang Wang
- , Yi Ming Yang
- & Di Jia
-
Article
| Open AccessMultiple hydrogen-bonding induced nonconventional red fluorescence emission in hydrogels
The development of fluorescent polymer hydrogels without the use of extended pi-conjugation is challenging. Here, the authors report the use of clustering-trigger emission to give red fluorescence on boiling polymer hydrogels, with tuneable emission properties.
- Jiayu Wu
- , Yuhuan Wang
- & Feng Zhou