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Tracking nuclear motion in single-molecule magnets using femtosecond X-ray absorption spectroscopy
The authors use femtosecond K-edge X-ray absorption spectroscopy to follow nuclear motion in a manganese-based tri-nuclear single-molecule magnet, and resolve changes in bond lengths on the order of hundreds of ångströms and on sub-picosecond timescales.
- Kyle Barlow
- , Ryan Phelps
- & J. Olof Johansson
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Mechanically controlled multifaceted dynamic transformations in twisted organic crystal waveguides
Crystals with mechanical responses are of interest, but often only one or two dynamic motions can be achieved with one crystal. Here, the authors report a combination of dynamic movements in naturally twisted optical waveguiding microcrystals.
- Mehdi Rohullah
- , Vuppu Vinay Pradeep
- & Rajadurai Chandrasekar
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Vitrification-enabled enhancement of proton conductivity in hydrogen-bonded organic frameworks
Proton conduction is one of the interesting applications of hydrogen-bonded organic frameworks. Here, the authors report hydrogen-bonded organic framework that can be transformed into glassy state, effectively mitigating grain boundary effects, and significantly enhancing proton conduction performance.
- Feng-Fan Yang
- , Xiao-Lu Wang
- & Linfeng Liang
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Sustainable 3D printing by reversible salting-out effects with aqueous salt solutions
Here, the authors show a facile and sustainable 3D printing by utilizing a reversible salting-out effect on poly(N-isopropylacrylamide) (PNIPAM) solutions. Aqueous salt solutions lower the phase transition temperature of PNIPAM solutions below 10 °C and instantly solidify the PNIPAM solutions upon contact.
- Donghwan Ji
- , Joseph Liu
- & Jinhye Bae
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Gas adsorption and framework flexibility of CALF-20 explored via experiments and simulations
CALF-20 is a water stable structure capable of selectively separating CO2 from flue gas. Here authors use a close feedback loop between theory and experiments to understand CO2/water adsorption and framework flexibility of CALF-20.
- Rama Oktavian
- , Ruben Goeminne
- & Peyman Z. Moghadam
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Bulk transparent supramolecular glass enabled by host–guest molecular recognition
Strategies to produce supramolecular glass and the study of its intrinsic structure and mechanical properties remains largely unexplored. Here, the authors prepare a supramolecular glass via the host–guest recognition between methyl-β-cyclodextrin and para-hydroxybenzoic acid with recyclability, compatibility, and thermal processability.
- Changyong Cai
- , Shuanggen Wu
- & Shengyi Dong
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Finely manipulating room temperature phosphorescence by dynamic lanthanide coordination toward multi-level information security
Room temperature phosphorescent materials have many desirable properties, but fine control of these can be challenging. Here, the authors report a strategy for this control by dynamic lanthanide coordination in combination with organic phosphors.
- Longqiang Li
- , Jiayin Zhou
- & Tao Chen
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Constructing ordered and tunable extrinsic porosity in covalent organic frameworks via water-mediated soft-template strategy
The synthesis of covalent organic frameworks (COFs) by a soft-template methodology is challenging. Here, the authors attach the soft templates to the COFs backbone via ion bonds, avoiding crystallization incompatibilities and allowing subsequent removal of the template by ion exchange for enhanced U(VI)/Th(IV) adsorption performance.
- Ningning He
- , Yingdi Zou
- & Lijian Ma
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Converting 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
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Cellulose 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
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Efficient recovery and recycling/upcycling of precious metals using hydrazide-functionalized star-shaped polymers
Despite the use of amine-functionalized polymers as metal adsorbents, they are generally ineffective at recovering precious metals. Here the authors prepare a star-shaped, hydrazide-functionalized polymer as a recoverable standalone adsorbent with high precious metal adsorption capability/selectivity and practical feasibility.
- Seung Su Shin
- , Youngkyun Jung
- & Jung-Hyun Lee
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Multi-color dual wavelength vat photopolymerization 3D printing via spatially controlled acidity
Dual wavelength vat photopolymerization has emerged as a powerful approach to create multimaterial objects but require changing the resin during the printing process. Here, the authors develop a method of dual-wavelength 3D printing that can directly access multicolor parts without requiring changing of resin feedstocks or introduction of new materials during the printing process.
- Kyle C. H. Chin
- , Grant Ovsepyan
- & Andrew J. Boydston
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Giant dielectric tunability in ferroelectric ceramics with ultralow loss by ion substitution design
The authors realize composite optimization in dielectric tunable materials by simultaneously achieving low electric field, large tunability, and low loss through ion substitution design in ferroelectric tunable materials.
- Ruitao Li
- , Diming Xu
- & Di Zhou
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Coordination cages integrated into swelling poly(ionic liquid)s for guest encapsulation and separation
The efficient encapsulation of guests by coordination cages in the solid state is prevented by their flexibility, dynamicity, and metal-ligand bond reversibility. Here, the authors report coordination cages integrated into poly(ionic liquid)s to control swelling and mechanical properties of the gels and develop efficient and regenerable supramolecular separation materials.
- Xiang Zhang
- , Dawei Zhang
- & Mingyuan He
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Color morphing surfaces with effective chemical shielding
Photochromic materials suffer from degradation when exposed to harsh chemical environments, but this can be overcome by providing chemical shielding via superomniphobicity. Here, the authors show the design rationale and careful materials selection for fabrication of color morphing surfaces that can simultaneously display excellent chemical resistance.
- Adil Majeed Rather
- , Sravanthi Vallabhuneni
- & Arun Kumar Kota
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Delayed room temperature phosphorescence enabled by phosphines
Room-temperature phosphorescence usually occurs immediately after the removal of excitation. Here the authors achieve combined instant and delayed phosphorescence through introduction of phosphines into carbazole emitters.
- Guang Lu
- , Jing Tan
- & Hui Xu
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Boosting organic phosphorescence in adaptive host-guest materials by hyperconjugation
Room-temperature phosphorescence is usually inefficient in purely organic material. Here, the authors achieve near-unity phosphorescence efficiency with color tunability in adaptive host-guest materials through use of hyperconjugation.
- Huili Ma
- , Lishun Fu
- & Wei Huang
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Isostructural doping for organic persistent mechanoluminescence
Organic mechanoluminescent materials have potential in a range of applications, but it can be challenging to achieve long-lived emission. Here, the authors report isostructural doping as a strategy to achieve multicolour and high efficiency organic mechanoluminescence, applied in stress sensing.
- Zongliang Xie
- , Yufeng Xue
- & Bin Liu
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In situ enzymatic control of colloidal phoresis and catalysis through hydrolysis of ATP
The design of synthetic systems that can sense chemical gradients and respond with directional motility and chemical activity is of interest. Here, the authors realize and control such behaviors in a synthetic system by tailoring multivalent interactions of adenosine nucleotides with catalytic microbeads.
- Ekta Shandilya
- , Bhargav Rallabandi
- & Subhabrata Maiti
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Self-condensation-assisted chemical vapour deposition growth of atomically two-dimensional MOF single-crystals
2D MOFs have a variety of applications, including molecular separation and atomically thin electronics. Here authors demonstrate the preparation of monolayer and few-layer MOF single-crystals using a self-condensation-assisted CVD method.
- Lingxin Luo
- , Lingxiang Hou
- & Jian Zheng
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Highly efficient in crystallo energy transduction of light to work
Crystals are known to have a range of responses to light, but multiple responses in the same material are rare. Here, the authors report different mechanical effects in response to light across three polymorphs as a result of a dimerization reaction.
- Jiawei Lin
- , Jianmin Zhou
- & Junbo Gong
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Visible-light-excited robust room-temperature phosphorescence of dimeric single-component luminophores in the amorphous state
Organic room temperature phosphorescence (RTP) is limited to rigid environments. Here, the authors report a single-component system with robust persistent RTP emissions in various aggregation states, such as crystalline, fine powder, and amorphous.
- Danman Guo
- , Wen Wang
- & Zhiyong Yang
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Staggered structural dynamic-mediated selective adsorption of H2O/D2O on flexible graphene oxide nanosheets
Graphene oxide is a promising material for molecular separation technologies. Here, the authors propose a realistic staggered stacking structure that plays a crucial role in H/D recognition in water adsorption, as well as high mobilities of water.
- Ryusuke Futamura
- , Taku Iiyama
- & Katsumi Kaneko
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Timescale correlation of shallow trap states increases electrochemiluminescence efficiency in carbon nitrides
Differences in timescales of electron transfer reactions limit the efficiency of electrochemiluminescence. Here, the authors coordinate the timescales using shallow trap states in carbon nitride to achieve high efficiencies applied in nitrite sensing.
- Yanfeng Fang
- , Hong Yang
- & Yuanjian Zhang
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Control of polymers’ amorphous-crystalline transition enables miniaturization and multifunctional integration for hydrogel bioelectronics
Soft elastic materials could be useful in the fabrication of brain-machine interfaces, but achieving the desirable material properties can be challenging. Here, the authors report control of the amorphous-crystalline transition of polymers to alter hydrogel properties and monitor mouse behaviour.
- Sizhe Huang
- , Xinyue Liu
- & Siyuan Rao
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Confining single Er3+ ions in sub-3 nm NaYF4 nanoparticles to induce slow relaxation of the magnetisation
Many of the most industrially important magnets require the addition of rare-earths to improve their coercivity and magnetic performance. Here, the authors place a single paramagnetic rare-earth ion, Er3+, in a diamagnetic nanoparticle, and study the slow relaxation of the resulting nanoparticles, providing vital information for the further development of rare-earth magnetic materials.
- Diogo A. Gálico
- , Emille M. Rodrigues
- & Muralee Murugesu
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Establishing superfine nanofibrils for robust polyelectrolyte artificial spider silk and powerful artificial muscles
Spider silk has desirable properties, but these are hard to replicate with artificial materials. Here, the authors report a polyelectrolyte artificial spider silk, with control over dissociation of the polymer chains by introduction of ions, and thermally driven supercontraction.
- Wenqian He
- , Meilin Wang
- & Zunfeng Liu
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Sweat permeable and ultrahigh strength 3D PVDF piezoelectric nanoyarn fabric strain sensor
Electronic packaging causes piezoelectric sensors to be airtight, resulting in poor wearing comfort. To address this issue, the authors develop a 3D all-fiber piezoelectric sensor with sweat permeable using the advanced 3D textile technology.
- Wei Fan
- , Ruixin Lei
- & Shengbo Ge
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Highly defective ultra-small tetravalent MOF nanocrystals
Crystalline materials’ properties are highly dependent on their size. Here authors report a general synthesis of ultrasmall (4–6 nm) and highly defective Zr/Hf-Metal Organic Frameworks nanoparticles that present enhanced peptide hydrolysis performance.
- Shan Dai
- , Charlotte Simms
- & Christian Serre
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An organic proton cage that is ultra-resistant to hydroxide-promoted degradation
Organic cations are typically unstable under low-humidity, alkaline conditions. Here, the authors report an organic cation featuring a proton protected within a cage that can withstand vapor-phase alkaline conditions.
- Chase L. Radford
- , Torben Saatkamp
- & Steven Holdcroft
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Redefined ion association constants have consequences for calcium phosphate nucleation and biomineralization
While clusters in calcium orthophosphate nucleation have long been known, their speciation and mechanistic pathways to hydroxyapatite remain debated. Here the authors report a revision of ion association in the calcium phosphate system and explore the consequences thereof on the early stages of phase separation.
- David P. McDonogh
- , Julian D. Gale
- & Denis Gebauer
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Intelligent perceptual textiles based on ionic-conductive and strong silk fibers
Perception plays a pivotal role in advancing future intelligent textiles. Here, the authors develop smart perceptual textiles using natural-derived ionic-conductive silk fibers. These textiles can electrically detect external hazards and precisely pinpointing human touch, making them suitable for smart protective clothing and soft human-machine interfaces.
- Haojie Lu
- , Yong Zhang
- & Yingying Zhang
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Rapid room-temperature phosphorescence chiral recognition of natural amino acids
Chiral recognition of amino acids with luminescence, despite its advantages, is usually slow and lacks generality. Here, the authors demonstrate that L-phenylalanine derived benzamide can manifest the structural difference between the natural, left-handed amino acid and its right-handed counterpart via the difference in room-temperature phosphorescence, irrespective of the specific chemical structure.
- Xiaoyu Chen
- , Renlong Zhu
- & Guoqing Zhang
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Orbital hybridization of donor and acceptor to enhance the conductivity of mixed-stack complexes
Mixed-stack complexes consisting of alternating donors and acceptors typically show low electrical conductivity. Here, the authors improved the conductivity by hybridizing the frontier orbitals of the donor and acceptor at the neutral–ionic boundary.
- Tomoko Fujino
- , Ryohei Kameyama
- & Hatsumi Mori
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Bioadhesive interface for marine sensors on diverse soft fragile species
It is useful to be able to equip marine animals with sensors, but it can be challenging to attach these to soft marine organisms. Here, the authors use an adhesive hydrogel to achieve rapid attachment of sensors to marine life including jellyfish, squid and lobster.
- Camilo Duque Londono
- , Seth F. Cones
- & Xuanhe Zhao
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Unconventional mechanical and thermal behaviours of MOF CALF-20
CALF-20 MOF is considered a benchmark sorbent for industrial scale CO2 capture. Here authors use machine-learning potential simulations to show that CALF-20 exhibits anomalous structural responses to temperature and strain stimuli, with potential applications in mechanical/thermal sensing.
- Dong Fan
- , Supriyo Naskar
- & Guillaume Maurin
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3D printable strong and tough composite organo-hydrogels inspired by natural hierarchical composite design principles
The preparation of composite hydrogels can allow for mechanical properties to be enhanced, and hierarchical structures can be effective. Here, the authors report improved mechanical properties by the addition of ceramic platelets to an organohydrogel in direct ink writing.
- Quyang Liu
- , Xinyu Dong
- & Wei Zhai
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Double-walled Al-based MOF with large microporous specific surface area for trace benzene adsorption
Trace benzene poses a risk to the health and safety of humans, resulting in a challenging task. Here authors synthesise double-walled Al-based MOF ZJU-520(Al) with trace benzene adsorption (5.98 mmol g–1) and excellent benzene/cyclohexane separation ability.
- Laigang Hu
- , Wenhao Wu
- & Kun Yang
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A facile one step route that introduces functionality to polymer powders for laser sintering
Polyamide-12 is the main polymer employed to produce 3D objects by laser sintering constraining the functionality of the items produced. Here, the authors report a clean and scalable approach for the functionalization of polyamide-12 particles, yielding materials that can be printed using commercial apparatus.
- Eduards Krumins
- , Liam A. Crawford
- & Steven M. Howdle
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Precision ion separation via self-assembled channels
Selective nanofiltration membranes with accurate molecular sieving offer a solution to recover rare metals and other valuable elements from brines but this demands the development of membranes with precise sub-nanometer pores surpassing those available today. Here, the authors report a scalable approach for membrane fabrication in which functionalized macrocycles are seamlessly oriented via supramolecular interactions during the interfacial polycondensation on a polyacrylonitrile support layer.
- Shanshan Hong
- , Maria Di Vincenzo
- & Suzana P. Nunes
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Beyond nothingness in the formation and functional relevance of voids in polymer films
Voids are known to impact the properties of materials, but the nanovoids also present are less well understood than macroscopic voids. Here, the authors utilise 3D imaging and graph theory to study nanovoid formation and impact on material properties.
- Falon C. Kalutantirige
- , Jinlong He
- & Qian Chen
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Highly robust supramolecular polymer networks crosslinked by a tiny amount of metallacycles
Supramolecular polymeric materials have exhibited attractive features such as self-healing, reversibility and stimuli-responsiveness but because of the weak bonding nature of most noncovalent interactions, constructing supramolecular polymer materials with high robustness remains challenging. Here, the authors describe the construction of highly robust stimuli-responsive supramolecular polymer networks by using only a tiny amount of metallacycles as the supramolecular crosslinkers.
- Lang He
- , Yu Jiang
- & Shijun Li
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Enabling robust blue circularly polarized organic afterglow through self-confining isolated chiral chromophore
The preparation of systems that give blue circularly polarised organic afterglow is desirable but challenging. Here, the authors confine a chiral chromophore within a polymer matrix to limit non-radiative transitions and give blue circularly polarised organic afterglow.
- Mingjian Zeng
- , Weiguang Wang
- & Wei Huang
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Vapor-induced phase-separation-enabled versatile direct ink writing
The extrusion-based three-dimensional printing of polymers, metals, and composites requires elevated temperatures and may lead to diverse undesirable defects on printed parts. Here, the authors develop a vapor-induced phase separation printing technique to construct polymeric, metallic, and composite parts by using a polymer as a binder.
- Marc Sole-Gras
- , Bing Ren
- & Yong Huang
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Fine-tuning the pore environment of ultramicroporous three-dimensional covalent organic frameworks for efficient one-step ethylene purification
The construction of three-dimensional covalent organic frameworks for gas separation is challenging due to the similar physicochemical properties of the gas mixture. Here, the authors report functional three-dimensional covalent organic frameworks by fine-tunning the pore environment with pyridine units to achieve effective separation of ethane from ethylene.
- Yang Xie
- , Wenjing Wang
- & Cheng Wang
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| Open Access
Slow magnetic relaxation in a europium(II) complex
This study introduces a Eu(II) single molecule magnet that exhibits slow magnetic relaxation at low temperatures. These results highlight the importance of the lanthanide ion’s crystal field in unlocking the magnet-like properties of Eu(II).
- Dylan Errulat
- , Katie L. M. Harriman
- & Muralee Murugesu
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Tumor-activated in situ synthesis of single-atom catalysts for O2-independent photodynamic therapy based on water-splitting
The utility of single-atom catalysts (SACs) for photodynamic therapy (PDT) has been limited by tumor hypoxia and side effects on normal tissues. Here the authors address these issues by developing an approach of tumor microenvironment-activated in situ synthesis of SACs for tumor-specific water-based PDT.
- Yiyan Yin
- , Xiyang Ge
- & Na Na
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Artificial kagome lattices of Shockley surface states patterned by halogen hydrogen-bonded organic frameworks
By utilizing the templating effect of a halogen hydrogen-bonded organic framework, the authors show that the Shockley surface states of coinage metals can be patterned into artificial kagome lattices with high tunability.
- Ruoting Yin
- , Xiang Zhu
- & Bing Wang
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Long 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
Stretchable phosphorescent polymers by multiphase engineering