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Article
| Open AccessRedefined 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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Article
| Open AccessIn-situ low-temperature sulfur CVD on metal sulfides with SO2 to realize self-sustained adsorption of mercury
Efficient removal of gaseous mercury (Hg0) from industrial flue gas is commonly constrained by SO2. Here, authors propose an in-situ sulfur CVD method on metal sulfides that reverses the harmful effects of SO2, achieving self-sustained adsorption of Hg0 and breaking the capacity limitations.
- Qinyuan Hong
- , Haomiao Xu
- & Naiqiang Yan
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Article
| Open AccessLate-stage meta-C–H alkylation of pharmaceuticals to modulate biological properties and expedite molecular optimisation in a single step
Installation of small aliphatic motifs within pharmaceuticals provides a medicinally relevant tool in drug discovery programmes. Here, the authors report a late-stage meta-C–H alkylation method facilitating the biological properties modulation of therapeutic agents.
- Lucas Guillemard
- , Lutz Ackermann
- & Magnus J. Johansson
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Article
| Open AccessElectric-field-assisted proton coupling enhanced oxygen evolution reaction
Manganese complexes have long been utilized by nature to catalyze the oxygen evolution reaction (OER) but mirroring their efficiency in artificial electrochemical systems has proven difficult. This study centers on alpha-manganese dioxide (α-MnO2), which closely mimics natural MnIV-O-MnIII-HxO motifs, presenting a novel method for manipulating proton coupling within the OER process using an external electric field.
- Xuelei Pan
- , Mengyu Yan
- & Liqiang Mai
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Article
| Open AccessRapid evolutionary change in trait correlations of single proteins
Trait correlations impact evolvability as selection on one trait can influence others. Here, the authors examine trait correlation in two proteins, a fluorescent protein & an antibiotic resistance enzyme, observing rapid evolution of trait correlations through changes in the biophysical properties of these proteins.
- Pouria Dasmeh
- , Jia Zheng
- & Andreas Wagner
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Article
| Open AccessExtrinsic hydrophobicity-controlled silver nanoparticles as efficient and stable catalysts for CO2 electrolysis
A key factor for the electrochemical reduction of CO2 to CO is limiting the competing H2 evolution reaction. Here, authors use real-time synchrotron X-ray computed tomography to show that a silver nanoparticle-ligand catalyst structure improves water management, thereby maintaining CO production.
- Young-Jin Ko
- , Chulwan Lim
- & Hyung-Suk Oh
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Article
| Open AccessNoncovalent interaction with a spirobipyridine ligand enables efficient iridium-catalyzed C–H activation
Exploitation of noncovalent interactions has received much attention for the design of metal catalysts. However, because of the weak nature, CH-π interactions have been less utilized for the control of organic reactions. Here, the authors report that the CH-π interaction can be used to kinetically accelerate catalytic C-H activation of arenes.
- Yushu Jin
- , Boobalan Ramadoss
- & Laurean Ilies
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Article
| Open AccessRapid 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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Article
| Open AccessSelenium catalysis enables negative feedback organic oscillators
Multiple autocatalytic reactions producing thiols are known, but negative feedback loop motifs are unavailable for thiol chemistry. Here, the authors develop a negative feedback loop based on the selenocarbonates, in which thiols induce the release of aromatic selenols that catalyze the oxidation of thiols by organic peroxides.
- Xiuxiu Li
- , Polina Fomitskaya
- & Sergey N. Semenov
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Article
| Open AccessAn enzymatic continuous-flow reactor based on a pore-size matching nano- and isoporous block copolymer membrane
Continuous-flow biocatalysis with immobilized enzymes is a sustainable route for chemical synthesis, but inadequate biocatalytic efficiency caused by non-productive enzyme immobilization or enzyme-carrier mismatches presents a challenge for its application. Here, the authors report an approach for the fabrication of a high-performance enzymatic continuous-flow reactor via integrating scalable isoporous block copolymer membranes as carriers with an oriented one-step enzyme immobilization via a genetically fused material binding peptide.
- Zhenzhen Zhang
- , Liang Gao
- & Volker Abetz
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Article
| Open AccessIntelligent 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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Article
| Open AccessPhotocatalytic Z/E isomerization unlocking the stereodivergent construction of axially chiral alkene frameworks
The stereospecific Z/E isomerization of tetrasubstituted alkenes remains underdeveloped, thus lacking in a stereodivergent synthesis of axially chiral alkenes. Here, authors report the atroposelective synthesis of tetrasubstituted alkene analogues by asymmetric allylic substitution-isomerization, followed by the photocatalyzed Z/E isomerization.
- Jie Wang
- , Jun Gu
- & Ying He
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Article
| Open AccessNanoparticles as an antidote for poisoned gold single-atom catalysts in sustainable propylene epoxidation
The poisoning of single-atom catalysts hampers their performance. Here, the authors propose Au nanoparticles as an antidote for poisoned Au single-atom catalysts, with trace addition shown to reinforce and sustain propylene epoxidation.
- Qianhong Wang
- , Keng Sang
- & Xuezhi Duan
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Article
| Open AccessOrbital 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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Article
| Open AccessBioadhesive 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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Article
| Open AccessAssembly of short amphiphilic peptoids into nanohelices with controllable supramolecular chirality
Helical protein assemblies are an important biological structure, but are challenging to mimic with synthetic materials. Here, the authors report the use of peptoids to form nanohelix structures with controllable supramolecular chirality.
- Renyu Zheng
- , Mingfei Zhao
- & Chun-Long Chen
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Article
| Open AccessUnconventional 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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Article
| Open AccessOn the role of asymmetric molecular geometry in high-performance organic solar cells
The correlation between asymmetric molecular geometry of non-fullerene acceptors and their optoelectronic properties was unclear. Here, the authors found asymmetric ones exhibit increased open-circuit voltage compared to their symmetric counterparts due to reduced non-radiative charge recombination.
- Jinfeng Huang
- , Tianyi Chen
- & Lijian Zuo
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Article
| Open AccessHybridizing carbonate and ether at molecular scales for high-energy and high-safety lithium metal batteries
Here, authors report a linear functionalized solvent through molecular hybridization. Complementary ethers and carbonates are integrated into a single molecule, exhibiting properties suited for high-energy and high safety lithium metal batteries.
- Jiawei Chen
- , Daoming Zhang
- & Yongyao Xia
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Article
| Open AccessElectrocatalytic hydrogenation of acetonitrile to ethylamine in acid
Proton exchange membrane electrolyzers hold promise for ethylamine synthesis from acetonitrile, yet local acidity fosters proton reduction. Here, authors systematically screen metal catalysts, verifying their effectiveness in such electrolyzers.
- Chongyang Tang
- , Cong Wei
- & Xiangfeng Duan
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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 Access3D 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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Article
| Open AccessTopology selectivity of a conformationally flexible precursor through selenium doping
Research into the control of conformational arrangements is of great importance for achieving bespoke nanoarchitectures. Here, the authors achieve topology selectivity of a conformationally flexible precursor by Se doping.
- Liangliang Cai
- , Tianhao Gao
- & Andrew T. S. Wee
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Article
| Open AccessAlkyne-tagged SERS nanoprobe for understanding Cu+ and Cu2+ conversion in cuproptosis processes
Simultaneously quantifying mitochondrial Cu+ and Cu2+ levels is vital for understanding the molecular mechanism of mitochondria-related biological events. Here the authors report an alkynyl-labeled SERS probe to simultaneously monitor free Cu+ and Cu2+ in mitochondria, and unveil their roles during ischemia and cuproptosis processes.
- Sihan Zhang
- , Yuxiao Mei
- & Yang Tian
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Article
| Open AccessDouble-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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Article
| Open AccessEmbedding biocatalysts in a redox polymer enhances the performance of dye-sensitized photocathodes in bias-free photoelectrochemical water splitting
A robust and efficient dye-sensitized NiO bio-hybrid photocathode based on a redox polymer and [FeFe]- hydrogenase has been developed to couple with a BiVO4 photoanode for water splitting without applied bias.
- Fangwen Cheng
- , Olha Pavliuk
- & Haining Tian
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Article
| Open AccessStress-induced ordering evolution of 1D segmented heteronanostructures and their chemical post-transformations
The formation mechanisms for periodic heterostructures are still poorly understood. Here, the authors propose a versatile approach to synthesize one-dimensional segmented heterostructures and reveal a stress-induced ordering mechanism through phase-field simulations.
- Qing-Xia Chen
- , Yu-Yang Lu
- & Shu-Hong Yu
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Article
| Open AccessEnhancing photocatalytic H2O2 production with Au co-catalysts through electronic structure modification
Photocatalytic H2O2 production using Au is hindered by its inherently weak O2 adsorption. Herein, the authors modify the electronic structure of Au with MoSx to form electron deficient Au sites to promote O2 adsorption and H2O2 production.
- Xidong Zhang
- , Duoduo Gao
- & Huogen Yu
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Article
| Open AccessQuantum phase synchronization via exciton-vibrational energy dissipation sustains long-lived coherence in photosynthetic antennas
Photosynthesis in biological systems occurs in a noisy environment that reduces the lifetime of coherences in the excitation energy transfer. Here the author demonstrate that long-lasting coherences are protected by quantum phase synchronization, realized in dimers by exciton-vibrational coupling where energy dissipation occurs predominantly in resonant anti-symmetric collective modes.
- Ruidan Zhu
- , Wenjun Li
- & Yuxiang Weng
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Article
| Open AccessFrustrated Lewis pair catalyst realizes efficient green diesel production
The commercial production of green diesel suffers from the requirement for continuous sulfur replenishment to maintain catalytic activity. Here, the authors report a sulfur-free catalytic system that can efficiently produce green diesel from various feedstocks over long periods of operation.
- De-Chang Li
- , Zhengyi Pan
- & Guang-Hui Wang
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Article
| Open AccessSolvent-free selective hydrogenation of nitroaromatics to azoxy compounds over Co single atoms decorated on Nb2O5 nanomeshes
Single atom catalysts can endow exceptional activity and selectively. Here, the authors report a single atom Co catalyst and reveal the importance of geometric and electronic properties for synthesizing azoxy compounds under solvent-free conditions.
- Zhijun Li
- , Xiaowen Lu
- & Yu Wang
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Article
| Open AccessA 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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Article
| Open AccessControlled condensation by liquid contact-induced adaptations of molecular conformations in self-assembled monolayers
Surface condensation is predetermined and is typically adjusted by chemical or topographical surface modification. Here, the authors report on a strategy to control the surface condensation behavior by adjusting molecular conformations in self-assembled monolayers.
- Guoying Bai
- , Haiyan Zhang
- & Yufeng Liu
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Article
| Open AccessSpiral packing and chiral selectivity in model membranes probed by phase-resolved sum-frequency generation microscopy
The properties of lipid membranes are intimately controlled by their complex heterogeneous structure. Here, the authors use phase-resolved sum-frequency generation microscopy to fully determine the hierarchical lipid packing from the molecular to the mesoscopic scale.
- Alexander P. Fellows
- , Ben John
- & Martin Thämer
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Article
| Open AccessPrecision 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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Article
| Open AccessTwo-dimensional lead halide perovskite lateral homojunctions enabled by phase pinning
Hong et al. report 2D perovskite lateral homojunction consists of ordered and disordered phases, achieved by organic cation doping induced phase pinning, built upon which they develop tuneable optical properties under external stimuli and directional exciton diffusion in the homojunctions.
- Huilong Hong
- , Songhao Guo
- & Yongping Fu
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Article
| Open AccessBeyond 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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Article
| Open AccessOrganocatalytic desymmetrization provides access to planar chiral [2.2]paracyclophanes
Planar chiral [2.2]paracyclophanes have a wide range of applications in asymmetric synthesis and materials science. However, they are accessed via time-consuming chiral separations or kinetic resolution approaches. Here, the authors report a simple, metal-free protocol for organocatalytic desymmetrization of prochiral diformyl[2.2]paracyclophanes.
- Vojtěch Dočekal
- , Filip Koucký
- & Jan Veselý
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Article
| Open AccessThermally stable Ni foam-supported inverse CeAlOx/Ni ensemble as an active structured catalyst for CO2 hydrogenation to methane
An inverse CeAlOx/Ni/Ni-foam structured catalyst with high thermal stability and water resistance is shown to be effective at CO2 methanation across a wide temperature range because of efficient heat/mass transport.
- Xin Tang
- , Chuqiao Song
- & Lili Lin
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Article
| Open AccessReverse water gas-shift reaction product driven dynamic activation of molybdenum nitride catalyst surface
Catalyst activation commonly occurs during reactions. This study demonstrates that the surface’s active structure in nitride catalysts during the reverse water gas-shift reaction varies with the partial pressure of reaction products, resulting in enhanced catalytic activity through positive feedback between catalytic activity and the evolution of MoNx’s active structure.
- Hui Xin
- , Rongtan Li
- & Xinhe Bao
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Article
| Open AccessLow-nuclearity CuZn ensembles on ZnZrOx catalyze methanol synthesis from CO2
The ideal metal selection and atomic-level arrangement for catalysts in CO2 hydrogenation are still uncertain. Here, copper is identified as the most effective promoter for enhancing ZnZrOx catalysts when precisely structured into CuZn ensembles, offering new insights for designing superior catalysts for CO2-based methanol synthesis.
- Thaylan Pinheiro Araújo
- , Georgios Giannakakis
- & Javier Pérez-Ramírez
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Article
| Open AccessElectrochemically coupled CH4 and CO2 consumption driven by microbial processes
The microbial valorisation of greenhouse gases could offer promising approaches climate change mitigation. Here, authors demonstrate the coupling of methane oxidation and carbon dioxide reduction by microbial consortia, facilitated by the redox cycling of iron minerals.
- Yue Zheng
- , Huan Wang
- & Feng Zhao
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Article
| Open AccessCarbon dioxide capture and functionalization by bis(N-heterocyclic carbene)-borylene complexes
Bis(N-heterocyclic carbene)-borylene complexes are capable of capturing and functionalizing CO2, but stable single-site-boron-carbon dioxide adducts are rarely reported. Here, the authors report the synthesis of a stable borylene-CO2 complex as well as the functionalization of the captured CO2.
- Jun Fan
- , An-Ping Koh
- & Cheuk-Wai So
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Article
| Open AccessHighly 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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Article
| Open AccessSurface oxidation/spin state determines oxygen evolution reaction activity of cobalt-based catalysts in acidic environment
Co-based catalysts are promising candidates for oxygen evolution reaction catalysis in an acidic environment, but the structure-activity relationship is unclear. Here, the authors discover that their acidic water oxidation activity is determined by the surface oxidation/spin state.
- Jinzhen Huang
- , Camelia Nicoleta Borca
- & Emiliana Fabbri
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Article
| Open AccessA 2D chiral microcavity based on apparent circular dichroism
Here the authors induce asymmetric transmission in planar Fabry–Pérot microcavities by embedding organic thin films exhibiting apparent circular dichroism (ACD), an optical phenomenon based on 2D chirality.
- Tzu-Ling Chen
- , Andrew Salij
- & Randall H. Goldsmith
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Article
| Open AccessExpedient production of site specifically nucleobase-labelled or hypermodified RNA with engineered thermophilic DNA polymerases
A general method for enzymatic synthesis of base-modified RNA was developed using engineered thermostable DNA polymerases enabling introduction of site-specific modifications or synthesis of hypermodified RNA not accessible by in vitro transcription.
- Mária Brunderová
- , Vojtěch Havlíček
- & Michal Hocek
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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 AccessEnabling 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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