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| Open AccessModulating the hierarchical fibrous assembly of Au nanoparticles with atomic precision
Constructing nanoparticle assemblies with atomic precision remains a major challenge in nanoscience. Here, the authors realize atomic‐level control over the 1D, 2D and hierarchical 3D assembly of Au nanoparticles by modulating the site‐specific surface ligands and associated counterions.
- Qi Li
- , Jake C. Russell
- & Rongchao Jin
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Article
| Open AccessAtom-hybridization for synthesis of polymetallic clusters
Multimetallic clusters are difficult to synthesize with control over elemental composition and organization. Here, the authors use dendrimers to precisely template the formation of five-element sub-nanoclusters, providing an elegant route to otherwise-inaccessible multinary compounds.
- Takamasa Tsukamoto
- , Tetsuya Kambe
- & Kimihisa Yamamoto
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Article
| Open AccessSolvatochromic covalent organic frameworks
Covalent organic frameworks (COFs) find increasing application as sensor material, but fast switching solvatochromism was not realized. Here the authors demonstrate that combination of electron-rich and -deficient building blocks leads to COFs which fast and reversibly change of their electronic structure depending on the surrounding atmosphere.
- Laura Ascherl
- , Emrys W. Evans
- & Florian Auras
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Article
| Open AccessAntagonistic chemical coupling in self-reconfigurable host–guest protocells
Multi-compartmentalised soft micro-systems are used as models of synthetic protocells. Here, the authors developed nested host–guest protocell constructs capable of self-reconfiguration in response to changes in pH generated by antagonistic modes of enzyme-mediated coupling.
- Nicolas Martin
- , Jean-Paul Douliez
- & Stephen Mann
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Article
| Open AccessSelective sorting of polymers with different terminal groups using metal-organic frameworks
The separation of high molecular weight polymers composed of the same number of monomeric units remains highly challenging. Here, the authors show that efficient separation and purification of mixtures of polymers that differ only by their terminal groups can be achieved through polymer threading in metal-organic framework channels.
- Benjamin Le Ouay
- , Chikara Watanabe
- & Takashi Uemura
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Article
| Open AccessBioinspired ultra-stretchable and anti-freezing conductive hydrogel fibers with ordered and reversible polymer chain alignment
High-performance stretchable conductive fibers are desired for the development of stretchable electronic devices but preparation of conductive hydrogel fibers is challenging. Inspired by spider silk the authors demonstrate here a spinning method to prepare stretchable conductive hydrogel fibers with ordered polymer chain alignment.
- Xue Zhao
- , Fang Chen
- & Mingming Ma
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Article
| Open AccessCrystalline TiO2 protective layer with graded oxygen defects for efficient and stable silicon-based photocathode
While silicon-based materials can convert sunlight directly to fuel and electricity, balancing their stability and efficiency constrains usage. Here, authors protect silicon photocathodes with crystalline titanium dioxide layers with graded oxygen defects to improve both durability and efficiency.
- Jianyun Zheng
- , Yanhong Lyu
- & Shuangyin Wang
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Article
| Open AccessNear-infrared-triggered photon upconversion tuning in all-inorganic cesium lead halide perovskite quantum dots
Optimizing luminescence from quantum dots benefits various optoelectronic and photovoltaic applications. Here the authors drive high-efficiency, tunable upconversion luminescence in perovskite quantum dots by energy transfer from lanthanide-doped nanoparticles excited by near-infrared light, to produce full-color emission with low driving power.
- Wei Zheng
- , Ping Huang
- & Xueyuan Chen
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Article
| Open AccessMorphology and structure of ZIF-8 during crystallisation measured by dynamic angle-resolved second harmonic scattering
Angle-resolved monitoring of structure parameters during crystal growth is often slow owing to mechanical movements. Here, the authors use second harmonic scattering and Fourier-plane imaging to dynamically monitor size, shape and concentration of ZIF-8 in situ during the growth process.
- Stijn Van Cleuvenbergen
- , Zachary J. Smith
- & Monique A. van der Veen
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Article
| Open AccessPhoto-generated dinuclear {Eu(II)}2 active sites for selective CO2 reduction in a photosensitizing metal-organic framework
Solar-to-chemical CO2 reduction provides a means to use light’s energy for CO2 removal and upgrading to useful products, although this photochemical conversion is challenging. Here, authors construct a Europium-containing metal-organic framework that selectively converts CO2 to formate with light.
- Zhi-Hao Yan
- , Ming-Hao Du
- & Lan-Sun Zheng
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Article
| Open AccessCo-crystallization of atomically precise metal nanoparticles driven by magic atomic and electronic shells
Atomic shell closure and electronic shell closure are generally considered to be competing effects in stabilizing magic-sized metal nanoclusters. Here, the authors show, by co-crystallizing two differently-sized clusters, that both mechanisms can work concurrently during magic cluster synthesis.
- Juanzhu Yan
- , Sami Malola
- & Nanfeng Zheng
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Article
| Open AccessDual stimuli-responsive rotaxane-branched dendrimers with reversible dimension modulation
Mechanically interlocked molecules are extensively applied as artificial molecular machines but rotaxane-branched dendrimers are rarely explored because of synthetic challenges. Here the authors present the construction of dual stimuli-responsive rotaxane-branched dendrimer which can be stimulated by DMSO or acetate ions.
- Xu-Qing Wang
- , Wei Wang
- & Hai-Bo Yang
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Article
| Open AccessCrystalline polymeric carbon dioxide stable at megabar pressures
The nature and stability of carbon dioxide under extreme conditions relevant to the Earth’s mantle is still under debate, in view of its possible role within the deep carbon cycle. Here, the authors perform high-pressure experiments providing evidence that polymeric crystalline CO2 is stable under megabaric conditions.
- Kamil F. Dziubek
- , Martin Ende
- & Ronald Miletich
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Article
| Open AccessA dynamic and multi-responsive porous flexible metal–organic material
Stimuli-responsive porous materials are attractive for a range of applications, but each material typically exhibits only one type of transformation. Here, the authors report on a metal–organic material that exhibits six distinct phases as a result of four types of structural transformation in response to different stimuli.
- Mohana Shivanna
- , Qing-Yuan Yang
- & Michael J. Zaworotko
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Article
| Open AccessBa3Mg3(BO3)3F3 polymorphs with reversible phase transition and high performances as ultraviolet nonlinear optical materials
Nonlinear optical crystals suitable for the UV spectral region could simplify short-wavelength generation and make it more efficient. Here, the authors design and demonstrate that one of two asymmetric borate polymorphs exhibits promising optical and mechanical properties for generating UV light.
- Miriding Mutailipu
- , Min Zhang
- & Shilie Pan
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Article
| Open AccessHighly sensitive switching of solid-state luminescence by controlling intersystem crossing
The development of intelligent materials, in particular those showing the highly sensitive mechanoresponsive luminescence (MRL), remains challenging. Here the authors report a strategy for constructing high performance On-Off MRL materials by introducing nitrophenyl groups to molecules with aggregation-induced emission characteristic.
- Weijun Zhao
- , Zikai He
- & Ben Zhong Tang
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Article
| Open AccessBlock copolymer crystalsomes with an ultrathin shell to extend blood circulation time
In block copolymer vesicles, crystallization often leads to defects and renders the structures leaky that undermines their potential biomedical application. Here the authors use an emulsion solution method to control the crystallization of an amphiphilic block copolymer at the curved liquid/liquid interface to improve the blood circulation time.
- Hao Qi
- , Hao Zhou
- & Christopher Y. Li
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Article
| Open AccessLong range electronic phase separation in CaFe3O5
Electronic phase separation is an important feature of many correlated perovskite compounds but hasn’t been seen in other complex oxides with similar physical behaviour such as magnetite. Hong et al. find phase separation between a magnetite-like charge ordered phase and a charge averaged phase in CaFe3O5.
- Ka. H. Hong
- , Angel M. Arevalo-Lopez
- & J. Paul Attfield
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Article
| Open AccessEvolution of cooperativity in the spin transition of an iron(II) complex on a graphite surface
Spin-crossover molecules offer a potential route towards molecular spintronics, but retaining the bistability of the spin state upon surface deposition is challenging. Here, the authors study the spin-crossover behaviours of an Fe(II) complex deposited on graphite, determining the scale limit at which cooperative spin switching becomes effective.
- Lalminthang Kipgen
- , Matthias Bernien
- & Wolfgang Kuch
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Article
| Open AccessA facile strategy for realizing room temperature phosphorescence and single molecule white light emission
The demonstration of pure organic room temperature phosphorescence (RTP) luminogens with complementary emission is a key requirement for developing low-cost white light emitters. Here, the authors construct RTP-active organic salt compounds by exchanging the counterion with a heavy halide ion.
- Jianguo Wang
- , Xinggui Gu
- & Ben Zhong Tang
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Article
| Open AccessDrug capture materials based on genomic DNA-functionalized magnetic nanoparticles
Chemotherapy agents are prone to producing severe side-effects, and their sequestration prior to their entering of the circulatory system is thus highly desirable. Here, the authors functionalize iron oxide nanoparticles with genomic DNA and achieve sequestration of doxorubicin, cisplatin, and epirubicin from biological solutions.
- Carl M. Blumenfeld
- , Michael D. Schulz
- & Robert H. Grubbs
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Article
| Open AccessNano-photosensitizer based on layered double hydroxide and isophthalic acid for singlet oxygenation and photodynamic therapy
Usually, several components are needed for efficient 2-photon photodynamic therapy (PDT). Here, the authors sandwiched carboxylic acids between layered double hydroxide nanosheets to obtain a single-handed biocompatible photosensitizer that generates singlet oxygen in high quantum yield.
- Rui Gao
- , Xuan Mei
- & Min Wei
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Article
| Open AccessMechanically tunable conductive interpenetrating network hydrogels that mimic the elastic moduli of biological tissue
Conductive and stretchable materials that match the elastic moduli of biological tissue are desired for enhanced interfacial and mechanical stability. Here the authors show a method for fabricating highly conductive hydrogels comprising two interpenetrating networks.
- Vivian R. Feig
- , Helen Tran
- & Zhenan Bao
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Article
| Open AccessSelf-assembly of metal–organic polyhedra into supramolecular polymers with intrinsic microporosity
Porosity in metal–organic materials typically relies on highly ordered crystalline networks, which hinders material processing and morphological control. Here, the authors use metal–organic polyhedra as porous monomers in supramolecular polymerization to produce colloidal spheres and gels with intrinsic microporosity.
- Arnau Carné-Sánchez
- , Gavin A. Craig
- & Shuhei Furukawa
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Article
| Open AccessDomino-like multi-emissions across red and near infrared from solid-state 2-/2,6-aryl substituted BODIPY dyes
The class of BODIPY dyes has high solubility and high quantum yields and is widely used in imaging applications. Here Tian et al. synthesize new dye molecules and demonstrate extended emission properties and application scope controllable both by the excitation wavelength and aggregation states.
- Dan Tian
- , Fen Qi
- & Wei Huang
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Article
| Open AccessCollective molecular switching in hybrid superlattices for light-modulated two-dimensional electronics
Photochromic molecules offer the unique opportunity to demonstrate multifunctional devices with light-tunable electrical characteristics. Gobbi et al. build light-switchable electronic heterojunctions based on atomically precise, photo-reversible molecular superlattices on graphene and MoS2.
- Marco Gobbi
- , Sara Bonacchi
- & Paolo Samorì
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Article
| Open AccessSingle-layer graphene membranes by crack-free transfer for gas mixture separation
Graphene shows great promise for gas separation applications, but obtaining large membranes that are free of cracks and tears remains highly challenging. Here, the authors realize monolayer, crack-free, millimeter-scale graphene membranes that exhibit selective gas permeation solely thanks to their intrinsic defects
- Shiqi Huang
- , Mostapha Dakhchoune
- & Kumar Varoon Agrawal
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Article
| Open AccessA coronene-based semiconducting two-dimensional metal-organic framework with ferromagnetic behavior
Endowing metal–organic frameworks with both high electrical conductivity and magnetic ordering could make such materials useful for spintronics. Here the authors design a layer-stacking coronene-based 2D MOF that exhibits a semiconducting feature with an electrical conductivity of ~10 S cm−1 at 300 K, as well as ferromagnetism below ~20 K.
- Renhao Dong
- , Zhitao Zhang
- & Xinliang Feng
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Article
| Open AccessUniversal geometric frustration in pyrochlores
The family of pyrochlore complex oxides includes many materials of fundamental or practical interest, such as spin ices and dielectrics. Trump et al. show that flexibility of the pyrochlores’ structure leads to local displacements that explain some of their unusual physical properties.
- B. A. Trump
- , S. M. Koohpayeh
- & T. M. McQueen
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Article
| Open AccessSpin–phonon couplings in transition metal complexes with slow magnetic relaxation
Transition metal complexes that display slow magnetic relaxation show promise for information storage, but our mechanistic understanding of the magnetic relaxation of such compounds remains limited. Here, the authors spectroscopically and computationally characterize the strength of spin–phonon couplings, which play an important role in the relaxation process.
- Duncan H. Moseley
- , Shelby E. Stavretis
- & Zi-Ling Xue
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Article
| Open AccessControl over the emerging chirality in supramolecular gels and solutions by chiral microvortices in milliseconds
Symmetry breaking and chiral amplification are fundamental principles in chemistry and biology but the control of initial chiral bias remains a great challenge. Here the authors show that chiral microvortices can lead to a selection of initial chiral bias of supramolecular systems composed of achiral molecules.
- Jiashu Sun
- , Yike Li
- & Minghua Liu
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Article
| Open AccessTopochemical conversion of an imine- into a thiazole-linked covalent organic framework enabling real structure analysis
Stabilization of covalent organic frameworks (COFs) by post-synthetic locking is a powerful tool to push the limits of COF utilization. Here the authors demonstrate a sulfur-assisted conversion of an imine-linked COF into a thiazole-linked COF, with retention of crystallinity and porosity, allowing for direct imaging of defects in COFs.
- Frederik Haase
- , Erik Troschke
- & Bettina V. Lotsch
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Article
| Open AccessVapor sublimation and deposition to build porous particles and composites
Fabrication of porous nanoparticles is often hampered by low efficiency production methods, challenging isolation of the material and poor control over the fabrication process. Here the authors demonstrate a facile ice-template vapor-phase synthesis which allows for production of porous poly-para-xylylene particles on a large scale.
- Hsing-Ying Tung
- , Zhen-Yu Guan
- & Hsien-Yeh Chen
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| Open AccessHigh-performance bifunctional porous non-noble metal phosphide catalyst for overall water splitting
Water electrolysis provides a carbon-neutral means to generate hydrogen fuel from water, but the process typically requires expensive, rare metal catalysts. Here, the authors prepare hydrogen- and oxygen-evolving electrocatalysts from earth-abundant elements that outperform noble-metal counterparts.
- Fang Yu
- , Haiqing Zhou
- & Zhifeng Ren
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Article
| Open AccessUnderstanding crystallization pathways leading to manganese oxide polymorph formation
Minor variations in synthesis conditions can redirect crystallization pathways through different nonequilibrium intermediates. Here, the authors present a theoretical framework to predict which polymorphs appear during MnO2 precipitation, which is validated by in situ X-ray scattering of reaction progression.
- Bor-Rong Chen
- , Wenhao Sun
- & Laura T. Schelhas
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Article
| Open AccessAccelerating the discovery of insensitive high-energy-density materials by a materials genome approach
The synthesis of explosive materials that are stable, highly dense, and have low sensitivity to external stimuli is a challenge. Here, the authors use a genomic approach to accelerate the discovery of insensitive high explosive molecules with good detonation and low sensitivity properties.
- Yi Wang
- , Yuji Liu
- & Yong Tian
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Article
| Open AccessSystematic design of superaerophobic nanotube-array electrode comprised of transition-metal sulfides for overall water splitting
Water splitting by nanostructured, abundant catalysts provides a renewable means to make carbon neutral fuels, but the ideal material morphology and composition remain uncertain. Here, the authors prepare superaerophobic, multi-metallic sulfide nanotube arrays as bifunctional water splitting catalysts.
- Haoyi Li
- , Shuangming Chen
- & Xun Wang
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Article
| Open AccessTailoring exciton and excimer emission in an exfoliated ultrathin 2D metal-organic framework
Two dimensional (2D) metal-organic frameworks have demonstrated unique photophysical properties compared to their bulk analogs. Here, the authors demonstrate that exfoliation of 2D MOFs can suppress interlayer exciton-related emission, allowing for modulation of the overall emission color and switching of optical memory states.
- Wei-Ming Liao
- , Jian-Hua Zhang
- & Cheng-Yong Su
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Article
| Open AccessOut-of-equilibrium microcompartments for the bottom-up integration of metabolic functions
Generating artificial cells able to carry out metabolic activities out-of-equilibrium is a current challenge in synthetic biology. Here the authors use a microfluidic platform for integration and analysis of minimal metabolic reactions in artificial microcompartments formed of water-in-oil droplets.
- Thomas Beneyton
- , Dorothee Krafft
- & Jean-Christophe Baret
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Article
| Open AccessRecipes for improper ferroelectricity in molecular perovskites
In layered inorganic materials lattice distortions can couple to break inversion symmetry and drive improper ferroelectricity, but in perovskites, symmetry prohibits such an effect. Here, the authors use group-theoretical analysis to provide crystal engineering design principles for improper ferroelectricity in molecular perovskites.
- Hanna L. B. Boström
- , Mark S. Senn
- & Andrew L. Goodwin
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Article
| Open AccessLiquid phase blending of metal-organic frameworks
The recently introduced glass and liquid states of metal–organic frameworks (MOFs) provide opportunities to design and explore new properties for this class of material. Here, the authors show that a MOF liquid can be blended with another MOF component to produce domain-structured MOF glasses with single, tailorable glass transitions.
- Louis Longley
- , Sean M. Collins
- & Thomas D. Bennett
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Article
| Open AccessOn-surface synthesis of poly(p-phenylene ethynylene) molecular wires via in situ formation of carbon-carbon triple bond
Incorporating carbon-carbon triple bonds into conjugated chains typically requires acetylenic precursors. Here, the authors synthesize poly(p-phenylene ethynylene) molecular wires on Cu(111) by directly coupling trichloromethyl-containing precursors, forming C-C triple bonds in situ
- Chen-Hui Shu
- , Meng-Xi Liu
- & Pei-Nian Liu
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Article
| Open AccessControlled synthesis of highly-branched plasmonic gold nanoparticles through peptoid engineering
Peptoids are promising crystallization agents, as they offer the molecular recognition capabilities of proteins and peptides but with higher stability and synthetic tunability. Here, the authors show that sequence-defined peptoids can controllably template the formation and shape evolution of gold nanostructures with defined morphologies.
- Feng Yan
- , Lili Liu
- & Chun-Long Chen
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Article
| Open AccessTopologically frustrated dynamics of crowded charged macromolecules in charged hydrogels
Diffusion of molecules in crowded environment is important for various living systems, but the dynamics of charged molecules in charged matrices remains still unexplored. Here the authors report a dynamics of DNA and polyelectrolytes in a charged hydrogel where the guest molecules do not diffuse but experience topologically frustrated dynamics.
- Di Jia
- & Murugappan Muthukumar
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Article
| Open AccessCrosslinking of fibrous hydrogels
Unlike synthetic hydrogels, biological gels are made of fibrous networks which give rise to unique properties, such as high porosity and mechanical responsiveness. Here the authors use polyisocyanide-based gels and selectively crosslink inside the bundles to lock the fibrous network and thus control the architecture and the mechanics.
- Daniël C. Schoenmakers
- , Alan E. Rowan
- & Paul H. J. Kouwer
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Article
| Open AccessTransient modes of zeolite surface growth from 3D gel-like islands to 2D single layers
While zeolites are industrially relevant as molecular sieves and catalysts, their growth mechanisms remain widely debated. Here, Rimer and colleagues probe the crystallization pathway of zeolite LTA with spatiotemporal resolution, identifying a distinctive nonclassical pathway, and demonstrating that growth is highly dependent on synthetic conditions.
- Manjesh Kumar
- , Madhuresh K. Choudhary
- & Jeffrey D. Rimer
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Article
| Open AccessCross-plane coherent acoustic phonons in two-dimensional organic-inorganic hybrid perovskites
Two-dimensional, organic-inorganic hybrid perovskites have sustained research interest due to attractive optoelectronic and excitonic properties. Here, Guo et al. systematically investigate coherent acoustic phonon transport versus layer thickness in these materials with strong acoustic impedance mismatch
- Peijun Guo
- , Constantinos C. Stoumpos
- & Richard D. Schaller
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Article
| Open AccessNanoparticle-templated nanofiltration membranes for ultrahigh performance desalination
Nanofiltration membranes are important for water desalination technologies, but designing membranes that achieve both high permeance and high salt rejection remains challenging. Here, the authors use sacrificial nanoparticles in the membrane fabrication process, leading to crumpled structures with ultrahigh permeance.
- Zhenyi Wang
- , Zhangxin Wang
- & Jian Jin
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Article
| Open AccessHigh-resolution AFM structure of DNA G-wires in aqueous solution
DNA and RNA G-quadruplexes can stack to form higher-order structures called G-wires. Here the authors report high-resolution AFM images of higher-order DNA G-quadruplexes in aqueous solution that could impact the design of G-wire based nanodevices and the understanding of G-wires in biology.
- Krishnashish Bose
- , Christopher J. Lech
- & Anh Tuân Phan