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Effect of pre-intercalation on Li-ion diffusion mapped by topochemical single-crystal transformation and operando investigation
Pre-intercalation with alkali-metal ions is attractive for accessing higher reversible capacity and improved rate performance in Li-ion batteries. Topochemical single-crystal transformations in a tunnel-structured positive electrode are used to clarify the effect of pre-intercalation in modifying the host lattice and altering diffusion pathways.
- Yuting Luo
- , Joseph V. Handy
- & Sarbajit Banerjee
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Article
| Open AccessTrapped O2 and the origin of voltage fade in layered Li-rich cathodes
Oxygen redox cathodes deliver higher energy densities than those based on transition metal redox but commonly exhibit voltage fade on extended cycling. The loss of O-redox capacity and voltage fade is shown to arise from a reduction in O2−/O2 redox process reversibility and O2 loss.
- John-Joseph Marie
- , Robert A. House
- & Peter G. Bruce
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Article
| Open AccessUnlocking Li superionic conductivity in face-centred cubic oxides via face-sharing configurations
Oxides with a face-centred cubic anion sublattice are generally not considered as solid-state electrolytes. Li superionic conductivity in face-centred cubic oxides with face-sharing Li configurations have now been created through cation over-stoichiometry in rocksalt-type lattices via excess Li.
- Yu Chen
- , Zhengyan Lun
- & Gerbrand Ceder
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Letter |
Thermal multiferroics in all-inorganic quasi-two-dimensional halide perovskites
Multiferroics can possess multiple ferroic orders, for example, electric polarization and magnetism, and are of interest for new device applications. Here thermal control is shown to manipulate electric and magnetic orders in a single-phase quasi-two-dimensional halide perovskite.
- Tong Zhu
- , Xue-Zeng Lu
- & Hiroshi Kageyama
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Coupling structural evolution and oxygen-redox electrochemistry in layered transition metal oxides
Transition metal oxide electrodes are promising for rechargeable batteries but are subject to suffer from structural transformations and electrochemical degradation. The evolution of oxygen-redox activity and reversibility in layered electrodes are shown to arise from cation-migration mechanisms during de/intercalation.
- Donggun Eum
- , Byunghoon Kim
- & Kisuk Kang
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Article |
Gate-tuneable and chirality-dependent charge-to-spin conversion in tellurium nanowires
All-electrical generation, manipulation and detection of spin polarization in chiral nanowires is demonstrated.
- Francesco Calavalle
- , Manuel Suárez-Rodríguez
- & Luis E. Hueso
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Article |
Hydride-ion-conducting K2NiF4-type Ba–Li oxyhydride solid electrolyte
Although using proton (H+) conductors is attractive for energy applications, practical conductivity at intermediate temperatures (200–400 °C) remains a challenge. A K2NiF4-type Ba–Li oxyhydride is shown to exhibit a temperature-independent hydrogen conductivity of more than 0.01 S cm–1 above 315 °C.
- Fumitaka Takeiri
- , Akihiro Watanabe
- & Genki Kobayashi
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News & Views |
Printing glass in the nano
A transparent suspension containing colloidal silica is used to additively manufacture three-dimensional structures and photonic devices of silica glass at the nanoscale.
- Paolo Colombo
- & Giorgia Franchin
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Article
| Open AccessPolycrystalline SnSe with a thermoelectric figure of merit greater than the single crystal
SnSe has a very high thermoelectric figure of merit ZT, but uncommonly polycrystalline samples have higher lattice thermal conductivity than single crystals. Here, by controlling Sn reagent purity and removing SnOx impurities, a lower thermal conductivity is achieved, enabling ZT of 3.1 at 783 K.
- Chongjian Zhou
- , Yong Kyu Lee
- & In Chung
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Article |
Extending insertion electrochemistry to soluble layered halides with superconcentrated electrolytes
Insertion compounds in layered oxide or sulfide electrodes provide the fundamental basis of current commercialized Li-ion batteries. The feasibility of reversibly intercalating Li+ electrochemically into halide compounds via the use of superconcentrated electrolytes is now demonstrated.
- Nicolas Dubouis
- , Thomas Marchandier
- & Alexis Grimaud
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Article |
A two-dimensional type I superionic conductor
Superionic conductors present liquid-like ionic diffusivity with applications ranging from energy storage to thermoelectrics. A two-dimensional type I superionic conductor α-KAg3Se2 is now reported and should help to design other materials with tailored ionic conductivities and phase transitions.
- Alexander J. E. Rettie
- , Jingxuan Ding
- & Mercouri G. Kanatzidis
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Obituary |
John Meurig Thomas (1932–2020)
Sir John Meurig Thomas, who was one of the leading materials and catalytic scientists of his generation, sadly died in November 2020, aged 87.
- Richard Catlow
- & Graham Hutchings
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News & Views |
Making large single crystals of 2D MOFs
Linking π-conjugated, electron-deficient ligands into atomically precise large single crystals of conducting 2D metal–organic frameworks can allow the determination of intrinsic electrical conductivity and charge transport mechanism.
- Renhao Dong
- & Xinliang Feng
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Article |
Revisiting metal fluorides as lithium-ion battery cathodes
Metal-fluoride-based lithium-ion battery cathodes are typically classified as conversion materials because reconstructive phase transitions are presumed to occur upon lithiation. Metal fluoride lithiation is now shown to be dominated instead by diffusion-controlled displacement mechanisms.
- Xiao Hua
- , Alexander S. Eggeman
- & Clare P. Grey
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Atomically precise single-crystal structures of electrically conducting 2D metal–organic frameworks
Two-dimensional MOFs can possess porosity and electrical conductivity but are difficult to grow as single crystals. Here, by balancing in-plane and out-of-plane interactions, single crystals of sizes up to 200 µm are grown, allowing in-plane transport measurements and atomic-resolution analysis.
- Jin-Hu Dou
- , Maxx Q. Arguilla
- & Mircea Dincă
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Comment |
Electrochemical methods for determining ionic charge in solids
Classical experiments from solid-state electrochemistry can be used to determine the charge of ions in solids. This Comment also clarifies how the charge of point defects fits with the standard picture of ionic charge, and highlights differences between these electrochemical experiments and methods that probe electrons directly.
- Roger A. De Souza
- & David N. Mueller
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Article |
Bulk fatigue induced by surface reconstruction in layered Ni-rich cathodes for Li-ion batteries
Ni-rich layered cathode materials are promising for high-energy-density Li-ion batteries, but their degradation mechanisms are still poorly understood. A structure-driven mechanism with a lowered accessible state of charge after repetitive cycling is proposed for a typical NMC811 cathode.
- Chao Xu
- , Katharina Märker
- & Clare P. Grey
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Article |
The interplay between thermodynamics and kinetics in the solid-state synthesis of layered oxides
Understanding the competition between thermodynamics and kinetics is crucial for the rational synthesis of inorganic materials. The synthesis of two-layer sodium metal oxides is investigated by in situ synchrotron XRD and a model is developed to rationalize why the observed phase progression proceeds through non-equilibrium three-layered intermediates.
- Matteo Bianchini
- , Jingyang Wang
- & Gerbrand Ceder
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News & Views |
Minerals from colloidal assembly
Magnetite crystals form by the aggregation and subsequent merger of crystalline precursors, which can be interpreted in terms of colloidal assembly.
- Jeffrey D. Rimer
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Article |
High oxide ion and proton conductivity in a disordered hexagonal perovskite
Fast oxide ion and proton conductors at intermediate temperature are required to improve the performance of ceramic fuel cells. An undoped hexagonal perovskite Ba7Nb4MoO20 electrolyte with high proton and oxide ion conductivity (4.0 mS cm−1) at 510 °C is now reported.
- Sacha Fop
- , Kirstie S. McCombie
- & Abbie C. Mclaughlin
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Article |
Understanding the conversion mechanism and performance of monodisperse FeF2 nanocrystal cathodes
The application of metal fluorides as cathodes for lithium ion batteries has been hindered by inadequate understanding of their electrochemical capabilities. Reversible conversion reaction in iron fluoride nanocrystals is shown to be due to topotactic cation diffusion and nucleation of metallic particles.
- Albert W. Xiao
- , Hyeon Jeong Lee
- & Mauro Pasta
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Letter |
Selective nitrogen adsorption via backbonding in a metal–organic framework with exposed vanadium sites
Nitrogenases use transition metals to selectively capture weak π acids such as N2 by employing backbonding interactions. Here, a metal–organic framework with exposed vanadium sites is presented that uses this approach for selective capture of N2 from CH4, with impressive selectivity and capacity.
- David E. Jaramillo
- , Douglas A. Reed
- & Jeffrey R. Long
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News & Views |
Charting stability space
A comprehensive chemical space of potential inorganic ternary metal nitrides has been explored by computational methods as a guideline for their experimental synthesis and discovery.
- Ralf Riedel
- & Zhaoju Yu
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Article |
A map of the inorganic ternary metal nitrides
High-throughput computation is especially useful for materials screening where synthesis is challenging. Here, it is used to construct a stability map of ternary nitrides, allowing discovery of stable compounds and providing insight into principles that govern nitride stability.
- Wenhao Sun
- , Christopher J. Bartel
- & Gerbrand Ceder
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Article |
Metal–oxygen decoordination stabilizes anion redox in Li-rich oxides
Reversible high-voltage redox is a key component for electrochemical technologies from electrocatalysts to lithium-ion batteries. A point defect explanation for why anion redox occurs with local structural disordering and voltage hysteresis is proposed.
- Jihyun Hong
- , William E. Gent
- & William C. Chueh
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Letter |
Organic-based magnon spintronics
Generation, transport and detection of spin-wave quanta in vanadium tetracyanoethylene, an organic ferrimagnet with low Gilbert damping, are reported.
- Haoliang Liu
- , Chuang Zhang
- & Z. Valy Vardeny
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News & Views |
Illuminating interlayer interactions
A synchrotron X-ray diffraction experiment demonstrates an unexpected accumulation of electron density in the interlayer region of TiS2, and provides a benchmark for theoretical models of weak interlayer bonding.
- Xiaohui Qiu
- & Wei Ji
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Thermochromic halide perovskite solar cells
CsPbI3–xBrx solar cells, which undergo temperature- and moisture-driven reversible transitions between a non-perovskite transparent phase and a perovskite light-absorbing phase, are used as thermochromic photovoltaic devices integrated in windows.
- Jia Lin
- , Minliang Lai
- & Peidong Yang
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Letter |
Liquid-like thermal conduction in intercalated layered crystalline solids
Investigation of the thermal transport properties of AgCrSe2 reveals complete suppression of the transverse acoustic phonons by ultrafast dynamic disorder with only the longitudinal acoustic mode surviving, resembling the thermal conduction of liquids.
- B. Li
- , H. Wang
- & M. G. Kanatzidis
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Article |
Reversible magnesium and aluminium ions insertion in cation-deficient anatase TiO2
Compared to monovalent lithium or sodium ions, the reversible insertion of multivalent ions into battery electrodes has proved challenging. An aliovalent doping strategy involving reversible Mg2+ and Al3+ insertion in anatase TiO2 is now reported.
- Toshinari Koketsu
- , Jiwei Ma
- & Damien Dambournet
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News & Views |
Stabilizing colour and intensity
Thermally activated defects in a blue-emitting phosphor can enhance energy transfer to the activator, and compensate for thermal quenching.
- Philippe F. Smet
- & Jonas J. Joos
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Article |
Evidence for anionic redox activity in a tridimensional-ordered Li-rich positive electrode β-Li2IrO3
For high-capacity electrodes with anionic redox, the importance of structural dimensionality has not been elucidated. The possibility of triggering anionic redox activity in a tridimensional-ordered Li-rich positive electrode is now demonstrated.
- Paul E. Pearce
- , Arnaud J. Perez
- & Jean-Marie Tarascon
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Letter |
Unravelling surface and interfacial structures of a metal–organic framework by transmission electron microscopy
The operational conditions used for electron microscopy can limit the insight that can be gained from fragile material samples. It is shown here how high-resolution TEM analysis of delicate MOFs can be achieved.
- Yihan Zhu
- , Jim Ciston
- & Yu Han
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Article |
A zero-thermal-quenching phosphor
A blue-emitting phosphor without thermal quenching is reported. The emission losses at high temperatures are compensated by a counter mechanism, originating in energy transfer between electron–hole pairs and thermally activated defect levels.
- Yoon Hwa Kim
- , Paulraj Arunkumar
- & Won Bin Im
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Letter |
Conductive MOF electrodes for stable supercapacitors with high areal capacitance
Using MOFs as active electrodes in electrochemical double layer capacitors has so far proved difficult. An electrically conductive MOF used as an electrode is now shown to exhibit electrochemical performance similar to most carbon-based materials.
- Dennis Sheberla
- , John C. Bachman
- & Mircea Dincă
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News & Views |
Rayleigh scattering revisited
Scaling of the phonon damping with the wavevector in glasses is found to be different from the traditionally assumed Rayleigh scattering, and related to surprising, long-range correlations in the local elasticity matrix.
- Jeppe C. Dyre
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Article |
Tuning magnetic anisotropy by interfacially engineering the oxygen coordination environment in a transition metal oxide
The thickness of Ca0.5Sr0.5TiO3 is found to modify the oxygen coordination environment of SrRuO3 in the heterostructure GdScO3/Ca0.5Sr0.5TiO3/SrRuO3, also allowing the magnetic anisotropy to be tuned in the entire SrRuO3 layer.
- Daisuke Kan
- , Ryotaro Aso
- & Yuichi Shimakawa
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Letter |
A new active Li–Mn–O compound for high energy density Li-ion batteries
The search for new materials that can improve the energy density of Li-ion batteries is technologically important. An electrochemically active compound with the composition Li4Mn2O5 exhibits an unprecedented discharge capacity of 355 mAh g−1.
- M. Freire
- , N. V. Kosova
- & V. Pralong
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Article |
Direct mapping of Li-enabled octahedral tilt ordering and associated strain in nanostructured perovskites
Understanding the mechanisms driving the formation of 2D and 3D superlattices at the atomic scale is difficult. An approach for direct mapping of Li-enabled octahedral tilt ordering and associated strain in nanostructured perovskites is now proposed.
- Ye Zhu
- , Ray L. Withers
- & Joanne Etheridge
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Article |
Fast and long-range triplet exciton diffusion in metal–organic frameworks for photon upconversion at ultralow excitation power
Controlled overlap of molecular orbitals in metal–organic frameworks enhances triplet exciton diffusion in these structures, which are now used in solid-state photon upconverters operating under excitation power comparable to solar irradiance.
- Prasenjit Mahato
- , Angelo Monguzzi
- & Nobuo Kimizuka
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News & Views |
'Ferroelectricity' in a metal
The discovery of a ferroelectric-like structural transition in metallic LiOsO3 identifies a new class of materials with unconventional properties, providing an exotic playground for theorists and experimentalists.
- Veerle Keppens
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Letter |
Locally enhanced conductivity due to the tetragonal domain structure in LaAlO3/SrTiO3 heterointerfaces
The emergence of conductivity at the {001} interface of LaAlO3 and SrTiO3 is one of the more celebrated examples of interface engineering. Using a microscopy approach based on a sensitive magnetometry probe, it is now shown that narrow paths of enhanced conductivity occur along the crystallographic axes of the oxide structures.
- Beena Kalisky
- , Eric M. Spanton
- & Kathryn A. Moler
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News & Views |
Bonding them all
A general approach for decorating nanoparticles with a highly dense shell of DNA linkers expands the range of building blocks that can be used for DNA-mediated nanoparticle self-assembly.
- Ulrich Simon
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