Featured
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| Open AccessEnhanced carbon dioxide electrolysis at redox manipulated interfaces
While solid oxide electrolysis presents an approach to remove CO2 from high-temperature emission streams, it is challenging to engineer stable yet active interfaces. Here, authors show in situ exsolution of nanoscale metal-metal oxide interfaces that improve cathode activities and durabilities.
- Wenyuan Wang
- , Lizhen Gan
- & Kui Xie
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Article
| Open AccessEnhancing oxygen evolution efficiency of multiferroic oxides by spintronic and ferroelectric polarization regulation
While splitting water into fuel may provide a green, renewable method for energy storage, water oxidation is its bottleneck. Here, authors reported multiferroic electrocatalysts with improved oxygen evolution performances assisted by polarization.
- Xiaoning Li
- , Huan Liu
- & Yalin Lu
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Article
| Open AccessBoundary activated hydrogen evolution reaction on monolayer MoS2
While water-splitting electrocatalysts enable energy storage in carbon-neutral fuels, a recent challenge has been the discovery and understanding of catalyst active sites. Here, authors find domain boundaries in MoS2 materials to present high-activity, stable, and scalable sites for H2 evolution.
- Jianqi Zhu
- , Zhi-Chang Wang
- & Guangyu Zhang
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Article
| Open AccessElectrochemical conversion of methane to ethylene in a solid oxide electrolyzer
Conversion of methane into ethylene is important for chemical feedstocks, but is challenged by catalysts with low selectivity and performance degradation. Here the authors report electrochemical oxidation of methane in a solid oxide electrolyzer, achieving ethylene production with high selectivity and yield.
- Changli Zhu
- , Shisheng Hou
- & Kui Xie
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Article
| Open AccessPromoting electrocatalytic CO2 reduction to formate via sulfur-boosting water activation on indium surfaces
CO2 conversion to liquid fuels provides an appealing means to remove the greenhouse gas, although it is challenging to find materials that are both active and selective. Here, authors show sulfur-doped indium to be a highly active and selective electrocatalyst that transforms CO2 into formate.
- Wenchao Ma
- , Shunji Xie
- & Ye Wang
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Article
| Open AccessSuppressed phase separation of mixed-halide perovskites confined in endotaxial matrices
The bandgap of mixed-halide perovskites can be continuously tuned by changing the halide ratio, but the crystals have poor photo-stability. Here the authors show that photoinduced phase separation is suppressed when perovskite nanocrystals are embedded in a non-perovskite endotaxial matrix.
- Xi Wang
- , Yichuan Ling
- & Hanwei Gao
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Article
| Open AccessExceptionally active iridium evolved from a pseudo-cubic perovskite for oxygen evolution in acid
While water splitting could provide a green means to store energy, there are few materials that can sustain high water oxidation half-reaction rates in acidic electrolytes. Here, authors design a perovskite oxide that generates high performance under-coordinated iridium sites during electrocatalysis.
- Yubo Chen
- , Haiyan Li
- & Zhichuan J. Xu
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Article
| Open AccessPhotoinduced semiconductor-metal transition in ultrathin troilite FeS nanosheets to trigger efficient hydrogen evolution
While earth-abundant materials are promising catalysts for renewable energy conversion, such materials tend to display poor activities. Here, authors show FeS troilite nanosheets to undergo a near-infrared light-triggered transition to a phase that displays improved H2 evolution performances.
- Gang Zhou
- , Yun Shan
- & Xinglong Wu
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Article
| Open AccessChromium-ruthenium oxide solid solution electrocatalyst for highly efficient oxygen evolution reaction in acidic media
H2 generated from water electrolysis is a promising, carbon-neutral fuel, but sluggish oxidation kinetics and poor catalyst stability in acid limits the chemistry. Here, authors prepare solid-solution catalysts based on ruthenium-chromium oxides that are stable and active for acidic water oxidation.
- Yichao Lin
- , Ziqi Tian
- & Liang Chen
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Article
| Open AccessAltered chemistry of oxygen and iron under deep Earth conditions
Iron oxides prevail in the deep Earth, at extreme pressures and temperatures, with different stoichiometries than in ambient conditions. Here, high-pressure synchrotron X-ray spectroscopic measurements reveal the oxidation states of Fe and O in iron superoxide, shedding light on the puzzling chemistry of iron and oxygen in the deep Earth
- Jin Liu
- , Qingyang Hu
- & Wendy L. Mao
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Article
| Open AccessUnusual synergistic effect in layered Ruddlesden−Popper oxide enables ultrafast hydrogen evolution
Water may serve as a renewable hydrogen fuel source to replace fossil fuels, although such electrolysis requires highly active catalysts. Here, authors explore Ruddlesden−Popper oxides as hydrogen evolution electrocatalysts that feature an unusual synergistic effect to promote high activity.
- Yinlong Zhu
- , Hassan A. Tahini
- & Zongping Shao
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Article
| Open AccessPressure-driven phase transitions and reduction of dimensionality in 2D silicon nanosheets
Silicon nanostructures have important applications as functional materials. Here the authors investigate the structural transformations of 2D silicon nanosheets under compression and decompression, showing the irreversible formation of 1D silicon nanowires.
- Gil Chan Hwang
- , Douglas A. Blom
- & Yongjae Lee
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Article
| Open AccessGas-responsive porous magnet distinguishes the electron spin of molecular oxygen
Gas-sensing materials are of increasing societal importance, but the ability to differentiate between similarly sized gases remains highly challenging. Here the authors report on a porous ferrimagnet that distinguishes diamagnetic N2 and CO2 gases from paramagnetic O2 gas.
- Wataru Kosaka
- , Zhaoyuan Liu
- & Hitoshi Miyasaka
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Article
| Open AccessEfficient oxygen evolution electrocatalysis in acid by a perovskite with face-sharing IrO6 octahedral dimers
While splitting water may provide a renewable source of carbon-neutral energy, the water oxidation half-reaction is sluggish and the materials needed show poor stability. Here, authors demonstrate an unusual iridium-based oxide to perform high-efficiency oxygen evolution in acid with good stability.
- Lan Yang
- , Guangtao Yu
- & Xiaoxin Zou
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Article
| Open AccessMetal-organic framework glasses with permanent accessible porosity
Metal–organic framework glasses have emerged as a new family of melt-quenched glass, but have yet to display the accessible porosity of their crystalline counterparts. Here, Bennett and colleagues report that glasses derived from ZIF-76 parent materials possess 4 – 8 Å pores and exhibit reversible gas adsorption.
- Chao Zhou
- , Louis Longley
- & Thomas D. Bennett
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Article
| Open AccessMetastable silica high pressure polymorphs as structural proxies of deep Earth silicate melts
As silica melts are believed to be important components of the Earth’s mantle, their structure should determine many of its properties. Here, the authors identify two crystalline modifications of SiO2, whose local structures closely resemble those of known melts, providing a structural model for their atomic ordering at the nanoscale.
- E. Bykova
- , M. Bykov
- & L. Dubrovinsky
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Article
| Open Access5D operando tomographic diffraction imaging of a catalyst bed
Multi-scale chemical imaging holds the potential to revolutionize our understanding of the relationships between structure and functionality in complex catalytic materials. Here the authors report the results from the first 5D tomographic diffraction imaging experiment of a complex Ni – Pd/ CeO2 – ZrO2/ Al2O3 catalyst used for methane reforming.
- A. Vamvakeros
- , S. D. M. Jacques
- & A. M. Beale
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Article
| Open AccessCooperative mechanisms of oxygen vacancy stabilization and migration in the isolated tetrahedral anion Scheelite structure
Fast oxide ion conductors are the key materials for some technological devices. Here the authors report the creation and stabilization of oxygen vacancies in BiVO4 Scheelite with isolated tetrahedral anion structures for improved ionic conducting performance and understanding of the conduction mechanism.
- Xiaoyan Yang
- , Alberto J. Fernández-Carrión
- & Xiaojun Kuang
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Article
| Open AccessActivity enhancement of cobalt catalysts by tuning metal-support interactions
Tuning metal-support interaction can strongly influence the performance of a catalyst, and is thus essential for catalyst design. Here, the authors investigate reduction-oxidation-reduction treatments as a method to affect metal-support interactions of cobalt-based catalysts in Fischer-Tropsch synthesis.
- Carlos Hernández Mejía
- , Tom W. van Deelen
- & Krijn P. de Jong
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Article
| Open AccessIdentifying an efficient, thermally robust inorganic phosphor host via machine learning
Identifying phosphors with good thermal stability and quantum efficiency is a prerequisite to improve the performance of white LED light sources. Here, a combined machine learning and density functional theory method is introduced to identify next generation inorganic phosphors.
- Ya Zhuo
- , Aria Mansouri Tehrani
- & Jakoah Brgoch
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| Open AccessA zeolitic vanadotungstate family with structural diversity and ultrahigh porosity for catalysis
Zeolitic transition metal oxides provide both porosity and redox activity, thereby further expanding the diversity of porous materials, but their design and development remain rare. Here, the authors report a new class of zeolitic vanadotungstates with tunable frameworks exhibiting a large porosity and redox activity.
- Zhenxin Zhang
- , Qianqian Zhu
- & Wataru Ueda
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Article
| Open AccessExceptional electrocatalytic oxygen evolution via tunable charge transfer interactions in La0.5Sr1.5Ni1−xFexO4±δ Ruddlesden-Popper oxides
Water electrolysis provides a potential means to large-scale renewable fuel generation, although sluggish oxygen evolution kinetics challenges progress. Here, authors report on Ruddlesden–Popper oxides as active oxygen evolution electrocatalysts that provide impetus for overcoming kinetic barriers.
- Robin P. Forslund
- , William G. Hardin
- & Keith J. Stevenson
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| Open AccessAtomic-level insight into super-efficient electrocatalytic oxygen evolution on iron and vanadium co-doped nickel (oxy)hydroxide
While splitting water could provide a renewable way to produce fuel, highly active catalysts are needed to overcome water oxidation’s sluggish kinetics. Here, authors gain atomic-level insight on metal ion synergetic interactions that boost water oxidation performances in co-doped nickel hydroxide.
- Jian Jiang
- , Fanfei Sun
- & Mei Wang
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Article
| Open AccessFe-N system at high pressure reveals a compound featuring polymeric nitrogen chains
Owing to the energetic nature of N–N bonds, poly-nitrogen compounds are considered promising high energy density materials. Here, the authors synthesize three iron–nitrogen compounds at high pressure, including FeN4, which features polymeric nitrogen chains of [N42−]n units.
- M. Bykov
- , E. Bykova
- & L. Dubrovinsky
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| Open AccessCorrosion engineering towards efficient oxygen evolution electrodes with stable catalytic activity for over 6000 hours
Earth-abundant water splitting materials are highly desirable for renewable fuel production, but such catalysts are rarely tested for long-term use. Here, the authors prepare active water-splitting electrocatalysts via corrosion engineering that are stable for thousands of hours.
- Yipu Liu
- , Xiao Liang
- & Jie-Sheng Chen
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Article
| Open AccessDoping-induced structural phase transition in cobalt diselenide enables enhanced hydrogen evolution catalysis
Transition metal dichalcogenides represent an exciting class of earth-abundant hydrogen-from-water electrocatalysts, although low efficiencies limit commercialization. Here, authors present a doping strategy to induce a phase transition in cobalt selenide and boost H2-evolution performance.
- Ya-Rong Zheng
- , Ping Wu
- & Shu-Hong Yu
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Article
| Open AccessA surface-modified antiperovskite as an electrocatalyst for water oxidation
Splitting water into its component elements, oxygen and hydrogen gas, provides a carbon-neutral fuel source, although the availability of cheap, earth-abundant catalysts is lacking. Here, the authors demonstrate antiperovskite-derived materials as high-performance water oxidation electrocatalysts.
- Yanping Zhu
- , Gao Chen
- & Zongping Shao
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Article
| Open AccessFormation of size-dependent and conductive phase on lithium iron phosphate during carbon coating
Coating the active materials of interest with carbon is a widely employed way to boost the performance of lithium ion batteries. Here the authors show the formation of a conductive phase on LiFePO4 during carbon coating, which is size, annealing temperature and reduction atmosphere dependent.
- Yulong Liu
- , Jian Liu
- & Xueliang Sun
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Article
| Open AccessRetrosynthesis of multi-component metal−organic frameworks
The crystal engineering of metal–organic frameworks has led to the construction of complex structures, but has yet to reach the same level of sophistication as organic synthesis. Here, Zhou and colleagues use retrosynthetic chemistry to design and produce complex multi-component frameworks.
- Shuai Yuan
- , Jun-Sheng Qin
- & Hong-Cai Zhou
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| Open AccessSelective control of fcc and hcp crystal structures in Au–Ru solid-solution alloy nanoparticles
The crystal structure of a solid-solution alloy is generally determined by its elemental composition, limiting synthetic control over the alloy’s properties. Here, the authors are able to selectively control the crystal structure of Au–Ru alloy nanoparticles by rationally tuning the reduction speed of the metal precursors.
- Quan Zhang
- , Kohei Kusada
- & Hiroshi Kitagawa
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Article
| Open AccessFacile storage and release of white phosphorus and yellow arsenic
White phosphorus and yellow arsenic represent useful elemental sources for synthetic applications, but their poor stabilities make their storage highly challenging. Here, Scheer and colleagues encapsulate P4 and As4 molecules within porous activated carbons and demonstrate their use in subsequent chemical reactions.
- Andreas E. Seitz
- , Felix Hippauf
- & Manfred Scheer
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Article
| Open AccessAntiferromagnetic correlations in the metallic strongly correlated transition metal oxide LaNiO3
The phase transitions of rare earth nickelates have attracted intensive study as they arise from the complex interplay of charge, spin and lattice degrees of freedom. Here Guo et al. present evidence that LaNiO3 has an unanticipated magnetically ordered metallic phase.
- H. Guo
- , Z. W. Li
- & A. C. Komarek
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Article
| Open AccessIn situ inward epitaxial growth of bulk macroporous single crystals
Porous single crystals are desirable for optoelectronic applications, but their fabrication remains challenging. Here the authors produce centimetre-sized macroporous GaN single crystals with electron mobility comparable to that of bulk crystals via in situ inward epitaxial growth on parent LiGaO2 crystals.
- Chenlong Chen
- , Shujing Sun
- & Kui Xie
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Article
| Open AccessCoupling between oxygen redox and cation migration explains unusual electrochemistry in lithium-rich layered oxides
Lithium ion battery electrodes employing anion redox exhibit high energy densities but suffer from poor cyclability. Here the authors reveal that the voltage of anion redox is strongly affected by structural changes that occur during battery cycling, explaining its unique electrochemical properties.
- William E. Gent
- , Kipil Lim
- & William C. Chueh
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Article
| Open AccessMagnetostriction-polarization coupling in multiferroic Mn2MnWO6
Double corundum-related polar magnets are promising for multiferroic and magnetoelectric applications in spintronics, but are limited by the challenging design and synthesis. Here the authors report the synthesis of Mn2MnWO6 as well as its appealing multiferroic and magnetoelectric properties.
- Man-Rong Li
- , Emma E. McCabe
- & Martha Greenblatt
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| Open AccessAlloy-assisted deposition of three-dimensional arrays of atomic gold catalyst for crystal growth studies
Parallel patterning of atoms over a large surface would represent a major advance over current serial methods of single atom manipulation. Here, the authors explore a periodic instability from liquid alloy droplets for high-throughput atom printing.
- Yin Fang
- , Yuanwen Jiang
- & Bozhi Tian
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| Open AccessProbing dopant segregation in distinct cation sites at perovskite oxide polycrystal interfaces
Space-charges in polycrystalline materials can drive segregation of dopants, however an in-depth understanding of this process is still missing. Here, the authors show that in polycrystalline perovskites the space-charge segregation and interfacial structure are nearly identical irrespective of the interface type.
- Hye-In Yoon
- , Dong-Kyu Lee
- & Sung-Yoon Chung
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| Open AccessA mesoporous cationic thorium-organic framework that rapidly traps anionic persistent organic pollutants
Cationic metal-organic frameworks provide promising opportunities to capture anionic pollutants, but stable frameworks with sufficiently large pores are lacking. Here the authors present a thorium-based mesoporous, cationic and hydrolytically-stable MOF that can rapidly trap inorganic and organic anionic pollutants.
- Yuxiang Li
- , Zaixing Yang
- & Shuao Wang
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Article
| Open AccessThe role of π-blocking hydride ligands in a pressure-induced insulator-to-metal phase transition in SrVO2H
Incorporating hydride anions into transition metal oxides can dramatically affect their structural and electronic properties. Here the authors reveal a pressure-induced insulator-to-metal transition in SrVO2H and show that the compressibility of hydride anions without π-symmetry valence orbitals causes them to act as π-blockers.
- Takafumi Yamamoto
- , Dihao Zeng
- & Michael A. Hayward
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Article
| Open AccessCoulomb spin liquid in anion-disordered pyrochlore Tb2Hf2O7
Experimental studies of frustrated spin systems such as pyrochlore magnetic oxides test our understanding of quantum many-body physics. Here the authors show experimentally that Tb2Hf2O7 may be a model material for investigating how structural disorder can stabilize a quantum spin liquid phase.
- Romain Sibille
- , Elsa Lhotel
- & Michel Kenzelmann
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Article
| Open AccessCapture of organic iodides from nuclear waste by metal-organic framework-based molecular traps
Capturing radioactive organic iodides from nuclear waste is important for safe nuclear energy usage, but remains a significant challenge. Here, Li and co-workers fabricate a stable metal–organic framework functionalized with tertiary amine groups that exhibits high capacities for radioactive organic iodides uptake.
- Baiyan Li
- , Xinglong Dong
- & Jing Li
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Article
| Open AccessOvercoming the crystallization and designability issues in the ultrastable zirconium phosphonate framework system
Zirconium phosphonate based metal-organic frameworks often exhibit superior chemical stabilities, but typically exist as poorly crystalline or amorphous materials. Here the authors exploit an ionothermal method to obtain highly porous and remarkably stable single crystalline zirconium phosphonate frameworks that can efficiently remove uranyl ions from aqueous solutions.
- Tao Zheng
- , Zaixing Yang
- & Shuao Wang
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Article
| Open AccessConstruction of hierarchically porous metal–organic frameworks through linker labilization
Expanding pore sizes and volumes in metal-organic frameworks is challenging, but crucial for the encapsulation of larger guest molecules. Here, Zhou and colleagues report a linker labilization strategy to construct MOFs containing hierarchical pore architectures with dimensions ranging from 1.5 to 18 nm.
- Shuai Yuan
- , Lanfang Zou
- & Hong-Cai Zhou
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Article
| Open AccessEnhancing CO2 electrolysis through synergistic control of non-stoichiometry and doping to tune cathode surface structures
Carbon dioxide electrolysers are promising for chemical storage of renewable electricity; however, achieving effective adsorption/activation of CO2 is still an issue. Here the authors make a perovskite titanate cathode where non-stoichiometry and chemical doping are used to tune the surface structures, facilitating CO2reduction.
- Lingting Ye
- , Minyi Zhang
- & Kui Xie
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Article
| Open AccessRare earth separations by selective borate crystallization
Trivalent lanthanides possess similar chemical properties, making their separation from one another challenging. Here, Wang and colleagues demonstrate that their subtle chemical differences can be greatly amplified during borate crystallization, leading to a low cost and highly efficient separation strategy.
- Xuemiao Yin
- , Yaxing Wang
- & Shuao Wang
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Article
| Open AccessSelective sulfur dioxide adsorption on crystal defect sites on an isoreticular metal organic framework series
The widespread emission of sulfur oxide gases from fossil fuel combustion presents major health risks. Here, the authors show that the selective sulfur dioxide capture performance of a metal organic framework is improved by the introduction of missing linker defects and extra-framework barium cations.
- L. Marleny Rodríguez-Albelo
- , Elena López-Maya
- & Jorge A.R. Navarro
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Article
| Open AccessModulating supramolecular binding of carbon dioxide in a redox-active porous metal-organic framework
Gaining molecular-level insight into host–guest binding interactions is fundamentally important, but experimentally challenging. Here, Schröder and co-workers study CO2–host hydrogen bonding interactions in a pair of isostructural redox-active VIII/VIVMOFs using neutron scattering and diffraction techniques.
- Zhenzhong Lu
- , Harry G. W. Godfrey
- & Martin Schröder
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Article
| Open AccessTunable thermal expansion in framework materials through redox intercalation
The positive thermal expansion exhibited by most materials at increased temperatures is a severe issue for many high precision applications. Here, Xing and co-workers show that redox intercalation of Li ions into a ScF3framework offers effective control of the thermal expansion for this simple material.
- Jun Chen
- , Qilong Gao
- & Xianran Xing
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Article
| Open AccessEllipsoidal analysis of coordination polyhedra
Simple polyhedra in crystalline compounds are often deformed, so methods for analysing their distortions are useful. Here, the authors demonstrate that analysis of the minimum bounding ellipsoid of a coordination polyhedron provides a general method for studying distortion.
- James Cumby
- & J. Paul Attfield