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Extending carbon chemistry at high-pressure by synthesis of CaC2 and Ca3C7 with deprotonated polyacene- and para-poly(indenoindene)-like nanoribbons
The authors demonstrate that carbides with infinite chains of fused [C6] and [C5] rings are synthesized at deep planetary pressures and temperatures. Hydrolysis of these carbides may lead to polycyclic aromatic hydrocarbons in the Universe.
- Saiana Khandarkhaeva
- , Timofey Fedotenko
- & Leonid Dubrovinsky
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Stabilization of N6 and N8 anionic units and 2D polynitrogen layers in high-pressure scandium polynitrides
The authors discover high-pressure Sc2N6, Sc2N8, and ScN5 polynitrides, synthesized at high pressure and temperature conditions, featuring a unique nitrogen catenation and previously unknown N66− anions, N86− anions and anionic corrugated 2D-polynitrogen layers.
- Andrey Aslandukov
- , Alena Aslandukova
- & Leonid Dubrovinsky
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Designing lithium halide solid electrolytes
The pursuit of all-solid-state batteries has motivated advancements in materials design. Here, the authors present a methodology demonstrating that ionic potential effectively captures crucial interactions within halide materials, guiding the design of the new materials with enhanced performance.
- Qidi Wang
- , Yunan Zhou
- & Marnix Wagemaker
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A fast ceramic mixed OH−/H+ ionic conductor for low temperature fuel cells
Low temperature ionic conducting materials such as OH- and H+ ionic conductors are important electrolyte materials. Here the authors report the discovery of fast mixed OH- /H+ conductors in ceramic materials, SrZr0.8Y0.2O3-δ and CaZr0.8Y0.2O3-δ, for potential use as electrolytes in fuel cells.
- Peimiao Zou
- , Dinu Iuga
- & Shanwen Tao
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Helical-caging enables single-emitted large asymmetric full-color circularly polarized luminescence
Circularly polarised luminescence (CPL) is essential for asymmetric synthetic photochemistry. Here, the authors integrate white quantum dots with chiral nematic liquid crystal or liquid crystal polymer to achieve single-emitted tuneable full-colour or white CPL for enantioselective polymerization.
- Yajie Zhou
- , Yaxin Wang
- & Taotao Zhuang
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Colloidal pathways of amorphous calcium carbonate formation lead to distinct water environments and conductivity
The mechanism of calcium carbonate formation has been of interest for decades, but additive-controlled systems are poorly understood. Here the authors show that polycarboxylates facilitate bicarbonate entrapment and thereby inhibit nucleation. Distinct water environments in amorphous calcium carbonate nanoparticles arise from colloidal formation pathways and lead to mineral conductivity.
- Maxim B. Gindele
- , Sanjay Vinod-Kumar
- & Guinevere Mathies
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In situ observation of a stepwise [2 + 2] photocycloaddition process using fluorescence spectroscopy
Using highly sensitive and selective in situ techniques to investigate the dynamics of intermediates formation is key to better understand reaction mechanisms but investigating the early stages of solid-state reactions or transformations is still challenging. Here the authors use in situ fluorescence spectroscopy to observe the evolution of intermediates during a two-step [2 + 2] photocycloaddition process in a coordination polymer.
- Meng-Fan Wang
- , Yun-Hu Deng
- & Jian-Ping Lang
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Anisotropic flexibility and rigidification in a TPE-based Zr-MOFs with scu topology
Metal-organic frameworks (MOFs) with adjustable porosity and tunable functionality have attracted considerable attention, but the directional control of intermolecular and intramolecular motion of TPE-based ligands in the non-interpenetrated flexible MOFs has not yet been studied. Here, the authors report a non-interpenetrated tetraphenylethylene-based MOF with anisotropic flexibility.
- Sha-Sha Meng
- , Ming Xu
- & Zhi-Yuan Gu
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Ce-mediated molecular tailoring on gigantic polyoxometalate {Mo132} into half-closed {Ce11Mo96} for high proton conduction
Polyoxometalates (POMs) are molecular clusters with diverse structures. Here authors present the synthesis of POMs by Ce-mediated molecular tailoring from gigantic {Mo132} into half-closed {Ce11Mo96}, with proton conductivity nearly two orders of magnitude higher than {Mo132}.
- Xue-Xin Li
- , Cai-Hong Li
- & Zhong-Min Su
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Article
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Atomic stiffness for bulk modulus prediction and high-throughput screening of ultraincompressible crystals
Fast and accurate prediction of bulk moduli for diverse materials is challenging. Here, the authors introduce the concept of atomic stiffness to accelerate bulk modulus prediction and high-throughput screening of ultra-incompressible crystals.
- Ruihua Jin
- , Xiaoang Yuan
- & Enlai Gao
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The curious case of the structural phase transition in SnSe insights from neutron total scattering
The thermoelectric properties of SnSe are attributed to a high-temperature phase transition, whose nature has not been resolved. Here the authors probe the transition at different length scales using neutron pair distribution function analysis and diffraction data, revealing a dynamic order-disorder nature, and shedding light on previous discrepancies.
- Bo Jiang
- , Jennifer Neu
- & Theo Siegrist
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Anion redox as a means to derive layered manganese oxychalcogenides with exotic intergrowth structures
Low temperature chemical transformations of solids using high-energy intermediates have enabled the synthesis of a new series of layered oxide chalcogenide containing oxidised chalcogenide dimers promising a new range of solids.
- Shunsuke Sasaki
- , Souvik Giri
- & Simon J. Clarke
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Complex phase transitions and phase engineering in the aqueous solution of an isopolyoxometalate cluster
Complex phase transitions including gelation in dilute aqueous solutions of polyanionic clusters ([Mo7O24]6−) in the presence of (Fe(NO3)3) and attributed to the counterion association and overcharging on the clusters, have been identified.
- Zhi-Da Wang
- , Song Liang
- & Hong-Ying Zang
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Boosting the interfacial superionic conduction of halide solid electrolytes for all-solid-state batteries
Compositional tuning is a standard procedure to improve the ionic conductivity of inorganic superionic conductors. Here, the authors report (electro)chemical stable composite halide solid electrolytes applying a nanostructure approach that promotes interfacial superionic conductivity.
- Hiram Kwak
- , Jae-Seung Kim
- & Yoon Seok Jung
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Rapid determination of solid-state diffusion coefficients in Li-based batteries via intermittent current interruption method
The galvanostatic intermittent titration technique (GITT) is the state-of-the-art method for determining the Li+ diffusion coefficients in battery materials. Here, authors propose the intermittent current interruption method as a reliable, accurate and faster alternative to GITT-based methods.
- Yu-Chuan Chien
- , Haidong Liu
- & Matthew J. Lacey
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Real-time insight into the multistage mechanism of nanoparticle exsolution from a perovskite host surface
The separation of nanoparticles from oxide hosts by exsolution forms the basis for catalytic and energy-related applications. Here, the authors elucidate the multistep mechanism of exsolution at perovskite surfaces by combining real-time electron microscopy and computational methods.
- Eleonora Calì
- , Melonie P. Thomas
- & David J. Payne
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Epitaxially grown silicon-based single-atom catalyst for visible-light-driven syngas production
Despite the natural abundance and promising properties of Si, there are few examples of crystalline Si-based catalysts. Here, the authors report an epitaxial growth method to construct Co single atoms on Si for light driven CO2 reduction to syngas.
- Huai Chen
- , Yangyang Xiong
- & Zhenyu Yang
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Understanding the evolution of lithium dendrites at Li6.25Al0.25La3Zr2O12 grain boundaries via operando microscopy techniques
Lithium metal penetration into solid-state electrolytes is a major drawback for developing all-solid-state batteries. Here, authors, via operando force microscopy, demonstrate that the trapping of electrons in garnet-type solid-state electrolyte grain boundaries is the origin of cell failure.
- Chao Zhu
- , Till Fuchs
- & Rüdiger Berger
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Quantification of gas-accessible microporosity in metal-organic framework glasses
Glasses derived from meltable metal-organic frameworks (MOFs) offer great potential for gas separation and solid state ionics. Here, the authors quantify the porosity of a series of MOF glasses by cryogenic carbon dioxide gas sorption and propose design principles for rational tuning the glasses‘ pore size and pore volume.
- Louis Frentzel-Beyme
- , Pascal Kolodzeiski
- & Sebastian Henke
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Unlocking the hidden chemical space in cubic-phase garnet solid electrolyte for efficient quasi-all-solid-state lithium batteries
Conventional compositions of garnet solid electrolytes have limited access to the cubic phase for a high Li content of 7.0, which is beneficial for stability against Li metals. Here, the authors unlock the hidden chemical space via a high entropy strategy, enabling stable long-term battery cycling.
- Sung-Kyun Jung
- , Hyeokjo Gwon
- & Ju-Sik Kim
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Single atom catalysts in Van der Waals gaps
A family of single-atom catalysts synthesized by intercalating metal single atoms into the van der Waals gap of two-dimensional SnS2 is reported. The materials are applied as hydrogen evolving catalysts with good durability and overpotential.
- Huaning Jiang
- , Weiwei Yang
- & Yongji Gong
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Water-stable porous Al24 Archimedean solids for removal of trace iodine
The removal of radioactive elements is important to human health and sustainable development. Here, the authors reveal the synthesis of water-stable Archimedean solids based on the earth-abundant element for the fast removal of trace iodine.
- Ya-Jie Liu
- , Yi-Fan Sun
- & Jian Zhang
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Electrically regulating nonlinear optical limiting of metal-organic framework film
Nonlinear optical properties of metal-organic framework can be tuned for potential optical applications. Here the authors demonstrate an enhancement the nonlinear absorption coefficient of MOF film by applying external electric field.
- Zhi-Zhou Ma
- , Qiao-Hong Li
- & Jian Zhang
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Biferroelectricity of a homochiral organic molecule in both solid crystal and liquid crystal phases
Ferroelectricity normally exists in either solid crystals or liquid crystals. Here, the authors report a homochiral organic compound which shows ferroelectricity in both solid crystal and liquid crystal phases.
- Xian-Jiang Song
- , Xiao-Gang Chen
- & Wei-Qiang Liao
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Synchronous quantitative analysis of chiral mesostructured inorganic crystals by 3D electron diffraction tomography
Chiral mesostructured inorganic crystals exhibit distinctive twisting and helical hierarchical stacking. Here, the authors report a general approach for the synchronous quantitative analysis of rotation axis, torsion angle, pitch length, and arrangement modes.
- Jing Ai
- , Xueliang Zhang
- & Lu Han
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Glassy thermal conductivity in Cs3Bi2I6Cl3 single crystal
The investigation of thermal conductivity is crucial to the success of many modern technologies. Here the authors have reported an unusual glass-like thermal conductivity in a single crystal of layered halide perovskite, Cs3Bi2I6Cl3.
- Paribesh Acharyya
- , Tanmoy Ghosh
- & Kanishka Biswas
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Bromo- and iodo-bridged building units in metal-organic frameworks for enhanced carrier transport and CO2 photoreduction by water vapor
Organolead halide hybrids are promising materials but are often unstable under moisture and/or light irradiation. Here, metal-organic frameworks containing lead halide secondary building units are shown to be stable for photocatalytic CO2 reduction with water vapor.
- Xinfeng Chen
- , Chengdong Peng
- & Honghan Fei
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Large breathing effect in ZIF-65(Zn) with expansion and contraction of the SOD cage
Flexible metal-organic frameworks have potential applications in the development of sensors and switching materials. Here, the authors report a large breathing effect in a zeolitic imidazolate framework upon guest adsorption.
- Meizhen Gao
- , Rui-Kang Huang
- & Jinxiang Dong
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Fundamental investigations on the sodium-ion transport properties of mixed polyanion solid-state battery electrolytes
Battery solid-state electrolytes rely on mixed polyanion networks to attain high ionic conductivities. Here, the authors investigate the effect of polyanion mixing on the solid-state electrolyte ion conductivity via theoretical calculations and electrochemical measurements.
- Zeyu Deng
- , Tara P. Mishra
- & Pieremanuele Canepa
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Development of vanadium-based polyanion positive electrode active materials for high-voltage sodium-based batteries
The development of high-capacity and high-voltage electrode materials can boost the performance of sodium-based batteries. Here, the authors report the synthesis of a polyanion positive electrode active material that enables high-capacity and high-voltage sodium battery performance.
- Semyon D. Shraer
- , Nikita D. Luchinin
- & Stanislav S. Fedotov
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Exploration of glassy state in Prussian blue analogues
Developments in Prussian blue analogues (PBAs) have centred solely on their crystalline state. Here, the authors describe the preparation of the glassy state of PBAs via a mechanically induced crystal-to-glass transformation and explore their properties.
- Nattapol Ma
- , Ryo Ohtani
- & Satoshi Horike
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Deciphering the phase transition-induced ultrahigh piezoresponse in (K,Na)NbO3-based piezoceramics
Functional oxides with coexisting states of comparable energy typically exhibit extraordinary responses to external stimuli. Here, the authors demonstrate that coexisting phase structures provide large electric field-triggered volume change.
- Mao-Hua Zhang
- , Chen Shen
- & Manuel Hinterstein
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Controllable multiple-step configuration transformations in a thermal/photoinduced reaction
Solid-state photochemical reactions of olefinic compounds provide access to organic cyclic molecules with specific configurations but the precise control of the stereochemistry in these reactions remains challenging. Here, the authors demonstrate control of the regiospecific configurations of C=C groups and the intermediates by varying temperatures in multi-step thermal and photoinduced ring opening and closing reactions using a single-crystal coordination polymer platform.
- Meng-Fan Wang
- , Yan Mi
- & Jian-Ping Lang
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Kinetically restrained oxygen reduction to hydrogen peroxide with nearly 100% selectivity
The electrocatalytic oxygen reduction reaction has been investigated in recent years for the production of H2O2 from O2. In this article, the authors report a single-atom rhodium catalyst, based on the Flavin-dependent oxidase, for this transformation.
- Jinxing Chen
- , Qian Ma
- & Shaojun Dong
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Achieving large thermal hysteresis in an anthracene-based manganese(II) complex via photo-induced electron transfer
Achieving magnetic bistability with large thermal hysteresis is still a challenge in material science. Here, the authors report a Mn(II) chain complex that enables light-induced magnetic bistability with a 177 K thermal hysteresis loop.
- Ji-Xiang Hu
- , Qi Li
- & Guo-Ming Wang
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Topotactic fluorination of intermetallics as an efficient route towards quantum materials
Insertion of light elements in intermetallics has been explored to synthesize functional materials. Here the authors report topotactic intercalation of fluorine atoms into intermetallics using a perfluorocarbon reactant with covalent C-F bonds to obtain quantum materials.
- Jean-Baptiste Vaney
- , Baptiste Vignolle
- & Sophie Tencé
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Spatial distribution modulation of mixed building blocks in metal-organic frameworks
Gaining control over the structure of metal organic–frameworks can be challenging. Here the authors report the modulation of the spatial distribution of mixed building blocks in a metal–organic framework from a uniform to a core–shell distribution; temperature control plays a crucial role.
- Seok Jeong
- , Junmo Seong
- & Myoung Soo Lah
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Highly selective cesium(I) capture under acidic conditions by a layered sulfide
The removal of radiocesium from acidic solutions is challenging. Here, the authors report the rapid and highly selective capture of cesium(I) from strongly acidic solutions by a robust layered metal sulfide.
- Jun-Hao Tang
- , Jian-Ce Jin
- & Xiao-Ying Huang
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Fine pore engineering in a series of isoreticular metal-organic frameworks for efficient C2H2/CO2 separation
The separation of acetylene and carbon dioxide by porous materials requires delicate control over the pore size. Herein, the authors fine-tune the pore size at sub-nanometer scale in a series of isoreticular metal-organic frameworks to control the acetylene/carbon dioxide separation performance; subtle structural differences lead to remarkable performance enhancement.
- Jun Wang
- , Yan Zhang
- & Banglin Chen
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Article
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Creation of an unexpected plane of enhanced covalency in cerium(III) and berkelium(III) terpyridyl complexes
Studying how the ligand design influences the bonding of f-block complexes is crucial to control their properties. Here, the authors report the preparation of Bk(III) and Ce(III) complexes featuring a terpyridyl ligand; structural, spectroscopic, electrochemical, and theoretical analysis reveal that the ligand induces unusual bonding by creating a plane of enhanced bond covalency.
- Alyssa N. Gaiser
- , Cristian Celis-Barros
- & Thomas E. Albrecht-Schönzart
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Striping of orbital-order with charge-disorder in optimally doped manganites
Manganite perovskites display the intriguing property of colossal magnetoresistance (CMR), but only at very specific doping values. Now, a detailed crystallographic analysis of a prototype system reveals a novel type of orbital ordering that coexists with charge-disorder stripes, occurring precisely at the doping value where CMR is maximised.
- Wei-Tin Chen
- , Chin-Wei Wang
- & Mark S. Senn
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Giant room temperature electrocaloric effect in a layered hybrid perovskite ferroelectric: [(CH3)2CHCH2NH3]2PbCl4
Most known electrocaloric materials show relatively poor cooling performance near room temperature, hindering their applications. Here, the authors achieve large electrocaloric effect near room temperature in a hybrid perovskite ferroelectric, useful for high-performance solid-state refrigeration.
- Xitao Liu
- , Zhenyue Wu
- & Junhua Luo
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Mixed alkali-ion transport and storage in atomic-disordered honeycomb layered NaKNi2TeO6
Honeycomb layered oxides are an emerging class of materials with peculiar physicochemical properties. Here, the authors report the synthesis and electrochemical energy storage characterisations of a mixed-alkali honeycomb layered oxide material capable of storing Na and K ions simultaneously.
- Titus Masese
- , Yoshinobu Miyazaki
- & Tomohiro Saito
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Atomic-scale unveiling of multiphase evolution during hydrated Zn-ion insertion in vanadium oxide
The detailed understanding of the structural variations during cycling in cathodes for Zn-ion aqueous rechargeable batteries is still limited. Here, the authors utilize atomic-column-resolved scanning transmission electron microscopy to elucidate multiphase evolution during hydrated Zn-Ion insertion in vanadium oxide.
- Pilgyu Byeon
- , Youngjae Hong
- & Sung-Yoon Chung
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Article
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A cost-effective and humidity-tolerant chloride solid electrolyte for lithium batteries
Stable inorganic solid electrolytes are instrumental in developing high-voltage Li metal batteries. Here, the authors present the synthesis and electrochemical energy storage properties of a cost-effective and humidity-tolerant chloride solid electrolyte.
- Kai Wang
- , Qingyong Ren
- & Cheng Ma
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Article
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A chalcogenide-cluster-based semiconducting nanotube array with oriented photoconductive behavior
Interesting properties of carbon nanotubes prompt a search for diverse inorganic nanotubes. Here, the authors report a supertetrahedral chalcogenide cluster-based semiconducting nanotube array that exhibits high electric conductivity and oriented photoconductive behavior.
- Jiaqi Tang
- , Xiang Wang
- & Tao Wu
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Frustrated flexibility in metal-organic frameworks
Responsiveness in metal-organic frameworks involving amorphous phases remains poorly understood. Here, the authors demonstrate MOFs that reversibly switch between well-defined crystalline and structurally degenerate amorphous states mediated by competing intra-framework forces.
- Roman Pallach
- , Julian Keupp
- & Sebastian Henke
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Design of metastable oxychalcogenide phases by topochemical (de)intercalation of sulfur in La2O2S2
Great progress has been made in topochemistry of mobile oxygen anions, but metastable compounds have not yet been achieved by deintercalation of sulfur anions. Here, the authors prepare metastable oxychalcogenide phases by taking advantage of redox-reactive sulfur dimers embedded in a layered oxysulfide.
- Shunsuke Sasaki
- , Maria Teresa Caldes
- & Laurent Cario
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| Open Access
Expanding the chemistry of borates with functional [BO2]− anions
Borates offer extended structural diversity and promise in diverse applications. Here the authors report a borate with linear BO2 units as well as NMR spectroscopy characterization that provides a quantitative basis for identification of BO2 units in polycrystalline and non-crystalline samples.
- Chunmei Huang
- , Miriding Mutailipu
- & Shilie Pan
Two-dimensional lead halide perovskite lateral homojunctions enabled by phase pinning