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A large family of filled skutterudites stabilized by electron count
Skutterudites are a family of materials whose properties make them appealing for studying thermoelectric, magnetic, heavy-fermion and superconducting effects, among many others. Through a combination of theoretical and experimental approaches, this study identifies 43 new skutterudite compounds.
- Huixia Luo
- , Jason W. Krizan
- & Robert J. Cava
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| Open AccessDynamic formation of single-atom catalytic active sites on ceria-supported gold nanoparticles
Computational investigation of heterogeneous catalytic systems is fundamentally important. Here, the authors show that, under reaction conditions, reactant-induced structural changes in ceria-supported gold nanoparticle catalysts lead to the dynamic formation of single-atom catalytic sites at the interface.
- Yang-Gang Wang
- , Donghai Mei
- & Roger Rousseau
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| Open AccessMolecular magnetic switch for a metallofullerene
Endohedral fullerenes are known to stabilize reactive radicals; however, the external magnetic manipulation of these species’ remains challenging. Here, the authors link a nitroxide radical to a paramagnetic fullerene system and are able to alter the spin behaviour of the fullerene via spin–spin interactions.
- Bo Wu
- , Taishan Wang
- & Chunru Wang
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| Open AccessFabrication of three-dimensionally interconnected nanoparticle superlattices and their lithium-ion storage properties
Three-dimensional nanoparticle superlattices are interesting, but their fabrication is generally limited to materials attainable as monodisperse colloidal nanoparticles. Here, the authors fabricate interconnected superlattices via self-assembly without the presynthesis of the constituent nanoparticles.
- Yucong Jiao
- , Dandan Han
- & Angang Dong
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Methane hydrate formation in confined nanospace can surpass nature
Methane hydrates may be one of the largest sources of hydrocarbons on Earth, although demanding temperature–pressure conditions are required for their formation. Here the authors exploit the confinement effects on nanopores to rapidly and reversibly produce methane hydrates under mild conditions.
- Mirian E. Casco
- , Joaquín Silvestre-Albero
- & Francisco Rodríguez-Reinoso
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Edge dislocation slows down oxide ion diffusion in doped CeO2 by segregation of charged defects
Electrochemical devices based on oxide materials, such as batteries or fuel cells, rely on the transport of ions through the crystal lattice. Here, the authors model ion diffusion through CeO2and observe that edge dislocations slow down ion diffusion, contrary to similar processes in metals.
- Lixin Sun
- , Dario Marrocchelli
- & Bilge Yildiz
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A multicentre-bonded [ZnI]8 cluster with cubic aromaticity
Zinc(I) bimetallic clusters have previously been reported, but they are not stable in air. Here, the authors synthesize octametallic Zinc(I) clusters with multi-centred zinc–zinc bonds and extensive electron delocalization over the cluster, resulting in cubic aromaticity and enhanced stability.
- Ping Cui
- , Han-Shi Hu
- & Jun Li
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Self-catalysed aerobic oxidization of organic linker in porous crystal for on-demand regulation of sorption behaviours
Controlling and selectively altering the structure of materials opens up the possibility of modulating their physical properties. Here, the authors report a method for altering the properties of a coordination polymer, where the metal centres active molecular oxygen to oxidize the organic ligand.
- Pei-Qin Liao
- , Ai-Xin Zhu
- & Xiao-Ming Chen
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Strong interactive growth behaviours in solution-phase synthesis of three-dimensional metal oxide nanostructures
It has been suggested that the growth rate of nanocrystals is affected by the size and density of surrounding crystals. Here, the authors study the anisotropic growth of zinc oxide nanorod arrays, and show that rod diameter and height are interdependent, and may be affected by local interactions.
- Jung Min Lee
- , You-Shin No
- & Won Il Park
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| Open AccessCarbon–carbon bond activation of cyclobutenones enabled by the addition of chiral organocatalyst to ketone
Activation of C–C bonds is a powerful method for directly functionalizing organic molecules, but is still a challenging task. Here, the authors show that N-heterocyclic carbenes can activate the C–C bonds in cyclic ketones, allowing the enantioselective formation of lactams.
- Bao-Sheng Li
- , Yuhuang Wang
- & Yonggui Robin Chi
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Evidence for an oxygen evolving iron–oxo–cerium intermediate in iron-catalysed water oxidation
Non-haeme iron complexes are known to be competent catalysts for chemically driven water oxidation. Here, the authors provide evidence for the formation of an inner-sphere iron(IV)- oxygen-cerium(IV) intermediate that may provide mechanistic insight into the naturally occurring oxygen evolving complex.
- Zoel Codolà
- , Laura Gómez
- & Julio Lloret-Fillol
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| Open AccessAn iron-based green approach to 1-h production of single-layer graphene oxide
Oxidants currently used in the preparation of graphene oxide (GO) require long reaction times, relatively high temperatures and costly waste treatment. Here, the authors propose the use of a strong green oxidant, K2FeO4, establishing a fast, safe, toxicity-free route to GO production.
- Li Peng
- , Zhen Xu
- & Chao Gao
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Discovery of optimal zeolites for challenging separations and chemical transformations using predictive materials modeling
Zeolites are industrially important materials, functioning as separation media and catalyst supports. Here, the authors use a large-scale, multi-step computational screening process to identify promising zeolites for challenging separations, namely ethanol purification and alkane adsorption.
- Peng Bai
- , Mi Young Jeon
- & J. Ilja Siepmann
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Stable metal-organic frameworks containing single-molecule traps for enzyme encapsulation
Enzymatic catalytic processes have great industrial potential, although their application is hampered by stability and reuse issues. Here, the authors report metal-organic frameworks with rationally designed single-molecule traps for enzyme encapsulation, and evaluate the activity of the confined enzymes.
- Dawei Feng
- , Tian-Fu Liu
- & Hong-Cai Zhou
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| Open AccessPorous coordination polymers with ubiquitous and biocompatible metals and a neutral bridging ligand
Inexpensive porous materials synthesized from Group II metals may be useful for industrial applications. Here, the authors demonstrate that neutral bridging ligands can be used for the synthesis of magnesium(II) and calcium(II) porous coordination polymers.
- Shin-ichiro Noro
- , Junya Mizutani
- & Takayoshi Nakamura
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| Open AccessAn efficient molybdenum disulfide/cobalt diselenide hybrid catalyst for electrochemical hydrogen generation
There is substantial research into new catalysts for electroreduction of water. Here, the authors report a robust and active molybdenum disulfide/cobalt diselenide hydrogen evolution catalyst with onset potential of 11 mV and Tafel slope of 36 mV per decade, approaching the activity of platinum.
- Min-Rui Gao
- , Jin-Xia Liang
- & Shu-Hong Yu
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Tandem intercalation strategy for single-layer nanosheets as an effective alternative to conventional exfoliation processes
The synthesis of single-layer transition metal chalcogenides (TMCs) is desirable, but challenging. Here, the authors propose a new exfoliation method, wherein single-layer TMCs are produced via a one-pot tandem molecular intercalation approach.
- Sohee Jeong
- , Dongwon Yoo
- & Jinwoo Cheon
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| Open AccessA ferromagnetically coupled Fe42 cyanide-bridged nanocage
One area of interest in the field of molecular magnetism is the development of high-spin molecules. Here, the authors report a cyanide-bridged nanocage consisting of 18 high-spin iron(III) ions ferromagnetically coupled through 24 low-spin iron(II) ions, with a ground state spin of S=45.
- Soonchul Kang
- , Hui Zheng
- & Osamu Sato
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RETRACTED ARTICLE: Reduction of carbon dioxide to oxalate by a binuclear copper complex
Although value-added organics are traditionally synthesized from fossil feedstocks, the conversion of carbon dioxide is an attractive alternative route. Here, the authors report a cyclic copper complex capable of converting carbon dioxide to oxalate in a simple redox process under mild conditions.
- Uttam R. Pokharel
- , Frank R. Fronczek
- & Andrew W. Maverick
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Bottom-up formation of endohedral mono-metallofullerenes is directed by charge transfer
An understanding of the formation mechanism of endohedral metallofullerenes may pave the way towards targeted synthesis of these nanomaterials. Here, the authors investigate their bottom-up synthesis and determine that charge transfer plays a key role in their formation.
- Paul W. Dunk
- , Marc Mulet-Gas
- & Harold W. Kroto
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Interstitial modification of palladium nanoparticles with boron atoms as a green catalyst for selective hydrogenation
Lindlar catalysts are widely used for partial hydrogenation of alkynes, however they can be somewhat limited by toxicity of lead and low selectivity. Here, the authors report that the modification of palladium nanoparticles with boron atoms in the interstitial sites yields selective hydrogenation catalysts.
- Chun Wong Aaron Chan
- , Abdul Hanif Mahadi
- & Shik Chi Edman Tsang
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Crystallographic and spectroscopic characterization and reactivities of a mononuclear non-haem iron(III)-superoxo complex
Non-haem iron superoxo species—proposed as key intermediates in catalytic activation of molecular oxygen—have proven difficult to structurally characterize. Here, the authors obtain crystallographic and spectral characterization of a non-haem iron(III)-superoxo species and subsequently study its reactivity.
- Seungwoo Hong
- , Kyle D. Sutherlin
- & Wonwoo Nam
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Effectively suppressing dissolution of manganese from spinel lithium manganate via a nanoscale surface-doping approach
Dissolution of manganese from the cathode in lithium manganate based batteries is a major cause for the capacity decay. Here, the authors show a nanoscale surface-doping approach to mitigate the problem and to improve the battery capacity and cycleability.
- Jun Lu
- , Chun Zhan
- & Khalil Amine
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Kinetically tuned dimensional augmentation as a versatile synthetic route towards robust metal–organic frameworks
The synthesis of ultra-stable, single crystalline metal–organic frameworks is challenging. Here, the authors describe a kinetically tuned augmentation synthetic route for the preparation of a range of robust crystalline materials from preformed trimetallic components.
- Dawei Feng
- , Kecheng Wang
- & Hong-Cai Zhou
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Photon energy upconversion through thermal radiation with the power efficiency reaching 16%
Energy transfer upconversion can increase the absorption efficiency but has been limited by multiphonon relaxation. Here, Wang et al. demonstrate that photon energy upconversion by thermal radiation benefits from multiphonon relaxation and achieves efficiencies as high as 16%.
- Junxin Wang
- , Tian Ming
- & Chun-Hua Yan
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Mercury nano-trap for effective and efficient removal of mercury(II) from aqueous solution
Decontamination of mercury pollution from fresh water is a serious environmental issue. Here, the authors report a porous organic polymer-based nano-trap, functionalized with mercury chelating groups, capable of efficient and rapid mercury removal from aqueous media.
- Baiyan Li
- , Yiming Zhang
- & Shengqian Ma
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General incorporation of diverse components inside metal-organic framework thin films at room temperature
General methods to introduce functional components into metal-organic frameworks are challenging to develop. Here, the authors report a method for encapsulating a range of functional components, such as proteins and nanoparticles, into the structures with properties dependent on both the framework and the guest.
- Yiyin Mao
- , Junwei Li
- & Xinsheng Peng
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High lithium anodic performance of highly nitrogen-doped porous carbon prepared from a metal-organic framework
Nitrogen-doped graphene can be used for lithium storage, but the nitrogen content is often quite low. Here, the authors synthesize graphene analogous with high nitrogen content using a zeolitic imidazolate framework, which show exceptional battery performances.
- Fangcai Zheng
- , Yang Yang
- & Qianwang Chen
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A heavy analogue of the smallest bridgehead alkene stabilized by a base
The highly strained nature of small bridgehead alkenes means that they often cannot be isolated, despite being postulated as transient intermediates. Here, the authors report base-stabilized heavy analogues of the smallest bridgehead alkene, with silicon occupying the vertices.
- Takeaki Iwamoto
- , Naohiko Akasaka
- & Shintaro Ishida
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| Open AccessQuantum signatures of a molecular nanomagnet in direct magnetocaloric measurements
The magnetocaloric effect is well understood in spin-frustrated low-dimensional systems, and should be observable in certain high-symmetry molecular structures. Here, the authors report the experimental observation of sub-Kelvin cooling with a molecular magnet, and probe the low-temperature spin behaviour.
- Joseph W. Sharples
- , David Collison
- & Marco Evangelisti
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Direct measurement of dysprosium(III)˙˙˙dysprosium(III) interactions in a single-molecule magnet
Modelling magnetic data for lanthanide clusters is challenging due to spin–orbit coupling and crystal field effects. Here, the authors use multi-frequency electron paramagnetic resonance spectroscopy to measure directly the interaction between two dysprosium(III) ions in a dimeric system.
- Eufemio Moreno Pineda
- , Nicholas F. Chilton
- & Richard E.P. Winpenny
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| Open AccessA hybrid absorption–adsorption method to efficiently capture carbon
Common approaches for carbon dioxide capture include absorption in amine solutions or adsorption in porous materials. Here, the authors combine these two strategies and report carbon dioxide capture in a slurry of metal-organic frameworks in glycol-2-methylimidazole, which has advantages of both techniques.
- Huang Liu
- , Bei Liu
- & Wenchuan Wang
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Efficient selective and atom economic catalytic conversion of glycerol to lactic acid
Lactic acid is a platform chemical with a variety of applications that is produced and used on a large scale. Here, the authors convert glycerol—a by-product of biodiesel production—into lactic acid in a highly efficient, homogenous catalytic process.
- Liam S. Sharninghausen
- , Jesús Campos
- & Robert H. Crabtree
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Colossal positive and negative thermal expansion and thermosalient effect in a pentamorphic organometallic martensite
The thermosalient effect is the unusual tendency of some crystals to visibly jump during phase changes. Here, the authors study the multiple phase changes in a prototypic thermosalient material and provide evidence for the factors that drive this self-actuation.
- Manas K. Panda
- , Tomče Runčevski
- & Panče Naumov
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Photoinitiated charge separation in a hybrid titanium dioxide metalloporphyrin peptide material
Peptides can be used as templates for the synthesis of dye-sensitised semiconducting materials. Here, the authors design two peptides that give excellent and sequence specific control over the spatial arrangement of the semiconducting materials with respect to the dye molecule.
- H. Christopher Fry
- , Yuzi Liu
- & Tijana Rajh
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| Open AccessA metal–ion-responsive adhesive material via switching of molecular recognition properties
While common adhesives stick indiscriminately to surfaces, there are many potential applications for smart adhesives that stick to specific surfaces only under certain conditions. Here, the authors report a polymer hydrogel as a functional adhesive material which responds to chemical stimulation by metal ions.
- Takashi Nakamura
- , Yoshinori Takashima
- & Akira Harada
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Polyoxometalate-mediated electron transfer–oxygen transfer oxidation of cellulose and hemicellulose to synthesis gas
Cellulose and hemicellulose are some of the most abundant naturally occurring organic materials, presenting a highly attractive target for energy production. Here, the authors use a polyoxometalate system to convert these materials directly to carbon monoxide and hydrogen gas.
- Bidyut Bikash Sarma
- & Ronny Neumann
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Accelerated discovery of cathode materials with prolonged cycle life for lithium-ion battery
A long cycle life of batteries is critical for efficiently utilizing renewable energy sources. Here, the authors use a computer screening approach to search for potential cathodes for lithium ion batteries, and present a co-substituted lithium iron phosphate cathode with promising cycling performance.
- Motoaki Nishijima
- , Takuya Ootani
- & Isao Tanaka
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Designed synthesis of large-pore crystalline polyimide covalent organic frameworks
Covalent organic frameworks are a potentially useful class of materials, although they are currently synthesized using relatively few reactions. Here, the authors show that the imidization reaction can be used to prepare a series of large pore polyimide frameworks with high surface area and thermal stability.
- Qianrong Fang
- , Zhongbin Zhuang
- & Yushan Yan
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Exfoliation of layered double hydroxides for enhanced oxygen evolution catalysis
The search for efficient catalysts for the oxygen evolution reaction is ongoing. Here, the authors show that liquid exfoliation of layered double hydroxides yields single-layer nanosheets with enhanced catalytic activity, attributed to the more numerous active sites and increased electronic conductivity.
- Fang Song
- & Xile Hu
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Engineering chiral porous metal-organic frameworks for enantioselective adsorption and separation
The separation of chiral molecules is a fundamental and industrially relevant challenge. Here, the authors report a chiral metal-organic framework that functions as a solid-state host capable of absorbing and separating mixtures of a range of chiral amines, with high enatioselectivity.
- Yongwu Peng
- , Tengfei Gong
- & Yong Cui
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| Open AccessA critical analysis of calcium carbonate mesocrystals
The term mesocrystal describes three-dimensional crystals formed by oriented assembly and that exhibit nanoparticle substructures. Here, the authors perform detailed structural analyses on synthetic calcium carbonate/polymer crystals, and show that common signatures used to assign mesocrystals may be unreliable.
- Yi-Yeoun Kim
- , Anna S. Schenk
- & Fiona C. Meldrum
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Fluorocarbon adsorption in hierarchical porous frameworks
Fluorocarbons are industrially important chemicals and materials for their adsorption and separation have applications in refrigeration and environmental technologies. Here, the authors investigate the adsorption behaviour of fluorocarbons on a series of metal-organic frameworks.
- Radha Kishan Motkuri
- , Harsha V. R. Annapureddy
- & Praveen K. Thallapally
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Highly efficient non-rare-earth red emitting phosphor for warm white light-emitting diodes
Manganese-activated fluoride phosphors for high-efficacy warm white light-emitting diodes have been limited by low photoluminescence quantum yields. Here, Zhu et al.use an efficient cation exchange reaction to synthesize manganese phosphors with photoluminescence quantum yields as high as 98%.
- Haomiao Zhu
- , Chun Che Lin
- & Xueyuan Chen
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Enantioselective control of lattice and shape chirality in inorganic nanostructures using chiral biomolecules
Inorganic structured nanomaterials with chiral symmetry groups may have interesting optical activities. Here, the authors use biomolecules to synthesize chiral tellurium and selenium nanostructures, which exhibit visible optical and chiroptical responses and may be used as templates for mixed metal structures.
- Assaf Ben-Moshe
- , Sharon Grayer Wolf
- & Gil Markovich
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Electrochemical tuning of layered lithium transition metal oxides for improvement of oxygen evolution reaction
Lithium cobalt oxide is widely studied for electrocatalytic applications. Here, the authors develop a technique for delithiating the material in organic electrolyte, and demonstrate that the oxygen evolution catalytic activity is significantly improved after the treatment.
- Zhiyi Lu
- , Haotian Wang
- & Yi Cui
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Giant negative linear compression positively coupled to massive thermal expansion in a metal–organic framework
Negative linear compressibility in materials is usually accompanied by a thermal contraction upon heating. Here, the authors report a metal organic framework that breaks this rule, exhibiting large intrinsic negative linear compressibility coinciding with strong positive thermal expansion.
- Weizhao Cai
- & Andrzej Katrusiak
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Origin of slow magnetic relaxation in Kramers ions with non-uniaxial anisotropy
Transition metal ions with long-lived spin states represent the minimum size magnetic bit. Here, the authors study the spin–lattice relaxation of a cobalt(II) complex and demonstrate the role of time-reversal symmetry that hinders direct spin–phonon processes regardless of the sign of the magnetic anisotropy.
- Silvia Gómez-Coca
- , Ainhoa Urtizberea
- & Fernando Luis
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| Open AccessFacile scission of isonitrile carbon–nitrogen triple bond using a diborane(4) reagent
The cleavage of triple bonds can be achieved through the use of transition metal catalysts; however, it is less well explored for metal-free systems. Here, the authors show complete cleavage of a carbon–nitrogen triple bond under mild conditions through the use of a diborane(4) reagent.
- Hiroki Asakawa
- , Ka-Ho Lee
- & Makoto Yamashita