Featured
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Article
| Open AccessExpanding 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
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Article
| Open AccessUnderstanding contact electrification at liquid–solid interfaces from surface electronic structure
Understanding contact electrification within the liquid–solid interface is critical for further applications in energy conversion and storage devices. Here, the authors reveal liquid–solid interactions regarding the charge transfer mechanism and pinning factor from the electronic perspective.
- Mingzi Sun
- , Qiuyang Lu
- & Bolong Huang
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Article
| Open AccessProbing electronic structure in berkelium and californium via an electron microscopy nanosampling approach
The obtention and study of actinide elements is challenging due to various factors including their radioactivity and scarcity. Herein, the authors characterize the atomic and electronic structure of Am, Cm, Bk, and Cf compounds using a transmission electron microscopy-based workflow that only requires nanogram amounts of the actinide element.
- Alexander Müller
- , Gauthier J.-P. Deblonde
- & Andrew M. Minor
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Article
| Open AccessFacile electron delivery from graphene template to ultrathin metal-organic layers for boosting CO2 photoreduction
While solar-to-fuel energy conversion is appealing, materials require accessible active sites for reactants and rapid electron transfer steps. Here, authors support ultrathin metal-organic layers with graphene oxide as both template and electron mediator to boost CO2 photoreduction performance.
- Jia-Wei Wang
- , Li-Zhen Qiao
- & Tong-Bu Lu
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Article
| Open AccessA combinatory ferroelectric compound bridging simple ABO3 and A-site-ordered quadruple perovskite
There are few reports of ferroelectricity due to symmetry breaking transition in A-site-ordered quadruple perovskites. Here, the authors find one with phase transition from a high-temperature centrosymmetric paraelectric phase to a low-temperature non-centrosymmetric ferroelectric phase in a high pressure synthesized compound.
- Jianfa Zhao
- , Jiacheng Gao
- & Changqing Jin
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Article
| Open AccessPreparation of iron(IV) nitridoferrate Ca4FeN4 through azide-mediated oxidation under high-pressure conditions
High-valent metal nitrides are difficult to stabilise due to the high thermodynamic stability and chemical inertness of N2. Here, the authors employ a large volume press to prepare an iron(IV) nitridoferrate Ca4FeIVN4 from Fe2N and Ca3N2 via azide-mediated oxidation under high pressure conditions.
- Simon D. Kloß
- , Arthur Haffner
- & J. Paul Attfield
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Article
| Open AccessNon-equilibrium metal oxides via reconversion chemistry in lithium-ion batteries
The charging of Fe and Mn oxide anodes in lithium-ion batteries are believed to form rocksalt phases via reconstructive conversion reactions. Here, the authors show that MxOy (M = Fe, Mn) transform into non-native body-centred cubic FeO and zincblende MnO via topotactic displacement-like pathways.
- Xiao Hua
- , Phoebe K. Allan
- & Andrew L. Goodwin
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Article
| Open AccessLi1.5La1.5MO6 (M = W6+, Te6+) as a new series of lithium-rich double perovskites for all-solid-state lithium-ion batteries
The development of the all solid-state battery requires the formation of stable solid/solid interfaces between different battery components. Here the authors tailor the composition to form both electrolyte and anode from the same novel family of perovskites with shared crystal chemistry.
- Marco Amores
- , Hany El-Shinawi
- & Edmund J. Cussen
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Article
| Open AccessHigh pressure synthesis of phosphine from the elements and the discovery of the missing (PH3)2H2 tile
Chemical elements at high pressure may behave more consistently with their periodic properties than they do at ambient conditions. The authors report the synthesis of PH3 from black phosphorous and hydrogen, and the crystallization of the van der Waals compound (PH3)2H2 which fills a gap in the chemistry of adjacent elements in the periodic table.
- Matteo Ceppatelli
- , Demetrio Scelta
- & Maurizio Peruzzini
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Article
| Open AccessStrain-induced creation and switching of anion vacancy layers in perovskite oxynitrides
Properties of perovskite oxides can be changed by manipulating anion-vacancy order patterns, but they are difficult to control. Here the authors show strain-induced creation and switching of anion vacancies in perovskite films in which the direction or periodicity of anion-vacancy planes is altered depending on the substrate employed.
- Takafumi Yamamoto
- , Akira Chikamatsu
- & Hiroshi Kageyama
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Article
| Open Access99TcO4− removal from legacy defense nuclear waste by an alkaline-stable 2D cationic metal organic framework
Separation of 99TcO4− from nuclear waste at the Savannah River Site is hampered by the extreme conditions. Here, the authors propose a solution by developing an alkaline-resistant metal organic framework material featuring unique recognition sites for selective incorporation of 99TcO4− anions.
- Nannan Shen
- , Zaixing Yang
- & Shuao Wang
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Article
| Open AccessUnravelling the room-temperature atomic structure and growth kinetics of lithium metal
Atomic structure of alkali metal is difficult to be revealed at room temperature because of the chemical reactivity and irradiation sensitivity. Here the authors show that electron beam-induced in situ growth of alkali metals enables the investigation of atomic structure and growth kinetics at high spatiotemporal resolution.
- Chao Liang
- , Xun Zhang
- & Yi Yu
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Article
| Open AccessRationally designed transition metal hydroxide nanosheet arrays on graphene for artificial CO2 reduction
The development of effective, earth-abundant cocatalysts is critical for photocatalytic CO2 reduction. Here, authors report the assembly of transition metal hydroxides on graphene to act as cocatalyst ensembles for efficient CO2 photoreduction.
- Kang-Qiang Lu
- , Yue-Hua Li
- & Yi-Jun Xu
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Article
| Open AccessStabilizing a metalloid {Zn12} unit within a polymetallide environment in [K2Zn20Bi16]6−
Low-valent zinc clusters, though exceedingly rare, are appealing synthetic targets because there is evidence that they may show unconventional chemical and physical behavior. Here, the authors obtain a large heterometallic zinc-bismuth cluster anion and discover that it bears a metalloid {Zn12} core with four-center bonding and essentially zero-valent character.
- Armin R. Eulenstein
- , Yannick J. Franzke
- & Stefanie Dehnen
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Review Article
| Open AccessSolid state chemistry for developing better metal-ion batteries
The development of high performing metal-ion batteries require guidelines to build improved electrodes and electrolytes. Here, the authors review the current state-of-the-art in the rational design of battery materials by exploiting the interplay between composition, crystal structure and electrochemical properties.
- Artem M. Abakumov
- , Stanislav S. Fedotov
- & Jean-Marie Tarascon
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Article
| Open AccessModulated structure determination and ion transport mechanism of oxide-ion conductor CeNbO4+δ
Materials with oxygen hyperstoichiometry received great attention in solid oxide fuel cells field because of the low activation energy of interstitial ion migration. Here the authors revealed the relationship between the structure and oxide ion migration for the whole series of CeNbO4+δ compounds.
- Jian Li
- , Fengjuan Pan
- & Junliang Sun
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Article
| Open AccessA family of lead clusters with precious metal cores
Many Zintl ions with a single endohedrally encapsulated transition metal ion are known, but relatively few where clusters of two or more metals are present. Here, the authors report the synthesis and characterization of two clusters, [Au8Pb33]6− and [Au12Pb44]12−, which contain Au8 and Au12 cores surrounded by Pb shells.
- Cong-Cong Shu
- , Harry W. T. Morgan
- & Zhong-Ming Sun
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Article
| Open AccessMolecule-based nonlinear optical switch with highly tunable on-off temperature using a dual solid solution approach
Switching of nonlinear optical signals is attractive for photoelectronics and photonics, but development is hindered by a lack of control over the switch temperature. Here the authors report a coordination polymer system that serves as an alloy-like nonlinear optical switch with a tunable switch temperature.
- Shi-Yong Zhang
- , Xia Shu
- & Xiao-Ming Chen
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Article
| Open AccessBlack indium oxide a photothermal CO2 hydrogenation catalyst
The utilization of white-colored, wide-bandgap CO2 hydrogenation photocatalysts has been hindered by their limited light-harvesting ability. By making stoichiometric white indium oxide non-stoichiometric and black, it is transformed from a highly inactive to a highly active photothermal catalyst.
- Lu Wang
- , Yuchan Dong
- & Geoffrey A. Ozin
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Article
| Open AccessLattice distortion induced internal electric field in TiO2 photoelectrode for efficient charge separation and transfer
The driving force for charge transfer in photoelectrochemical systems is typically derived from band bending at a surface-electrolyte interface. In this work, battery-type lithiation of TiO2 generates a built-in electric field in the bulk material, giving a 750% enhancement in photocurrent density.
- Yuxiang Hu
- , Yuanyuan Pan
- & Lianzhou Wang
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Article
| Open AccessDirect evidence of boosted oxygen evolution over perovskite by enhanced lattice oxygen participation
While water splitting provides a renewable means to store energy, the sluggish O2 evolution half-reaction limits applications. Here, authors examine a silicon-incorporated strontium cobaltite perovskite and correlate lattice oxygen participation in O2 evolution to the oxygen ion diffusivity.
- Yangli Pan
- , Xiaomin Xu
- & Zongping Shao
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Article
| Open AccessMacroscopic Polarization Change via Electron Transfer in a Valence Tautomeric Cobalt Complex
Polarization change from directional electron transfer attracts considerable attention owing to its fast switching rate and potential light control. Here, the authors provide a proof-of-concept of electronic pyroelectricity induced by intramolecular electron transfer in the single crystal of a valence tautomeric compound.
- Shu-Qi Wu
- , Meijiao Liu
- & Osamu Sato
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Article
| Open AccessSolid solution for catalytic ammonia synthesis from nitrogen and hydrogen gases at 50 °C
Ammonia synthesis via the Haber–Bosch process typically takes place at an elevated temperature in order to achieve a reasonable rate. Here the authors report on a CaFH solid solution with low activation energy for catalytic ammonia synthesis at lower temperatures.
- Masashi Hattori
- , Shinya Iijima
- & Michikazu Hara
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Article
| Open AccessSelf-sustainable protonic ceramic electrochemical cells using a triple conducting electrode for hydrogen and power production
While producing renewable fuel is crucial for a sustainable energy economy, there is still a need for active and durable materials capable of efficient fuel generation and utilization. Here, authors demonstrate a triple-conductive oxide as an oxygen electrode for H2 or electricity production.
- Hanping Ding
- , Wei Wu
- & Dong Ding
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Article
| Open AccessSite-selective doping of ordered charge states in magnetite
Charge ordering in magnetite is an important example of the complex behaviour that emerges in transition metal oxides. Here the authors show that doping causes selective oxidation of one site in the established trimeron pattern, introducing an additional charge-ordered structure.
- E. Pachoud
- , J. Cumby
- & J. P. Attfield
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Review Article
| Open AccessA reflection on lithium-ion battery cathode chemistry
The 2019 Nobel Prize in Chemistry has been awarded to a trio of pioneers of the modern lithium-ion battery. Here, Professor Arumugam Manthiram looks back at the evolution of cathode chemistry, discussing the three major categories of oxide cathode materials with an emphasis on the fundamental solid-state chemistry that has enabled these advances.
- Arumugam Manthiram
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Article
| Open AccessIntroducing the crystalline phase of dicalcium phosphate monohydrate
Understanding the crystal structure of different calcium phosphates is important for a range of different subjects from geology to biomedicine. Here, the authors report on the synthesis and determination of the crystal structure of dicalcium phosphate monohydrate.
- Bing-Qiang Lu
- , Tom Willhammar
- & Denis Gebauer
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Article
| Open AccessDirect observation of nuclear reorganization driven by ultrafast spin transitions
Electron spin is a fundamental property of molecules, and changes in spin state affect both molecular structure and dynamics. Here, the authors resolve, by ultrafast electron diffraction, the nuclear reorganization stabilizing spin transitions in a [FeII(bpy)3](PF6)2 crystal.
- Yifeng Jiang
- , Lai Chung Liu
- & R. J. Dwayne Miller
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Article
| Open AccessTitanium-based potassium-ion battery positive electrode with extraordinarily high redox potential
The Ti4+/Ti3+ redox couple is usually a good choice for anodes due to its low potential. Here, the authors show that the potential can be increased to nearly 4.0 V in KTiPO4F, which serves as a high-performance cathode for K-ion batteries.
- Stanislav S. Fedotov
- , Nikita D. Luchinin
- & Evgeny V. Antipov
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Article
| Open AccessAmorphization activated ruthenium-tellurium nanorods for efficient water splitting
Elctrochemical water splitting is of vital significance for energy conversion and storage. Here the authors show an electrocatalyst based on amorphous ruthenium-tellurium porous nanorods which exhibit significantly improved OER performance than its crystalline counterparts
- Juan Wang
- , Lili Han
- & Xiaoqing Huang
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Article
| Open AccessUnsupervised discovery of solid-state lithium ion conductors
Predictions of new solid-state Li-ion conductors are challenging due to the diverse chemistries and compositions involved. Here the authors combine unsupervised learning techniques and molecular dynamics simulations to discover new compounds with high Li-ion conductivity.
- Ying Zhang
- , Xingfeng He
- & Chen Ling
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Article
| Open AccessDivalent europium-doped near-infrared-emitting phosphor for light-emitting diodes
Here the authors report a near-infrared K3LuSi2O7:Eu2+ phosphor for non-visible light source application. The selective site occupation of Eu2+ in LuO6 and K2O6 polyhedrons is found to be responsible for the light emission and these insights could serve as design principles for discovery and design of such phosphors.
- Jianwei Qiao
- , Guojun Zhou
- & Zhiguo Xia
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Article
| Open AccessMetallic porous nitride single crystals at two-centimeter scale delivering enhanced pseudocapacitance
Metallic porous nitride single crystals combine the advantages of large surface area, high conductivity and active sites at twisted surfaces. Here the authors grow metallic porous nitride single crystals at 2-cm scale, and demonstrate enhanced pseudocapacitance and cycling stability.
- Shaobo Xi
- , Guoming Lin
- & Kui Xie
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Article
| Open AccessSynthesis of magnesium-nitrogen salts of polynitrogen anions
Polynitrogen compounds are potentially promising high energy density materials, but are difficult to synthesize due to their instability. Here, the authors observe the formation, under high pressure, of a Mg2N4 magnesium–tetranitrogen salt which remains stable at ambient conditions.
- Dominique Laniel
- , Bjoern Winkler
- & Natalia Dubrovinskaia
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Article
| Open AccessMagnetoelectric behavior via a spin state transition
Magnetoelectric effect enables versatile electronic and spintronic devices. Here the authors demonstrate a different strategy to achieve magnetoelectric coupling in which the electric polarization is controlled by magnetic spin state transition instead of the traditional ferro- or antiferromagnetic order.
- Shalinee Chikara
- , Jie Gu
- & Vivien S. Zapf
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Article
| Open AccessTowards general network architecture design criteria for negative gas adsorption transitions in ultraporous frameworks
Porous framework material DUT-49 was recently demonstrated to exhibit a unique counterintuitive negative gas adsorption (NGA) behaviour. Here the authors identify framework DUT-50 as an additional pressure amplifying material that features distinct NGA transitions, and suggest structural design criteria to access other such materials.
- Simon Krause
- , Jack D. Evans
- & Stefan Kaskel
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Article
| Open AccessPorous single-crystalline titanium dioxide at 2 cm scale delivering enhanced photoelectrochemical performance
Porous single crystals in large size can significantly enhance their functionality owing to the structural coherence and large surface area. Here the authors show porous single-crystalline titanium dioxide based photoelectrodes with large dimensions leading to improved photoelectrochemical performance.
- Fangyuan Cheng
- , Guoming Lin
- & Kui Xie
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Article
| Open AccessConstruction of stabilized bulk-nano interfaces for highly promoted inverse CeO2/Cu catalyst
Cu-CeO2 has been considered as promising alternative to Cu-Zn-Al catalyst for water-gas shift (WGS) reaction, but it still suffers from low activity caused by Cu sintering. Here, the authors develop inverse CeO2/Cu catalyst with remarkable activity and stability in WGS via construction of stabilized bulk-nano interfaces.
- Han Yan
- , Chun Yang
- & Chun-Jiang Jia
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Article
| Open AccessPolyhydride CeH9 with an atomic-like hydrogen clathrate structure
Obtainment of hydrogen-rich metal hydrides that are high-temperature superconductors has been demonstrated under very high pressure, but is still largely unexplored. Here the authors synthesize CeH9, with a structure related to solid metallic hydrogen, at relatively low pressure and without need for heating.
- Xin Li
- , Xiaoli Huang
- & Tian Cui
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Article
| Open AccessHigh-pressure synthesis of ultraincompressible hard rhenium nitride pernitride Re2(N2)(N)2 stable at ambient conditions
High pressure experiments may yield materials with unusual combinations of properties, but typically in small amounts and unstable. Here the authors synthesize millimeter-sized samples of metallic, ultraincompressible and very hard rhenium nitride pernitride, recoverable at ambient conditions.
- Maxim Bykov
- , Stella Chariton
- & Leonid Dubrovinsky
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Article
| Open AccessPenta- and hexa-coordinated beryllium and phosphorus in high-pressure modifications of CaBe2P2O8
Beryllium in inorganic compounds is usually coordinated to four oxygen atoms, but higher coordination numbers have been predicted. Here the authors observe a pressure induced stepwise transition in CaBe2P2O8 where Be coordination changes to trigonal-bipyramidal and octahedral, implying that d orbitals are not mandatory for high coordination.
- Anna Pakhomova
- , Georgios Aprilis
- & Leonid Dubrovinsky
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Article
| Open AccessEmbedding laser generated nanocrystals in BiVO4 photoanode for efficient photoelectrochemical water splitting
While photoelectrochemical water splitting offers a low-cost, integrated means to generate fuel from light, poor charge carrier transport limits performances. Here, authors embed laser-synthesized colloids in bismuth vanadate photoanodes to boost charge carrier mobilities and enhance photocurrents.
- Jie Jian
- , Youxun Xu
- & Hongqiang Wang
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Article
| Open AccessNickel@Siloxene catalytic nanosheets for high-performance CO2 methanation
There is a strong push to develop new catalysts and supports to convert low-value CO2 into high-value CH4. Here, authors found that the internal or external confinement of Ni on multi-layered siloxene supports determined the reaction pathway, activity, selectivity, and stability in CO2 methanation.
- Xiaoliang Yan
- , Wei Sun
- & Geoffrey A. Ozin
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Article
| Open AccessCharacteristic fast H− ion conduction in oxygen-substituted lanthanum hydride
Hydride ions are promising for energy storage since they are abundant, lightweight, and highly mobile, but ionic conductivity should be improved. Here the authors achieve fast hydride ion conductivity in a mixed-anion compound by tuning oxygen content.
- Keiga Fukui
- , Soshi Iimura
- & Hideo Hosono
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Article
| Open AccessNa-doped ruthenium perovskite electrocatalysts with improved oxygen evolution activity and durability in acidic media
While water splitting may afford a renewable means to store energy in chemical bonds, water oxidation catalysts suffer from poor stabilities in acidic media. Here, authors show sodium doping of strontium ruthenate to improve the catalytic durability while maintaining a high O2 evolution activity.
- María Retuerto
- , Laura Pascual
- & Sergio Rojas
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Article
| Open AccessSr[Li2Al2O2N2]:Eu2+—A high performance red phosphor to brighten the future
Developing innovative materials for reduced energy consumption in phosphor converted white light-emitting diodes remains a challenge. Here, the authors report a narrow band red-emitting oxonitride material with a highly symmetrical Sr2 + coordination for energy efficient white light-emitting diodes.
- Gregor J. Hoerder
- , Markus Seibald
- & Hubert Huppertz
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Article
| Open AccessSelective photoelectrochemical oxidation of glycerol to high value-added dihydroxyacetone
The selective conversion of inexpensive precursors to high-value chemicals presents valuable academic and industrial consequences. Here, the authors show bismuth vanadate photoanodes to utilize light and photoelectrochemically oxidize glycerol selectively to valuable industrial products.
- Dong Liu
- , Jin-Cheng Liu
- & Bin Liu
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Article
| Open AccessSingle platinum atoms embedded in nanoporous cobalt selenide as electrocatalyst for accelerating hydrogen evolution reaction
While water splitting chemistry provides a renewable means to produce carbon-neutral hydrogen fuel, the most efficient catalysts require rare and expensive platinum. Here, authors prepare single-atom platinum on cobalt selenide as a high-performance hydrogen evolution electrocatalyst.
- Kang Jiang
- , Boyang Liu
- & Yongwen Tan
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Article
| Open AccessBoosting oxygen evolution of single-atomic ruthenium through electronic coupling with cobalt-iron layered double hydroxides
While water splitting offers a carbon-neutral means to store energy, water oxidation is sluggish and corrosive over earth-abundant electrocatalysts. Here, authors show single ruthenium atoms over cobalt-iron layered double hydroxides to be effective and stable oxygen evolution electrocatalysts.
- Pengsong Li
- , Maoyu Wang
- & Xiaoming Sun