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| Open AccessDirect oxygen isotope effect identifies the rate-determining step of electrocatalytic OER at an oxidic surface
Understanding reaction mechanisms is crucial for catalyst design. Here, natural-abundance isotope quantifications of O2 yield mechanistically significant reaction kinetic isotope effects for water oxidation over metal oxide electrodes, the bottleneck step of water electrolysis.
- Sandra Haschke
- , Michael Mader
- & Julien Bachmann
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Article
| Open AccessAtomic cobalt as an efficient electrocatalyst in sulfur cathodes for superior room-temperature sodium-sulfur batteries
Room-temperature sodium-sulfur batteries hold promise, but are hindered by low reversible capacity and fast capacity fade. Here the authors construct a multifunctional sulfur host comprised of cobalt-decorated carbon nanospheres that impart attractive performance as a cathode in a sodium sulfide battery.
- Bin-Wei Zhang
- , Tian Sheng
- & Shi-Xue Dou
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Article
| Open AccessA fully protected hydrogenase/polymer-based bioanode for high-performance hydrogen/glucose biofuel cells
Hydrogenases are promising alternatives to noble metal-based catalysts for hydrogen oxidation. Here the authors fully protect air-sensitive hydrogenases from high potential and oxygen damage using a polymer multilayer bioanode in a biofuel cell that delivers a benchmark open circuit voltage.
- Adrian Ruff
- , Julian Szczesny
- & Wolfgang Schuhmann
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Article
| Open AccessBoosting potassium-ion batteries by few-layered composite anodes prepared via solution-triggered one-step shear exfoliation
Developing high-performance potassium-ion batteries remains a challenge. Here, the authors show that few-layered Sb2S3/carbon composite anode synthesized via simple exfoliation minimizes the volume changes during (de)intercalation of K+ ions with boosted rate performance and cyclability.
- Yajie Liu
- , Zhixin Tai
- & Hua Kun Liu
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Article
| Open AccessSolubility-mediated sustained release enabling nitrate additive in carbonate electrolytes for stable lithium metal anode
The solid-electrolyte interphase (SEI) is one of the governing factors for the reversibility of Li metal anode. Here, the authors reveal the impact of nitrate additive on the SEI in carbonate electrolytes, and demonstrate a method to overcome the solubility limitation of nitrate.
- Yayuan Liu
- , Dingchang Lin
- & Yi Cui
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Article
| Open AccessSelective conversion of CO2 and H2 into aromatics
Selective conversion of CO2 and H2 into aromatics remains challenging due to the high unsaturation degree and complex structure of aromatics. Here the authors report a composite catalyst of ZnAlOx and H-ZSM-5 which promotes the formation of aromatics with high selectivity while inhibiting CO and CH4 formation in CO2 hydrogenation reactions.
- Youming Ni
- , Zhiyang Chen
- & Zhongmin Liu
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Article
| Open AccessUnderstanding the apparent fractional charge of protons in the aqueous electrochemical double layer
A detailed atomic-scale description of the electrochemical interface is essential to the understanding of electrochemical energy transformations. Here, the authors investigate the solvated proton at the electrochemical interface and show that it unexpectedly carries a fractional charge.
- Leanne D. Chen
- , Michal Bajdich
- & Jens K. Nørskov
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Article
| Open AccessLight-induced formation of partially reduced oxygen species limits the lifetime of photosystem 1-based biocathodes
Photobiodevices use photosynthetic proteins such as those of the photosystem 1 (PS1) to enable light-induced charge separation, but they suffer from limited long-term stability. Here authors employ scanning photoelectrochemical microscopy on a PS1 biocathode and find that several pathways generate oxygen radicals.
- Fangyuan Zhao
- , Steffen Hardt
- & Felipe Conzuelo
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Article
| Open AccessRechargeable lithium-ion cell state of charge and defect detection by in-situ inside-out magnetic resonance imaging
The development of noninvasive methodology plays an important role in advancing lithium ion battery technology. Here the authors utilize the measurement of tiny magnetic field changes within a cell to assess the lithiation state of the active material, and detect defects.
- Andrew J. Ilott
- , Mohaddese Mohammadi
- & Alexej Jerschow
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Article
| Open AccessHighly nitrogen doped carbon nanofibers with superior rate capability and cyclability for potassium ion batteries
The development of potassium ion batteries calls for cheap, sustainable, and high-performance electrode materials. Here, the authors report a highly nitrogen-doped soft carbon anode that exhibits superior rate capability and cyclability based on a surface dominated charge storage mechanism.
- Yang Xu
- , Chenglin Zhang
- & Yong Lei
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Article
| Open AccessPerovskite seeding growth of formamidinium-lead-iodide-based perovskites for efficient and stable solar cells
Formamidinium-lead-iodide-based perovskites have a preferred bandgap below 1.55 eV for solar cell applications but suffer from operational instability. Here, Zhao et al. improve the film quality using cesium-containing seeded growth to show high stabilized efficiency and more than 100 h lifetime under simulated sunlight.
- Yicheng Zhao
- , Hairen Tan
- & Edward H. Sargent
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Article
| Open AccessDual properties of a hydrogen oxidation Ni-catalyst entrapped within a polymer promote self-defense against oxygen
Bio-inspired Ni-based molecular catalysts are efficient for H2 oxidation, but are suffering from the poor stability in the presence of O2. Here, the authors develop a strategy to boost greatly their stability by dispersing them in a hydrophobic and redox-silent polymer matrix.
- Alaa A. Oughli
- , Adrian Ruff
- & Olaf Rüdiger
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Article
| Open AccessKinetics of lithium peroxide oxidation by redox mediators and consequences for the lithium–oxygen cell
The kinetics of Li2O2 oxidation is of high importance to the operation of Li–O2 batteries. Here the authors work on different types of mediators revealing the dependence of the kinetics on the nature of the redox active site and its steric hindrance.
- Yuhui Chen
- , Xiangwen Gao
- & Peter G. Bruce
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Article
| Open AccessDendritic core-shell nickel-iron-copper metal/metal oxide electrode for efficient electrocatalytic water oxidation
Splitting water into high-energy fuel represents a renewable way to generate energy, yet the sluggish oxidation kinetics drives up technological costs. Here, the authors prepare tri-metallic core-shell electrodes using nickel, iron, and copper metals to accelerate electricity-driven water splitting.
- Peili Zhang
- , Lin Li
- & Licheng Sun
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Article
| Open AccessSpectroscopic detection of halogen bonding resolves dye regeneration in the dye-sensitized solar cell
Dye-sensitized solar cells rely on molecular dyes to absorb light and conduct electrons. Parlane et al. show that weak forces such as hydrogen bonding can be responsible for the dye regeneration step of solar cells and have an impact on the photovoltage and the efficiency.
- Fraser G. L. Parlane
- , Chantal Mustoe
- & Curtis P. Berlinguette
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Article
| Open AccessCubic gauche polymeric nitrogen under ambient conditions
Polymeric phases of nitrogen are promising as environmentally-friendly, high energy-density materials, but are inherently unstable. Here, the authors report the synthesis and stabilization of polymeric nitrogen in its cubic gauche phase under near-ambient conditions, via plasma-enhanced chemical vapour deposition.
- El Mostafa Benchafia
- , Zhenhua Yao
- & Zafar Iqbal
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Article
| Open AccessRechargeable aqueous zinc-manganese dioxide batteries with high energy and power densities
The development of rechargeable aqueous zinc batteries are challenging but promising for energy storage applications. With a mild-acidic triflate electrolyte, here the authors show a high-performance Zn-MnO2 battery in which the MnO2 cathode undergoes Zn2+ (de)intercalation.
- Ning Zhang
- , Fangyi Cheng
- & Jun Chen
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Review Article
| Open AccessUnderstanding materials challenges for rechargeable ion batteries with in situ transmission electron microscopy
In situ TEM is a powerful tool that helps to understand energy storage behaviors of various materials. This review summarizes the critical discoveries, enabled by in situTEM, in rechargeable ion batteries, and foresees its bright future for extensive applications.
- Yifei Yuan
- , Khalil Amine
- & Reza Shahbazian-Yassar
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Article
| Open AccessRationalizing the light-induced phase separation of mixed halide organic–inorganic perovskites
Mixed halide hybrid perovskites possess tunable band gaps, however, under illumination they undergo phase separation. Using spectroscopic measurements and theoretical modelling, Draguta and Sharia et al. quantitatively rationalize the microscopic processes that occur during phase separation.
- Sergiu Draguta
- , Onise Sharia
- & Masaru Kuno
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Article
| Open AccessSelective production of arenes via direct lignin upgrading over a niobium-based catalyst
Lignin is cheap and abundant, and potentially a major source of aromatic compounds. Here the authors show selective production of arenes via hydrodeoxygenation of lignin over Ru/Nb2O5, and mechanistically show the strong influence of the Nb2O5support on phenolic bond dissociation energies.
- Yi Shao
- , Qineng Xia
- & Yanqin Wang
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Article
| Open AccessExsolution trends and co-segregation aspects of self-grown catalyst nanoparticles in perovskites
Exsolution of transition metals from perovskites provides an effective route to useful catalysts, but the underlying factors governing exsolution remain poorly understood. Here, the authors find trends in exsolution in layered perovskites, showing that co-segregation of B-site dopant and oxygen vacancies plays a central role.
- Ohhun Kwon
- , Sivaprakash Sengodan
- & Guntae Kim
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Article
| Open AccessIn situ dynamic observations of perovskite crystallisation and microstructure evolution intermediated from [PbI6]4− cage nanoparticles
The photovoltaic performances of perovskite materials are strongly influenced by their crystallinity and film morphology. Here, the authors investigate the formation and morphology evolution mechanisms of lead halide perovskites and reveal that bulk polycrystals grow from intermediate [PbI6]4−cage nanoparticles.
- Qin Hu
- , Lichen Zhao
- & Qihuang Gong
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Article
| Open Access11% efficiency solid-state dye-sensitized solar cells with copper(II/I) hole transport materials
Inadequate pore infiltration and low conductivity of hole transporter materials limit the performance of solid-state dye-sensitized solar cells. Using fast charge-exchange Cu(II/I) complexes as part of the hole transporting material, Caoet al. overcome these issues to achieve a record photoconversion efficiency of 11%.
- Yiming Cao
- , Yasemin Saygili
- & Michael Grätzel
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Article
| Open AccessThe controlled disassembly of mesostructured perovskites as an avenue to fabricating high performance nanohybrid catalysts
Disassembly of three-dimensionally ordered materials generates nanoparticles with new structural and physicochemical properties. Here the authors show a fragmentation strategy applied to a perovskite material leading to nanostructures with improved catalytic activity in the methane combustion.
- Yuan Wang
- , Hamidreza Arandiyan
- & Rose Amal
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Article
| Open AccessEfficient hydrogen production on MoNi4 electrocatalysts with fast water dissociation kinetics
In water-alkali electrolyzers, sluggish water dissociation kinetics on platinum-free electrocatalysts result in poor hydrogen-production activities. Here the authors report a MoNi4electrocatalyst which reduces the kinetic energy barrier of water dissociation, leading to improved hydrogen-production performance.
- Jian Zhang
- , Tao Wang
- & Xinliang Feng
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Article
| Open AccessStructure and interstitial iodide migration in hybrid perovskite methylammonium lead iodide
The mechanism underpinning the photovoltaic effect in hybrid perovskite solar cells has remained unclear. Here, Green and co-workers suggest that iodide ions in methylammonium lead iodide perovskite migrate via interstitial sites and undergo a redox reaction to form molecular iodine and free electrons.
- J. L. Minns
- , P. Zajdel
- & M. A. Green
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Article
| Open AccessFast oxygen diffusion and iodide defects mediate oxygen-induced degradation of perovskite solar cells
Determining the degradation pathways in lead halide perovskites is key to its development as a viable solar technology. Aristidouet al. identify iodide vacancies as the preferred sites in mediating the photo-induced formation of superoxide species from intercalated oxygen.
- Nicholas Aristidou
- , Christopher Eames
- & Saif A. Haque
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Article
| Open AccessHomogeneously catalysed conversion of aqueous formaldehyde to H2 and carbonate
Aqueous formaldehyde is an attractive hydrogen storage system due to the high weight percentage of hydrogen present. Here the authors report a highly active homogeneous ruthenium catalyst system, allowing hydrogen production from formaldehyde-water under mild conditions.
- M. Trincado
- , Vivek Sinha
- & Hansjörg Grützmacher
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Article
| Open AccessMultifunctionality of silver closo-boranes
Silver compounds have long been known to possess exceptional solid-state conductivity. Here the authors present silvercloso-boranes in which facile Ag+migration occurs, leading to exceptionally high ion conductivities and potential utility in silver nanowire production and photocatalysis due to their semiconductivity.
- Mark Paskevicius
- , Bjarne R. S. Hansen
- & Torben R. Jensen
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Article
| Open AccessDynamic behaviour of interphases and its implication on high-energy-density cathode materials in lithium-ion batteries
In lithium-ion batteries the interactions between the electrode and electrolyte represent a complex but critical process. Here the authors reveal the dynamic behaviour of interphases driven by conductive carbon through chemical and imaging analyses of a model transition-metal oxide cathode material.
- Wangda Li
- , Andrei Dolocan
- & Arumugam Manthiram
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Article
| Open AccessMultiscale structural and electronic control of molybdenum disulfide foam for highly efficient hydrogen production
The hydrogen evolution reaction is a complicated process involving liquid-solid-gas three-phase interface behaviour. Here, the authors report the multiscale structural and electronic control of molybdenum disulfide foam and demonstrate its high activity and stability for hydrogen evolution.
- Jiao Deng
- , Haobo Li
- & Xinhe Bao
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Article
| Open AccessLight-assisted delithiation of lithium iron phosphate nanocrystals towards photo-rechargeable lithium ion batteries
Photo-rechargable energy storage cells can provide plug-free power for various applications. Here the authors integrate a photo-absorbing dye complex with LiFePO4nanocrystals as a lithium-ion battery cathode in a two-electrode system demonstrating its photo-charging and galvanostatic discharging.
- Andrea Paolella
- , Cyril Faure
- & Karim Zaghib
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Article
| Open AccessAdvanced rechargeable aluminium ion battery with a high-quality natural graphite cathode
Rechargeable aluminium ion batteries are an emerging class of energy storage device. Here the authors reveal high-quality natural graphite as a promising cathode for Al-ion batteries, also identifying chloroaluminate anion intercalation in graphite by Raman spectroscopy.
- Di-Yan Wang
- , Chuan-Yu Wei
- & Hongjie Dai
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Article
| Open AccessPhase transformation mechanism in lithium manganese nickel oxide revealed by single-crystal hard X-ray microscopy
As an intercalation electrode material for lithium ion batteries, spinel LixMn1.5Ni0.5O4possesses a metastable nature during the electrochemical operation. Here the authors reveal the phase transformation mechanism by using single-crystal hard X-ray microscopy to detect the local phase distribution.
- Saravanan Kuppan
- , Yahong Xu
- & Guoying Chen
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Article
| Open AccessEvidence for ion migration in hybrid perovskite solar cells with minimal hysteresis
Ion migration has been related to hysteresis in perovskite solar cells, but not all perovskite cells exhibit a hysteresis. Here, Caladoet al. show that ion migration occurs regardless of hysteresis, but photogenerated carriers screen the effects of ionic charge for some solar cell architectures.
- Philip Calado
- , Andrew M. Telford
- & Piers R.F. Barnes
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Article
| Open AccessA small electron donor in cobalt complex electrolyte significantly improves efficiency in dye-sensitized solar cells
The electrolyte is an important component of dye-sensitized solar cells. Here, Haoet al. use an electron donor additive in the cobalt-based electrolyte, which speeds up the dye regeneration and slows down recombinations. The resulting devices are stable and more efficient than those without additive.
- Yan Hao
- , Wenxing Yang
- & Gerrit Boschloo
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Article
| Open AccessNonstoichiometric acid–base reaction as reliable synthetic route to highly stable CH3NH3PbI3 perovskite film
The stability of perovskite thin films and devices depends on a number of environmental factors, amongst which humidity. Here, Longet al. develop a synthetic route using a nonstoichiometric acid-base reaction to prepare films stable in humid environments for two months.
- Mingzhu Long
- , Tiankai Zhang
- & Keyou Yan
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Article
| Open AccessA biomimetic redox flow battery based on flavin mononucleotide
Redox flow batteries using organic active materials are highly sought after because of their potential to satisfy low cost and sustainability requirements. Here, the authors report a biomimetic flow battery based on flavin mononucleotide and a hydrotrope with promising performance characteristics.
- Akihiro Orita
- , Michael G. Verde
- & Ying Shirley Meng
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Article
| Open AccessSingle-catalyst high-weight% hydrogen storage in an N-heterocycle synthesized from lignin hydrogenolysis products and ammonia
Energy storage and biomass utilization are two major challenges for sustainability. Here the authors use a major lignin hydrogenolysis product for the synthesis of an N-heterocycle and develop a bimetallic catalyst for repeated hydrogenation/dehydrogenation of this and other molecules for hydrogen storage.
- Daniel Forberg
- , Tobias Schwob
- & Rhett Kempe
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Article
| Open AccessUltrasmall and phase-pure W2C nanoparticles for efficient electrocatalytic and photoelectrochemical hydrogen evolution
Tungsten carbide has yet to live up to its long-believed potential as a replacement for precious metal electrocatalysts. Here, Li and co-workers demonstrate that ditungsten carbide in the form of ultrasmall, phase-pure nanoparticles is a better candidate for the hydrogen evolution reaction.
- Qiufang Gong
- , Yu Wang
- & Shuit-Tong Lee
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Article
| Open AccessMetal-encapsulated organolead halide perovskite photocathode for solar-driven hydrogen evolution in water
Lead-halide perovskites are sensitive to humidity, which limits their use in water splitting applications. Here, the authors protect the perovskite layer with Field’s metal, driving photoelectrocatalytic hydrogen evolution in an aqueous solution for approximately one hour under constant illumination.
- Micaela Crespo-Quesada
- , Luis M. Pazos-Outón
- & Erwin Reisner
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Article
| Open AccessA nickel iron diselenide-derived efficient oxygen-evolution catalyst
Metal selenides have been reported as promising oxygen-evolution catalysts but their active forms are yet to be elucidated. Here, the authors show that metal selenides are unstable under oxygen-evolution conditions and that in situgenerated metal oxides/hydroxides are responsible for their high activity.
- Xiang Xu
- , Fang Song
- & Xile Hu
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Article
| Open AccessPentlandite rocks as sustainable and stable efficient electrocatalysts for hydrogen generation
There are comparable structural properties between the natural enzyme [FeNi]-hydrogenase and the natural ore, pentlandite. Here the authors, inspired by these similarities, use the mineral as a ‘rock’ electrode, and evaluate its electrocatalytic hydrogen evolution performance.
- Bharathi Konkena
- , Kai junge Puring
- & Ulf-Peter Apfel
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Article
| Open AccessMeasurement of the cleavage energy of graphite
Knowing the cleavage energy of graphite layers is important to understand the mechanical properties of graphite, graphene and related compounds. Here, the authors report a high accuracy experimental measurement of the cleavage energy and validation through multiscale modelling.
- Wen Wang
- , Shuyang Dai
- & Quanshui Zheng
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Article |
Origins of hydration lubrication
Subnanometre-thick hydration layers can greatly reduce the friction between two sliding objects, an effect termed hydration lubrication. Here, Ma et al.determine the frictional dissipation in such layers, which can account for the observed lubricating action of hydrated ions or zwitterions.
- Liran Ma
- , Anastasia Gaisinskaya-Kipnis
- & Jacob Klein