Featured
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| Open AccessDirect electrosynthesis of 52% concentrated CO on silver’s twin boundary
Isolating purified electrosynthesis product is a major challenge in electrochemical carbon dioxide reduction. Here, the authors report a nanotwinned silver electrocatalyst and a pneumatic-trough cell system to produce a 52% concentrated CO, which is further utilized as a carbon feedstock for graphene production.
- Can Tang
- , Peng Gong
- & Zhengzong Sun
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Article
| Open AccessPromoting photocatalytic CO2 reduction with a molecular copper purpurin chromophore
Designing highly efficient chromophores comprising earth-abundant elements is essential for both light harvesting and electron transfer reactions. Here, authors prepare a copper purpurin complex that shows enhanced photocatalytic activity for CO2 reduction to CO with a high selectivity.
- Huiqing Yuan
- , Banggui Cheng
- & Zhiji Han
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Article
| Open AccessFlexible thermal interface based on self-assembled boron arsenide for high-performance thermal management
Well-developed prototype interface materials for electronics thermal management are limited to a low thermal conductivity or high elastic modulus. Here, the authors report flexible thermal interfaces through self-assembled manufacturing of polymetric composites based on the high thermal conductivity of cubic boron arsenide.
- Ying Cui
- , Zihao Qin
- & Yongjie Hu
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Article
| Open AccessA high throughput optical method for studying compositional effects in electrocatalysts for CO2 reduction
A high-throughput method is presented for the synthesis and testing of alloy electrocatalysts for gas phase CO2 electrolysis. Active ternary alloy catalysts were discovered and their structures characterized by X-ray pair distribution functional analysis.
- Jeremy L. Hitt
- , Yuguang C. Li
- & Thomas E. Mallouk
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Article
| Open AccessHigh oxide-ion conductivity through the interstitial oxygen site in Ba7Nb4MoO20-based hexagonal perovskite related oxides
Oxide-ion conductors are important in various applications for clean energy. Here, authors report high oxide-ion conductivity of hexagonal perovskite-related oxide Ba7Nb3.9Mo1.1O20.05, which is ascribed to the interstitialcy diffusion and low activation energy for oxide-ion conductivity.
- Masatomo Yashima
- , Takafumi Tsujiguchi
- & Stephen J. Skinner
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Article
| Open AccessSelective filling of n-hexane in a tight nanopore
Molecular sieving typically occurs when molecules with smaller kinetic diameter than a nanopore selectively enter the pore. Here the authors show, using photoluminescence imaging and ab initio molecular dynamics simulations, that single-walled carbon nanotubes can separate n-hexane from cyclohexane, despite both having larger kinetic diameter than the nanopore.
- Haoran Qu
- , Archith Rayabharam
- & YuHuang Wang
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Article
| Open AccessSingle-layered organic photovoltaics with double cascading charge transport pathways: 18% efficiencies
Efficiency of organic solar cells is determined by the physical properties of donors and acceptors in bulk heterojunction film. The authors optimise quaternary blends to realize a double cascading energy level alignment enabling efficient carrier dissociation and transport, achieving 18% efficiency.
- Ming Zhang
- , Lei Zhu
- & Feng Liu
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Article
| Open AccessReducing the impact of Auger recombination in quasi-2D perovskite light-emitting diodes
Designing efficient perovskite light-emitting diodes remains a challenge due to the strong Auger recombination and resulting Joule heating. Here, the authors propose polarizable p-fluorophenethylammonium to generate quasi-2D perovskites with reduced binding energy developing perovskite light-emitting diodes with a peak EQE of 20.36% and a maximum luminance of 82,480 cdm-2.
- Yuanzhi Jiang
- , Minghuan Cui
- & Mingjian Yuan
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Article
| Open AccessIsolated copper single sites for high-performance electroreduction of carbon monoxide to multicarbon products
Electrochemical carbon monoxide reduction is a promising strategy to yield valuable multicarbon products but low selectivities and Faradaic efficiencies are common. Here the authors show single atom copper catalyst supported on MXene with high CO reduction performance and stability.
- Haihong Bao
- , Yuan Qiu
- & Xuping Sun
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Article
| Open AccessSynthesis of bio-based methylcyclopentadiene via direct hydrodeoxygenation of 3-methylcyclopent-2-enone derived from cellulose
Synthesis of methylcyclopentadiene (MCPD) with abundant biomass is appealing. Here the authors show that cellulose-derived 3-methylcyclopent-2-enone can be directly hydrodeoxygenated to MCPD over a partially reduced Zn-Mo oxide catalyst.
- Yanting Liu
- , Ran Wang
- & Ning Li
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Article
| Open AccessTransforming carbon dioxide into jet fuel using an organic combustion-synthesized Fe-Mn-K catalyst
Design and discovery of catalysts to make clean energy and mitigate the harmful effect of greenhouse gases remains a massive challenge. Here the authors report a combustion-synthesised iron-based catalyst of high activity and selectivity for directly converting CO2 to aviation jet fuel.
- Benzhen Yao
- , Tiancun Xiao
- & Peter P. Edwards
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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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Comment
| Open AccessA few basic concepts in electrochemical carbon dioxide reduction
Electrochemical carbon dioxide (CO2) reduction has the potential to sustainably produce carbon-based fuels and chemicals while mitigating the increasing levels of CO2 in the atmosphere. In this comment, the author discusses a few basic concepts in the fundamental mechanistic studies of electrochemical CO2 reduction.
- Karen Chan
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Perspective
| Open AccessIdentification and elimination of false positives in electrochemical nitrogen reduction studies
Discovering a sustainable route to ammonia as a fertiliser and as an energy carrier is critically important, but many recent reports on the electrochemical nitrogen reduction are false positives. Here the authors uncover the emerging experimental traps and detail protocols to reliably avoid them.
- Jaecheol Choi
- , Bryan H. R. Suryanto
- & Alexandr N. Simonov
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Article
| Open AccessAtomically dispersed Lewis acid sites boost 2-electron oxygen reduction activity of carbon-based catalysts
H2O2 production via oxygen reduction offers a renewable approach to obtain an often-used oxidant. Here, authors show the incorporation of Lewis acid sites into carbon-based materials to improve H2O2 electrosynthesis.
- Qihao Yang
- , Wenwen Xu
- & Liang Chen
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Article
| Open AccessDopants fixation of Ruthenium for boosting acidic oxygen evolution stability and activity
There is an increasing interest in understanding how defect chemistry can alter material reactivity. Here, authors tune the electronic structure of RuO2 by introducing W and Er dopants that boost acidic oxygen evolution performances by limiting oxygen vacancy formation during catalysis.
- Shaoyun Hao
- , Min Liu
- & Xingwang Zhang
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Comment
| Open AccessThe future of low-temperature carbon dioxide electrolysis depends on solving one basic problem
Low-temperature carbon dioxide electrolysis is an attractive process for sustainable fuel synthesis, but current systems suffer from low efficiency. In this comment, authors discuss the limitations arising from the reaction between carbon dioxide and hydroxide, highlighting the need for new research to address this fundamental problem.
- Joshua A. Rabinowitz
- & Matthew W. Kanan
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Article
| Open AccessPhotobase effect for just-in-time delivery in photocatalytic hydrogen generation
Efficient photocatalytic hydrogen generation relies on highly choreographed delivery of protons and electrons to the reaction site such that they arrive just in time. Here, authors show that proton transport can be controlled by light with the photobase effect to increase H2 generation rate.
- Jiawen Fang
- , Tushar Debnath
- & Jacek K. Stolarczyk
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Article
| Open AccessRoll-to-roll gravure-printed flexible perovskite solar cells using eco-friendly antisolvent bathing with wide processing window
Driven by recent improvement in efficiency and stability of perovskite solar cells, the next step toward commercialisation is upscaling. Here, the authors demonstrate pilot-scale fully roll-to-roll manufacturing of flexible perovskite solar cells through gravure-printing and antisolvent bathing.
- Young Yun Kim
- , Tae-Youl Yang
- & Jangwon Seo
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Article
| Open AccessPreparation of nickel-iron hydroxides by microorganism corrosion for efficient oxygen evolution
Developing facile strategies to realize the precise construction of Ni-Fe structures is of significance for water oxidation. Here, the authors demonstrate a universal microorganism-assisted corrosion strategy for preparing highly efficient Ni-Fe composites towards oxygen evolution.
- Huan Yang
- , Lanqian Gong
- & Bao Yu Xia
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Article
| Open AccessHigh-power lithium–selenium batteries enabled by atomic cobalt electrocatalyst in hollow carbon cathode
Lithium selenium batteries are attractive energy storage systems, but they are hindered by low selenium reaction activity and rapid capacity fading. Herein, the authors report a selenium host with atomic cobalt electrocatalyst which exhibits superior performances in lithium-selenium batteries.
- Hao Tian
- , Huajun Tian
- & Guoxiu Wang
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Comment
| Open AccessAlcohol oxidation as alternative anode reactions paired with (photo)electrochemical fuel production reactions
(Photo)electrochemical cells that produce fuels have often relied on water oxidation to complete the redox cycle. Here, the authors discuss alcohol oxidation as an alternative reaction and consider general mechanistic features of oxidation electrocatalysts.
- Michael T. Bender
- , Xin Yuan
- & Kyoung-Shin Choi
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Article
| Open AccessStabilization of a molecular water oxidation catalyst on a dye−sensitized photoanode by a pyridyl anchor
Understanding the properties of water-splitting assemblies in dye-sensitized photoelectrochemical cells is a key challenge in artificial photosynthesis. Here, the authors report the importance of anchoring groups on a water oxidation catalyst in determining active species on metal oxide surfaces.
- Yong Zhu
- , Degao Wang
- & Thomas J. Meyer
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Article
| Open AccessA direct coupled electrochemical system for capture and conversion of CO2 from oceanwater
Isolating CO2 to use in electrochemical CO2 reduction systems is an ongoing issue. Here, the authors present a proof-of-concept integrated system combining a bipolar membrane electrodialysis cell with a vapor-fed CO2 reduction cell for capture and conversion of CO2 from oceanwater.
- Ibadillah A. Digdaya
- , Ian Sullivan
- & Chengxiang Xiang
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Article
| Open AccessTuning proton-coupled electron transfer by crystal orientation for efficient water oxidization on double perovskite oxides
Proton-coupled electron transfer (PCET) has been observed in chemical, energy, and biological transformation processes. Here we demonstrate that the rate of PCET and oxygen evolution reaction can be dramatically enhanced by tuning crystal orientation and the correlated proton diffusion.
- Yunmin Zhu
- , Zuyun He
- & Meilin Liu
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Article
| Open AccessCoordination engineering of iridium nanocluster bifunctional electrocatalyst for highly efficient and pH-universal overall water splitting
Water electrolysis offers a promising energy conversion technology, although there is still a need to understand the catalysis on the atomic-level. Here, the authors report Ir nanoclusters coordinated with both N and S as an efficient and pH-universal electrocatalyst for overall water splitting.
- Qilun Wang
- , Cong-Qiao Xu
- & Bin Liu
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Article
| Open AccessSurface chelation of cesium halide perovskite by dithiocarbamate for efficient and stable solar cells
Surface engineering is a known strategy to optimize the perovskite solar cells but it is usually based on weak bondings, such as Van der Waals, or coorordiating interacterions. Here He et al. report a chelation strategy using strongly adsorbed dithiocarbamate molecules and achieve high efficiency of 17.03% with excellent stability for CsPbI2Br based solar cells.
- Jingjing He
- , Junxian Liu
- & Hua Gui Yang
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Article
| Open AccessDirect insights into the role of epoxy groups on cobalt sites for acidic H2O2 production
The production of hydrogen peroxide by electrochemical oxygen reduction is an attractive alternative to the industrial process, but catalysts should be optimized. Here, the authors enhance hydrogen peroxide production in acidic media with epoxy groups near cobalt centers on carbon nanotubes.
- Qingran Zhang
- , Xin Tan
- & Xunyu Lu
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Article
| Open AccessDynamic evolution and reversibility of single-atom Ni(II) active site in 1T-MoS2 electrocatalysts for hydrogen evolution
While single atom catalysis combines heterogeneous materials with molecular understanding, the role of the single atoms remains vague. Here, authors examine single Ni on MoS2 via in situ X-ray absorption spectroscopy to reveal the intermediate and catalytically active species.
- Brian Pattengale
- , Yichao Huang
- & Jier Huang
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Article
| Open AccessMetal 3D printing technology for functional integration of catalytic system
Metal 3D printing is a very promising technology to revolutionize catalytic systems. Here the authors show that metal 3D printing products themselves can simultaneously serve as chemical reactors and catalysts for conversion of C1 molecules into high value-added chemicals.
- Qinhong Wei
- , Hangjie Li
- & Noritatsu Tsubaki
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Article
| Open AccessEnergy storing bricks for stationary PEDOT supercapacitors
Fired brick is a universal building material, produced by thousand-year-old technology, which throughout history has seldom served any other purpose. Here, the authors show that bricks can store energy after chemical treatment to convert their iron oxide content into conducting polymer nanofibers.
- Hongmin Wang
- , Yifan Diao
- & Julio M. D’Arcy
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Article
| Open AccessRevealing the role of crystal orientation of protective layers for stable zinc anode
Zinc affinity plays a key role in the zinc plating and stripping processes but its internal mechanism is still unclear. Here, the authors report a protective layer with controllable zinc affinity by adjusting the crystal orientation to suppress the dendrite growth on the zinc anode interface.
- Qi Zhang
- , Jingyi Luan
- & Haiyan Wang
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Article
| Open AccessSpontaneous solar water splitting with decoupling of light absorption and electrocatalysis using silicon back-buried junction
The simultaneous management of optical, electrical, and catalytic properties is challenging for photoelectrochemical devices. Here, authors design Si back-buried junction photoelectrodes that can be series connected for unassisted water-splitting with a high solar-to-hydrogen efficiency of 15.62%.
- Hui-Chun Fu
- , Purushothaman Varadhan
- & Jr-Hau He
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Article
| Open AccessScalable neutral H2O2 electrosynthesis by platinum diphosphide nanocrystals by regulating oxygen reduction reaction pathways
The synthesis of high concentration H2O2 from water and oxygen at moderate conditions could provide an on-site H2O2 source for medical and water purification applications. Here, authors show Al2O3-stabilized PtP2 nanocrystals to enable selective, stable and efficient neutral pH H2O2 production.
- Hui Li
- , Peng Wen
- & Scott M. Geyer
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Article
| Open AccessScalable aesthetic transparent wood for energy efficient buildings
Transparent wood composites are promising engineered materials for green energy-efficient building. Here, authors demonstrate novel aesthetic wood with integrated functions of optical transparency, UV-blocking, thermal insulation, and mechanical strength for this sustainable application.
- Ruiyu Mi
- , Chaoji Chen
- & Liangbing Hu
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Article
| Open AccessEnhanced multi-carbon alcohol electroproduction from CO via modulated hydrogen adsorption
The electrocatalytic upgrading of CO to higher-value fuels provides a promising route to multi-carbon alcohol products. Here, the authors show that high alcohol selectivity and activity can be achieved by incorporating palladium in copper.
- Jun Li
- , Aoni Xu
- & David Sinton
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Article
| Open AccessChemical instability at chalcogenide surfaces impacts chalcopyrite devices well beyond the surface
Anion vacancies are a hurdle for technologies based on chalcogenide semiconductors and topological insulators. Even at room temperature, oxidation and cyanide etching can lead to selenium vacancies in CuInSe2 photovoltaic material but suitable post deposition treatments can mitigate their effect.
- Diego Colombara
- , Hossam Elanzeery
- & Susanne Siebentritt
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Article
| Open AccessElectrochemical CO2 reduction to high-concentration pure formic acid solutions in an all-solid-state reactor
Electrochemical CO2 reduction to liquid fuels is limited by low product concentrations and formation of mixtures with traditional liquid electrolytes. Here the authors report an all-solid-state system for a continuous generation of high-purity and high-concentration formic acid vapors and solutions.
- Lei Fan
- , Chuan Xia
- & Haotian Wang
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Article
| Open AccessOperando time-resolved X-ray absorption spectroscopy reveals the chemical nature enabling highly selective CO2 reduction
A systematic time-resolved study can provide key insights on selective carbon dioxide electro-reduction. Here, the authors report operando seconds-resolved X-ray absorption spectroscopy to uncover the chemical state evolution of working catalysts in a carbon dioxide electroreduction process.
- Sheng-Chih Lin
- , Chun-Chih Chang
- & Hao Ming Chen
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Article
| Open AccessHighly reversible oxygen redox in layered compounds enabled by surface polyanions
Oxygen-anion redox in lithium-rich layered oxides can boost the capacity of lithium-ion battery cathodes. Here, the authors investigate the mechanism of surface degradation caused by oxygen oxidation and the kinetics of surface reconstruction.
- Qing Chen
- , Yi Pei
- & Graeme Henkelman
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Matters Arising
| Open AccessUnrealistic energy and materials requirement for direct air capture in deep mitigation pathways
- Sudipta Chatterjee
- & Kuo-Wei Huang
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Article
| Open AccessImpact of dual-layer solid-electrolyte interphase inhomogeneities on early-stage defect formation in Si electrodes
Severe structural deformation during (de)lithiation is the main factor limiting the stability of Si anodes in Li-ion batteries. Here, a multi-modal approach is used to visualize these deformations in their early-stage and link them to inhomogeneities in the dual-layer solid-electrolyte interphase.
- Chunguang Chen
- , Tao Zhou
- & Peter H. L. Notten
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Article
| Open AccessEfficient wettability-controlled electroreduction of CO2 to CO at Au/C interfaces
Great advances have been made in CO2 electroreduction, however, the role of wettability-controlled interfacial structures remains poorly understood. Here, the authors apply confocal laser scanning microscopy to gain deeper understanding of these phenomena in gas diffusion electrodes.
- Run Shi
- , Jiahao Guo
- & Tierui Zhang
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Article
| Open AccessEnabling safe aqueous lithium ion open batteries by suppressing oxygen reduction reaction
Despite the non-flammable nature of water-based electrolytes, aqueous lithium-ion batteries still carry an explosion risk due to the sealing structure. Here the authors report a safe aqueous battery with an open configuration, utilizing highly concentrated electrolytes and Al2O3 coated anodes.
- Long Chen
- , Longsheng Cao
- & Chunsheng Wang
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Article
| Open AccessIn-situ structure and catalytic mechanism of NiFe and CoFe layered double hydroxides during oxygen evolution
NiFe and CoFe layered double hydroxides are among the most active electrocatalysts for the alkaline oxygen evolution reaction. Here, by combining operando experiments and rigorous DFT calculations, the authors unravel their active phase, the reaction center and the catalytic mechanism.
- Fabio Dionigi
- , Zhenhua Zeng
- & Peter Strasser
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Article
| Open AccessSelective electroreduction of CO2 to acetone by single copper atoms anchored on N-doped porous carbon
Efficient electroreduction of CO2 to multi-carbon products is challenging. Here, the single atom Cu encapsulated on N-doped porous carbon catalysts are designed for reducing CO2 to acetone at low overpotentials and the active sites are identified as Cu coordination with four pyrrole-N atoms.
- Kun Zhao
- , Xiaowa Nie
- & Jingguang G. Chen
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Article
| Open AccessTuning lithium-peroxide formation and decomposition routes with single-atom catalysts for lithium–oxygen batteries
Li–O2 batteries represent one of the promising paths toward high energy density battery systems. Here the authors synthesize single atom Co electrocatalysts to regulate the formation and decomposition of the major discharge product Li2O2, realizing high round-trip efficiency and stability in a Li–O2 cell.
- Li-Na Song
- , Wei Zhang
- & Ji-Jing Xu
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Article
| Open AccessOperando visualisation of battery chemistry in a sodium-ion battery by 23Na magnetic resonance imaging
Na-ion batteries offer multiple advantages, but there is a critical need for improved materials and understanding of sodiation mechanisms. Here the authors deploy operando 23Na magnetic resonance imaging and spectroscopy to observe sodium battery chemistry and dendrite formation, enabling new insight.
- Joshua M. Bray
- , Claire L. Doswell
- & Melanie M. Britton
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Article
| Open AccessHighly efficient electrosynthesis of hydrogen peroxide on a superhydrophobic three-phase interface by natural air diffusion
H2O2 electrosynthesis has garnered great attention as a green alternative to the anthraquinone process. Here the authors propose a cost-effective cathode to greatly improve the O2 diffusion coefficient, resulting in a high H2O2 production without the need for aeration.
- Qizhan Zhang
- , Minghua Zhou
- & Xuedong Du