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| Open AccessA solid-state lithium-ion battery with micron-sized silicon anode operating free from external pressure
Applying high stack pressure is primarily done to address the mechanical failure issue of solid-state batteries. Here, the authors propose a mechanical optimization strategy involving elastic electrolyte to realize solid-state batteries operating without external pressurizing.
- Hui Pan
- , Lei Wang
- & Haoshen Zhou
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Article
| Open AccessInter-site structural heterogeneity induction of single atom Fe catalysts for robust oxygen reduction
Here, authors report an inter-site structural heterogeneity induced effect of hierarchical single atom Fe catalysts for robust oxygen reduction. Dynamic evolutions and insights into structure-activity relationship are presented.
- Peng Zhang
- , Hsiao-Chien Chen
- & Yuan Pan
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Article
| Open AccessMolecular anchoring of free solvents for high-voltage and high-safety lithium metal batteries
Advanced electrolyte is essential for high-energy-density lithium metal batteries. Here, the authors design a molecular anchoring dilute electrolyte via intermolecular hydrogen bonding with free solvents to improve the battery electrochemical and thermal stabilities.
- Zhuangzhuang Cui
- , Zhuangzhuang Jia
- & Xiaodi Ren
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Article
| Open AccessDynamic chloride ion adsorption on single iridium atom boosts seawater oxidation catalysis
The seawater oxidation reaction faces challenges from competitive chloride oxidation reaction. Herein, the authors have utilized chlorine adsorption to modulate the single-atom Ir coordination state and promote seawater oxidation and catalyst stability.
- Xinxuan Duan
- , Qihao Sha
- & Xiaoming Sun
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Article
| Open AccessCation desolvation-induced capacitance enhancement in reduced graphene oxide (rGO)
Understanding local electrochemical processes can help improve electrochemical energy storage. Here, the authors report a charge storage mechanism in aqueous electrolyte for reduced graphene oxide using an electrochemical quartz crystal microbalance.
- Kangkang Ge
- , Hui Shao
- & Patrice Simon
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Article
| Open AccessInfluence of electric double layer rigidity on CO adsorption and electroreduction rate
High-pressure infrared spectroscopy shows concentrated cations suppress CO adsorption. Here the authors report two electrochemical interfaces forming distinct double layer structures and reaction rates at elevating pressure and various potentials.
- Jiajie Hou
- , Bingjun Xu
- & Qi Lu
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| Open AccessSingle-atom tailored atomically-precise nanoclusters for enhanced electrochemical reduction of CO2-to-CO activity
Tailoring catalytic performance of atomically-precise metal nanoclusters catalysts is of great interest but remains challenging. Here, the authors report a co-eletropolymerization strategy to modify well-defined Au8 nanoclusters by single-atom sites to enhance its electrocatalytic activity for the reduction of CO2 towards CO.
- Yi-Man Wang
- , Fang-Qin Yan
- & Shuang-Quan Zang
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Article
| Open AccessContinuous strain tuning of oxygen evolution catalysts with anisotropic thermal expansion
Tuning compressive strain is an effective way to accelerate the oxygen evolution reaction kinetics. Here the authors show that anisotropic thermal expansion induces compressive strains on IrO6 octahedron in Sr2IrO4, shifting its d-band center downward and accelerating water oxidation kinetics beyond traditional thermal diffusion effects.
- Yu Du
- , Fakang Xie
- & Zhigang Zou
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Article
| Open AccessIn situ copper faceting enables efficient CO2/CO electrolysis
Copper electrocatalysts enable carbon dioxide/carbon monoxide reduction but suffer from low production rates. Here, the authors promote in situ growth of Cu(100) during electrolysis, enabling efficient and stable electrosynthesis of multicarbon products at industrially-relevant current densities
- Kaili Yao
- , Jun Li
- & Hongyan Liang
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Article
| Open AccessNanocurvature-induced field effects enable control over the activity of single-atom electrocatalysts
Modulating interfacial electric fields provides a means to control electrocatalyst activity for a broad range of reactions. Here the authors show that this can be achieved by tuning the nanocurvature of carbon supported single-atom catalysts.
- Bingqing Wang
- , Meng Wang
- & Yanwei Lum
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Article
| Open AccessCreation of a point-of-care therapeutics sensor using protein engineering, electrochemical sensing and electronic integration
Low-cost point-of-care sensors are vital for precision medicine. Here, the authors have repurposed a glucometer for breast cancer therapeutic detection capable of sensing tamoxifen in human blood, utilizing blood glucose to power and amplify the therapeutic signals
- Rong Cai
- , Chiagoziem Ngwadom
- & Caroline M. Ajo-Franklin
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Article
| Open AccessEfficient direct repairing of lithium- and manganese-rich cathodes by concentrated solar radiation
Rapid capacity decay and voltage drop hinder lithium- and manganese-rich cathode material (LMRO) development. Here, the authors apply concentrated solar radiation arrays on cycled LMRO electrodes, inducing inverse spinel phase to boost redox activity and reversibility, yielding enhanced electrochemical performance.
- Hailong Wang
- , Xin Geng
- & Xin He
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Article
| Open AccessUnveiling the nature of Pt-induced anti-deactivation of Ru for alkaline hydrogen oxidation reaction
Despite the high intrinsic activity of Ru for hydrogen oxidation reaction, the surface oxidation-induced deactivation limits the application. Here, the authors report the introduction of Pt atoms could prevent the surface oxidation-related interfacial water network damage, preventing the deactivation of Ru.
- Yanyan Fang
- , Cong Wei
- & Gongming Wang
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Article
| Open AccessLiquid Madelung energy accounts for the huge potential shift in electrochemical systems
Electrode potential in any electrochemical systems has long been discussed by classical Debye-Hückel theory which holds only under extremely dilute concentrations. Here, the authors establish the concept ‘liquid Madelung potential’ to comprehensively describe the potential shift at practical concentrations.
- Norio Takenaka
- , Seongjae Ko
- & Atsuo Yamada
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Article
| Open AccessPromoting high-voltage stability through local lattice distortion of halide solid electrolytes
Solid electrolytes play a crucial role as ion conductors and separator between electrodes in all-solid-state batteries. Here, the authors report a high-entropy halide solid electrolyte, which reveals the structure evolution with the increasing configurational entropy and improves the high-voltage stability.
- Zhenyou Song
- , Tengrui Wang
- & Wei Luo
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Article
| Open AccessOxygen-tolerant CO2 electroreduction over covalent organic frameworks via photoswitching control oxygen passivation strategy
Direct use of flue gas for the electrocatalytic CO2 reduction reaction is desirable but severely limited by the thermodynamically favorable oxygen reduction reaction. Here the authors report an oxygen passivation strategy to improve electrocatalytic CO2 reduction reaction under aerobic conditions using a covalent organic frameworks with a photoswitching unit.
- Hong-Jing Zhu
- , Duan-Hui Si
- & Yuan-Biao Huang
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Article
| Open AccessFacilitating alkaline hydrogen evolution reaction on the hetero-interfaced Ru/RuO2 through Pt single atoms doping
Exploring an active and cost-effective catalyst for alkaline hydrogen evolution reaction remains elusive to date. Here, the authors report the platinum single-atoms doped ruthenium/ruthenium oxides showing distinctly enhanced catalytic performance.
- Yiming Zhu
- , Malte Klingenhof
- & Jiwei Ma
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Article
| Open AccessHigh-spin Co3+ in cobalt oxyhydroxide for efficient water oxidation
Regulating spin state of metal cations in catalysts is recognized as a strategy to improve water oxidation. Herein, the authors constructed high-spin cobalt ions in cobalt oxyhydroxides, experimentally demonstrating accelerated electron transfer ability and thereby superior water oxidation performance.
- Xin Zhang
- , Haoyin Zhong
- & Junmin Xue
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Article
| Open AccessElectrocatalytic water oxidation with manganese phosphates
Understanding water oxidation on Mn-based catalysts remains a long-standing challenge. Here, the authors use homologous KMnPO4 and KMnPO4•H2O as model catalyst to show that Mn(V)=O is responsible for O−O bond formation and its concentration determines the intrinsic activity.
- Shujiao Yang
- , Kaihang Yue
- & Wei Zhang
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Article
| Open AccessCa-dimers, solvent layering, and dominant electrochemically active species in Ca(BH4)2 in THF
Alternatives to lithium-ion electrochemistry present challenges due to undesirable phenomena at the electrode-electrolyte interface. Through simulations, the authors find that the performance of a calcium-based electrolyte is driven entirely by molecular-scale processes within approximately 1 nm of the electrode.
- Ana Sanz Matias
- , Fabrice Roncoroni
- & David Prendergast
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| Open AccessHierarchical Li electrochemistry using alloy-type anode for high-energy-density Li metal batteries
Utilizing an ultra-thin Li anode with a thickness below 50 μm is crucial for enhancing the energy density of batteries. Here, the authors develop a finely tunable, thin alloy-based Li anode that features a hierarchical Li electrochemistry, enabling stable cycling and superior energy density in Li metal batteries.
- Jiaqi Cao
- , Yuansheng Shi
- & Xia Lu
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Article
| Open AccessSolvation-property relationship of lithium-sulphur battery electrolytes
In the Li-S battery, a promising next-generation battery chemistry, electrolytes are vital because of solvated polysulfide species. Here, the authors investigate solvation-property relationships via the measurement of solvation free energy of the electrolytes, guiding advanced electrolyte design for Li-S batteries.
- Sang Cheol Kim
- , Xin Gao
- & Yi Cui
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Article
| Open AccessA surface strategy boosting the ethylene selectivity for CO2 reduction and in situ mechanistic insights
The electrochemical reduction of CO2 into multi-carbon product is interesting yet requires further research. Here, the authors develop a surface strategy to achieve high CO2-to-ethylene selectivity by dodecanethiol modification CuO electrode and show that dodecanethiol facilitates CO2 transfer, enhances *CO coverage and stabilize Cu(100) facet.
- Yinchao Yao
- , Tong Shi
- & Zhuo Chen
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Article
| Open AccessAcidic media enables oxygen-tolerant electrosynthesis of multicarbon products from simulated flue gas
Direct electroreduction of dilute CO2 in flue gas streams is challenging due to the presence of O2 impurities. Here the authors demonstrate that an acidic electrolyte can overcome this challenge, enabling the generation of multicarbon products from simulated flue gas at reasonable rates.
- Meng Wang
- , Bingqing Wang
- & Yanwei Lum
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Article
| Open AccessRedox-tunable isoindigos for electrochemically mediated carbon capture
Electrochemically-mediated carbon capture has good energy efficiency and potential in carbon dioxide separation, but optimisation of these systems is challenging. Here, the authors report the use of isoindigo derivatives to give fine-tuned interactions with CO2 for carbon capture methods.
- Xing Li
- , Xunhua Zhao
- & Yayuan Liu
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Article
| Open AccessRe-evaluation of battery-grade lithium purity toward sustainable batteries
Due to recent fluctuations in lithium prices, the instability of lithium-ion batteries prices is on the rise. Here, through a re-evaluation of purity criteria, the authors report that the presence of magnesium impurity in lithium precursor actually improves cathode performance, economics, and environmental aspects.
- Gogwon Choe
- , Hyungsub Kim
- & Yong-Tae Kim
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Article
| Open AccessHigh voltage electrolytes for lithium-ion batteries with micro-sized silicon anodes
Micro-sized silicon are promising anode materials due to low-cost and high-energy, yet their application is hindered by inaccessible electrolytes. Here, the authors report sulfolane-based electrolytes that form silicon-phobic interphases and enable high-voltage pouch cells to achieve superior cycle life.
- Ai-Min Li
- , Zeyi Wang
- & Chunsheng Wang
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Article
| Open AccessCapacitive tendency concept alongside supervised machine-learning toward classifying electrochemical behavior of battery and pseudocapacitor materials
Analysis of capacitive behavior of electrode materials used in batteries and pseudocapacitors is challenging. Here, authors report an electrochemical signal analysis method available as an online tool to classify the charge storage behavior of a material as battery-like or a pseudocapacitor-like.
- Siraprapha Deebansok
- , Jie Deng
- & Olivier Fontaine
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Article
| Open AccessTuning the apparent hydrogen binding energy to achieve high-performance Ni-based hydrogen oxidation reaction catalyst
Nickel-based electrocatalysts for the hydrogen oxidation reaction in hydroxide exchange membrane fuel cells show promise, but their activity requires further enhancement. Here, the authors report NiCuCr alloy with high activity, owing to the efficient tuning of both hydrogen and water binding on Ni sites by alloying with Cu and Cr.
- Xingdong Wang
- , Xuerui Liu
- & Zhongbin Zhuang
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Article
| Open AccessImplanting oxophilic metal in PtRu nanowires for hydrogen oxidation catalysis
Designing an efficient electrocatalyst of hydrogen oxidation reaction is highly critical for anion exchange membrane fuel cells. Here the authors report implanting oxophilic metal atoms in PtRu nanowires to significantly improve the mass activity, stability, and resistance to CO-poisoning for hydrogen oxidation.
- Zhongliang Huang
- , Shengnan Hu
- & Xiaoqing Huang
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Article
| Open AccessPotential and electric double-layer effect in electrocatalytic urea synthesis
Electrochemical urea synthesis presents a promising alternative to conventional synthesis methods, yet the elusive mechanism hindered its development. Here, the authors take copper as an example to explore the potential and electric double-layer effect in electrocatalytic urea synthesis, and reveal two essential strategies to promote the efficiency of urea synthesis.
- Qian Wu
- , Chencheng Dai
- & Zhichuan J. Xu
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Article
| Open AccessSubtractive transformation of cathode materials in spent Li-ion batteries to a low-cobalt 5 V-class cathode material
Direct recycling or upcycling is promising for sustainable battery resource management. Here, the authors report a subtractive transformation strategy for upcycling spent cathode materials to high-performance 5 V-class cathodes, reducing reliance on rare elements for the sustainable Li-ion battery industry.
- Jun Ma
- , Junxiong Wang
- & Guangmin Zhou
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Article
| Open AccessDesigning lithium halide solid electrolytes
The pursuit of all-solid-state batteries has motivated advancements in materials design. Here, the authors present a methodology demonstrating that ionic potential effectively captures crucial interactions within halide materials, guiding the design of the new materials with enhanced performance.
- Qidi Wang
- , Yunan Zhou
- & Marnix Wagemaker
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Article
| Open AccessSelf-assembled hydrated copper coordination compounds as ionic conductors for room temperature solid-state batteries
The design of inorganic-organic hybrid solid-state electrolytes is expected to merge the merits of both inorganic and organic material. Here, the authors craft Li-ion-implanted copper maleate hydrate nanoflakes via a bottom-up self-assembly approach to reveal superior room-temperature Li-ion conductivity.
- Xiao Zhan
- , Miao Li
- & Li Zhang
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Article
| Open AccessLattice oxygen activation and local electric field enhancement by co-doping Fe and F in CoO nanoneedle arrays for industrial electrocatalytic water oxidation
Oxygen evolution reaction is crucial in renewable energy conversion technologies. Here the authors report rough arrays of Fe and F co-doped CoO nanoneedles that highlight a conceptual strategy of coupling lattice oxygen activation and local electric field for industrial water oxidation applications.
- Pengcheng Ye
- , Keqing Fang
- & Yong Hu
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Article
| Open AccessOptimizing potassium polysulfides for high performance potassium-sulfur batteries
Potassium-sulfur battery are promising materials for next-generation high energy, low cost batteries. Here the authors explore a tungsten based catalytic composite for optimizing potassium polysulfides and improve K-S electrochemistry in batteries
- Wanqing Song
- , Xinyi Yang
- & Wenbin Hu
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Article
| Open AccessIntegrated energy storage and CO2 conversion using an aqueous battery with tamed asymmetric reactions
A system integrating CO2 conversion and energy storage holds great promise, but faces a major challenge due to degraded catalysts on charge. Here, the authors present a highly efficient energy storage and CO2 reduction method in an aqueous battery, achieved through oxidation of reducing molecules.
- Yumei Liu
- , Yun An
- & Quanquan Pang
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Article
| Open AccessBoosting a practical Li-CO2 battery through dimerization reaction based on solid redox mediator
Li–CO2 batteries following Li2CO3-product route suffers from low output voltage and severe parasitic reactions. Here, the authors introduce a copper-based solid redox mediator in Li–CO2 batteries with an efficient Li2C2O4 product route to circumvent the shuttle effect and sluggish kinetics caused by soluble mediators.
- Wei Li
- , Menghang Zhang
- & Haoshen Zhou
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Article
| Open AccessElectrostatic catalysis of a click reaction in a microfluidic cell
Can we utilize electric fields (EF) as a smart reagent to catalyze chemical processes? Here the authors develop a continuous-flow electrostatic reactor as a microfluidic platform that allows for the effective catalysis of click reaction over a large electrode surface exploiting voltage-controlled EF as the sole catalyst.
- Semih Sevim
- , Roger Sanchis-Gual
- & Josep Puigmartí-Luis
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Article
| Open AccessAn extended substrate screening strategy enabling a low lattice mismatch for highly reversible zinc anodes
The growth of dendrites and the occurrence of side reactions at zinc anodes currently impede the practical use of aqueous zinc batteries. Here, the authors present an advanced substrate screening approach aimed at stabilizing zinc anodes, thereby enabling the development of high-rate zinc-metal batteries.
- Zhiyang Zheng
- , Xiongwei Zhong
- & Guangmin Zhou
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Article
| Open AccessMechanistic insights into C-C coupling in electrochemical CO reduction using gold superlattices
Developing operando spectroscopic techniques with high sensitivity and reproducibility is of great importance for mechanistic investigations of surface-mediated electrochemical reactions. Here the authors study reaction mechanism of CO electroreduction using highly ordered gold superlattices as substrate for surface-enhanced infrared absorption spectroscopy.
- Xiaoju Yang
- , Chao Rong
- & Xuan Yang
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Article
| Open AccessDithiine-linked metalphthalocyanine framework with undulated layers for highly efficient and stable H2O2 electroproduction
Realization of stable and industrial-level hydrogen peroxide electroproduction still faces great challenge due large partly to the easy decomposition of this product. Here the authors report a strategy to achieve superior performance by promoting an increased electron density of Co center due to the introduction of sulfur atoms in the linking units of 2D CoPc-S-COF
- Qianjun Zhi
- , Rong Jiang
- & Jianzhuang Jiang
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Article
| Open AccessElectrophotocatalytic hydrogenation of imines and reductive functionalization of aryl halides
Open-shell catalytically active species are widely used in energy-consuming redox reactions, but their excited-state lifetimes are usually short. Here, the authors report a closed-shell thioxanthone-hydrogen anion species generated under electrochemical conditions, which can be photochemically converted to a potent and long-lived reductant.
- Wen-Jie Kang
- , Yanbin Zhang
- & Hao Guo
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Article
| Open AccessSite-selective protonation enables efficient carbon monoxide electroreduction to acetate
This work regulates solid/liquid/gas triple-phase interface, facilitating site-selective protonation in carbon monoxide electroreduction. It achieves increased energy-efficiency in acetate production and contributes to the understanding of selectively controlling the electrosynthesis of a single product.
- Xinyue Wang
- , Yuanjun Chen
- & Edward H. Sargent
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Article
| Open AccessMolecular understanding of the critical role of alkali metal cations in initiating CO2 electroreduction on Cu(100) surface
Alkali metal cations affect CO2 electroreduction performance. Here, the authors provide a comprehensive molecular understanding of the alkali metal cation effects on both CO2 activation and competing hydrogen evolution based on explicit solvation models.
- Zhichao Zhang
- , Hengyu Li
- & Jia Li
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Article
| Open AccessAlkaline-based aqueous sodium-ion batteries for large-scale energy storage
Aqueous sodium-ion batteries show promise for large-scale energy storage, yet face challenges due to water decomposition, limiting their energy density and lifespan. Here, the authors report a cathode surface coating strategy in an alkaline electrolyte to enhance the stability of both electrolyte and battery.
- Han Wu
- , Junnan Hao
- & Shi-Zhang Qiao
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Article
| Open AccessSite-specific metal-support interaction to switch the activity of Ir single atoms for oxygen evolution reaction
Common methods for regulating metal-support interactions for single-atom catalysts usually suffer from interference of the variation of supports or sacrificing the stability of catalysts. Here, the authors report a facile electrochemical deposition strategy to design highly active oxygen evolution catalysts with site-specific metal-support interactions via selective anchoring of single atoms.
- Jie Wei
- , Hua Tang
- & Jie Zeng
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Article
| Open AccessGas diffusion enhanced electrode with ultrathin superhydrophobic macropore structure for acidic CO2 electroreduction
Carbon dioxide electroreduction in acidic environments has been suboptimal. Here, the authors addressed this issue by designing a gas diffusion electrode with a special metal structure, which achieves efficient electroreduction while conducting a systematic investigation of the underlying mechanism.
- Mingxu Sun
- , Jiamin Cheng
- & Miho Yamauchi
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Article
| Open AccessA dicarbonate solvent electrolyte for high performance 5 V-Class Lithium-based batteries
Rechargeable lithium batteries featuring 5 V cathodes offer high energy density yet struggle with stability. Here, the authors formulate an electrolyte incorporating dimethyl 2,5-dioxahexanedioate solvent, which facilitates stable lithium plating and stripping while offering an extended cycle life.
- Xiaozhe Zhang
- , Pan Xu
- & Alexandru Vlad