Electrochemical energy storage devices with a high energy density are an important technology in modern society, especially for electric vehicles. The most effective approach to improve the energy ...density of batteries is to search for high‐capacity electrode materials. According to the concept of energy quality, a high‐voltage battery delivers a highly useful energy, thus providing a new insight to improve energy density. Based on this concept, a novel and successful strategy to increase the energy density and energy quality by increasing the discharge voltage of cathode materials and preserving high capacity is proposed. The proposal is realized in high‐capacity Li‐rich cathode materials. The average discharge voltage is increased from 3.5 to 3.8 V by increasing the nickel content and applying a simple after‐treatment, and the specific energy is improved from 912 to 1033 Wh kg−1. The current work provides an insightful universal principle for developing, designing, and screening electrode materials for high energy density and energy quality.
Li‐ion batteries with high energy quality require a high capacity coupled with high operating voltage. This requires the electrode materials to not only have a high specific capacity but also a high discharge voltage for cathode materials and low charge voltage for anode materials.
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BFBNIB, FZAB, GIS, IJS, KILJ, NLZOH, NUK, OILJ, SAZU, SBCE, SBMB, UL, UM, UPUK
Gradient surface Na‐ion doping is realized and demonstrated as an effective strategy to enhance the kinetics of Li‐rich cathode materials. Owing to the pinning effect of Na‐doping in the Li layer, ...the resultant Li‐rich particles exhibit superior electrochemical performances in terms of specific capacity, Coulombic efficiency, and cycling stability.
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FZAB, GIS, IJS, KILJ, NLZOH, NUK, OILJ, SAZU, SBCE, SBMB, UL, UM, UPUK
As one of the most promising cathodes for rechargeable sodium‐ion batteries (SIBs), O3‐type layered transition metal oxides commonly suffer from inevitably complicated phase transitions and sluggish ...kinetics. Here, a NaLi0.05Ni0.3Mn0.5Cu0.1Mg0.05O2 cathode material with the exposed {010} active facets by multiple‐layer oriented stacking nanosheets is presented. Owing to reasonable geometrical structure design and chemical substitution, the electrode delivers outstanding rate performance (71.8 mAh g−1 and 16.9 kW kg−1 at 50C), remarkable cycling stability (91.9% capacity retention after 600 cycles at 5C), and excellent compatibility with hard carbon anode. Based on the combined analyses of cyclic voltammograms, ex situ X‐ray absorption spectroscopy, and operando X‐ray diffraction, the reaction mechanisms behind the superior electrochemical performance are clearly articulated. Surprisingly, Ni2+/Ni3+ and Cu2+/Cu3+ redox couples are simultaneously involved in the charge compensation with a highly reversible O3–P3 phase transition during charge/discharge process and the Na+ storage is governed by a capacitive mechanism via quantitative kinetics analysis. This optimal bifunctional regulation strategy may offer new insights into the rational design of high‐performance cathode materials for SIBs.
An O3‐type NaLi0.05Ni0.3Mn0.5Cu0.1Mg0.05O2 cathode material with exposed {010} active facets by multiple‐layer oriented stacking nanosheets is successfully constructed via reasonable structure design and chemical substitution. An optimal bifunctional regulation is demonstrated to be an efficient strategy to restrain the unfavorable multiphase transformation and greatly improve Na+ transport kinetics resulting in excellent performance for sodium‐ion batteries.
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BFBNIB, FZAB, GIS, IJS, KILJ, NLZOH, NUK, OILJ, SAZU, SBCE, SBMB, UL, UM, UPUK
As one of the most promising cathode candidates for room‐temperature sodium‐ion batteries (SIBs), P2‐type layered oxides face the challenge of simultaneously realizing high‐rate performance while ...achieving long cycle life. Here, a stable Na2/3Ni1/6Mn2/3Cu1/9Mg1/18O2 cathode material is proposed that consists of multiple‐layer oriented stacking nanoflakes, in which the nickel sites are partially substituted by copper and magnesium, a characteristic of the material that is confirmed by multiscale scanning transmission electron microscopy and electron energy loss spectroscopy techniques. Owing to the optimal morphology structure modulation and chemical element substitution strategy, the electrode displays remarkable rate performance (73% capacity retention at 30C compared to 0.5C) and outstanding cycling stability in Na half‐cell system couple with unprecedented full battery performance. The underlying thermal stability, phase stability, and Na+ storage mechanisms are clearly elucidated through the systematical characterizations of electrochemical behaviors, in situ X‐ray diffraction at different temperatures, and operando X‐ray diffraction upon Na+ deintercalation/intercalation. Surprisingly, a quasi‐solid‐solution reaction is switched to an absolute solid‐solution reaction and a capacitive Na+ storage mechanism is demonstrated via quantitative electrochemical kinetics calculation during charge/discharge process. Such a simple and effective strategy might reveal a new avenue into the rational design of excellent rate capability and long cycle stability cathode materials for practical SIBs.
A stable copper and magnesium cosubstituted Na2/3Ni1/6Mn2/3Cu1/9Mg1/18O2 cathode material consisting of multiple‐layer oriented stacking nanoflakes is reported. An optimal structure design and a chemical element substitution strategy are demonstrated to greatly improve Na+ transport kinetics and structural stability of P2‐type cathode material, resulting in high‐rate and long cycle life for a sodium‐ion battery.
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Metallic lithium affords the highest theoretical capacity and lowest electrochemical potential and is viewed as a leading contender as an anode for high-energy-density rechargeable batteries. ...However, the poor wettability of molten lithium does not allow it to spread across the surface of lithiophobic substrates, hindering the production and application of this anode. Here we report a general chemical strategy to overcome this dilemma by reacting molten lithium with functional organic coatings or elemental additives. The Gibbs formation energy and newly formed chemical bonds are found to be the governing factor for the wetting behavior. As a result of the improved wettability, a series of ultrathin lithium of 10-20 μm thick is obtained together with impressive electrochemical performance in lithium metal batteries. These findings provide an overall guide for tuning the wettability of molten lithium and offer an affordable strategy for the large-scale production of ultrathin lithium, and could be further extended to other alkali metals, such as sodium and potassium.
Abstract
Na-ion cathode materials operating at high voltage with a stable cycling behavior are needed to develop future high-energy Na-ion cells. However, the irreversible oxygen redox reaction at ...the high-voltage region in sodium layered cathode materials generates structural instability and poor capacity retention upon cycling. Here, we report a doping strategy by incorporating light-weight boron into the cathode active material lattice to decrease the irreversible oxygen oxidation at high voltages (i.e., >4.0 V vs. Na
+
/Na). The presence of covalent B–O bonds and the negative charges of the oxygen atoms ensures a robust ligand framework for the NaLi
1/9
Ni
2/9
Fe
2/9
Mn
4/9
O
2
cathode material while mitigating the excessive oxidation of oxygen for charge compensation and avoiding irreversible structural changes during cell operation. The B-doped cathode material promotes reversible transition metal redox reaction enabling a room-temperature capacity of 160.5 mAh g
−1
at 25 mA g
−1
and capacity retention of 82.8% after 200 cycles at 250 mA g
−1
. A 71.28 mAh single-coated lab-scale Na-ion pouch cell comprising a pre-sodiated hard carbon-based anode and B-doped cathode material is also reported as proof of concept.
Lithium‐rich layered oxides with the capability to realize extraordinary capacity through anodic redox as well as classical cationic redox have spurred extensive attention. However, the ...oxygen‐involving process inevitably leads to instability of the oxygen framework and ultimately lattice oxygen release from the surface, which incurs capacity decline, voltage fading, and poor kinetics. Herein, it is identified that this predicament can be diminished by constructing a spinel Li4Mn5O12 coating, which is inherently stable in the lattice framework to prevent oxygen release of the lithium‐rich layered oxides at the deep delithiated state. The controlled KMnO4 oxidation strategy ensures uniform and integrated encapsulation of Li4Mn5O12 with structural compatibility to the layered core. With this layer suppressing oxygen release, the related phase transformation and catalytic side reaction that preferentially start from the surface are consequently hindered, as evidenced by detailed structural evolution during Li+ extraction/insertion. The heterostructure cathode exhibits highly competitive energy‐storage properties including capacity retention of 83.1% after 300 cycles at 0.2 C, good voltage stability, and favorable kinetics. These results highlight the essentiality of oxygen framework stability and effectiveness of this spinel Li4Mn5O12 coating strategy in stabilizing the surface of lithium‐rich layered oxides against lattice oxygen escaping for designing high‐performance cathode materials for high‐energy‐density lithium‐ion batteries.
A heterostructured spinel Li4Mn5O12 encapulated lithium‐rich layered oxide cathode is designed by the controlled KMnO4 oxidiation strategy. Spinel Li4Mn5O12 is chosen due to its lattice stability against oxygen release as well as a 3D lithium diffusion framework with minimal Jahn–Teller distortion. Such uniform coating can suppress lattice oxygen release, associated phase transformation, and catalytic side reactions, consequently ensuring improved electrochemical performance.
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Delivery of high‐energy density with long cycle life is facing a severe challenge in developing cathode materials for rechargeable sodium‐ion batteries (SIBs). Here a composite Na0.6MnO2 with ...layered–tunnel structure combining intergrowth morphology of nanoplates and nanorods for SIBs, which is clearly confirmed by micro scanning electron microscopy, high‐resolution transmission electron microscopy as well as scanning transmission electron microscopy with atomic resolution is presented. Owing to the integrated advantages of P2 layered structure with high capacity and that of the tunnel structure with excellent cycling stability and superior rate performance, the composite electrode delivers a reversible discharge capacity of 198.2 mAh g−1 at 0.2C rate, leading to a high‐energy density of 520.4 Wh kg−1. This intergrowth integration engineering strategy may modulate the physical and chemical properties in oxide cathodes and provide new perspectives on the optimal design of high‐energy density and high‐stable materials for SIBs.
A novel layered–tunnel intergrowth structure with stoichiometric Na0.6MnO2 composition is designed as a high‐performance cathode for sodium‐ion batteries (SIBs). Owing to the integrated advantages of the P2 layered structure with high capacity and that of the tunnel structure with excellent cycling stability and superior rate performance, this intergrowth cathode might be a promising cathode candidate for the large‐scale energy storage application of SIBs.
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Low‐cost and stable sodium‐layered oxides (such as P2‐ and O3‐phases) are suggested as highly promising cathode materials for Na‐ion batteries (NIBs). Biphasic hybridization, mainly involving P2/O3 ...and P2/P3 biphases, is typically used to boost their electrochemical performances. Herein, a P3/O3 intergrown layered oxide (Na2/3Ni1/3Mn1/3Ti1/3O2) as high‐rate and long‐life cathode for NIBs via tuning the amounts of Ti substitution in Na2/3Ni1/3Mn2/3−xTixO2 (x = 0, 1/6, 1/3, 2/3) is demonstrated. The X‐ray diffraction (XRD) Rietveld refinement and aberration‐corrected scanning transmission electron microscopy show the co‐existence of P3 and O3 phases, and density functional theory calculation corroborates the appearance of the anomalous O3 phase at the Ti substitution amount of 1/3. The P3/O3 biphasic cathode delivers an unexpected rate capability (≈88.7% of the initial capacity at a high rate of 5 C) and cycling stability (≈68.7% capacity retention after 2000 cycles at 1 C), superior to those of the sing phases P3‐Na2/3Ni1/3Mn2/3O2, P3‐Na2/3Ni1/3Mn1/2Ti1/6O2, and O3‐Na2/3Ni1/3Ti2/3O2. The highly reversible structural evolution of the P3/O3 integrated cathode observed by ex situ XRD, ex situ X‐ray absorption spectra, and the rapid Na+ diffusion kinetics, underpin the enhancement. These results show the important role of P3/O3 biphasic hybridization in designing and engineering layered oxide cathodes for NIBs.
P3/O3 biphasic Na2/3Ni1/3Mn1/3Ti1/3O2 cathode material is prepared for Na‐ion batteries by tuning the Ti amounts. This P3/O3 intergrown cathode delivers superior rate capability and cycling stability to those of the pristine P3 and O3 phases, which are underpinned by the observed highly reversible structural transition of P3/O3 biphase and the rapid Na+ diffusion kinetics.
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Summary
Microglia‐mediated neuroinflammation plays a dual role in various brain diseases due to distinct microglial phenotypes, including deleterious M1 and neuroprotective M2. There is growing ...evidence that the peroxisome proliferator‐activated receptor γ (PPARγ) agonist rosiglitazone prevents lipopolysaccharide (LPS)‐induced microglial activation. Here, we observed that antagonizing PPARγ promoted LPS‐stimulated changes in polarization from the M1 to the M2 phenotype in primary microglia. PPARγ antagonist T0070907 increased the expression of M2 markers, including CD206, IL‐4, IGF‐1, TGF‐β1, TGF‐β2, TGF‐β3, G‐CSF, and GM‐CSF, and reduced the expression of M1 markers, such as CD86, Cox‐2, iNOS, IL‐1β, IL‐6, TNF‐α, IFN‐γ, and CCL2, thereby inhibiting NFκB–IKKβ activation. Moreover, antagonizing PPARγ promoted microglial autophagy, as indicated by the downregulation of P62 and the upregulation of Beclin1, Atg5, and LC3‐II/LC3‐I, thereby enhancing the formation of autophagosomes and their degradation by lysosomes in microglia. Furthermore, we found that an increase in LKB1–STRAD–MO25 complex formation enhances autophagy. The LKB1 inhibitor radicicol or knocking down LKB1 prevented autophagy improvement and the M1‐to‐M2 phenotype shift by T0070907. Simultaneously, we found that knocking down PPARγ in BV2 microglial cells also activated LKB1–AMPK signaling and inhibited NFκB–IKKβ activation, which are similar to the effects of antagonizing PPARγ. Taken together, our findings demonstrate that antagonizing PPARγ promotes the M1‐to‐M2 phenotypic shift in LPS‐induced microglia, which might be due to improved autophagy via the activation of the LKB1–AMPK signaling pathway.
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DOBA, FZAB, GIS, IJS, IZUM, KILJ, NLZOH, NUK, OILJ, PILJ, PNG, SAZU, SBCE, SBMB, UILJ, UKNU, UL, UM, UPUK
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