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1.
Artigo em Inglês | MEDLINE | ID: mdl-39361831

RESUMO

Silicon oxide-based (SiOx-based) materials show great promise as anodes for high-energy lithium-ion batteries due to their high specific capacity. However, their practical application is hindered by the inevitable volumetric expansion during the lithiation/delithiation process. Constructing high-performance binders for SiOx-based anodes has been regarded as an efficient strategy to mitigate their volume expansion and preserve structural integrity. In this work, we propose a green water-solution PAA-LS binder composed of poly(acrylic acid) (PAA) and sodium lignosulfonate (LS) with fast self-healing properties. The designed binder can be restored due to the strong affinity between Fe3+-catechol coordination bonds, thereby effectively alleviating the volumetric strain of SiOx-based anodes. Notably, with an optimized LS content of 0.5%, the SiOx@PAA-LS electrode exhibits excellent performance, delivering a high capacity of 997.3 mAh g-1 after 450 cycles at 0.5 A g-1. Furthermore, the SiOx||NCM622 full cell also demonstrates superior cycling stability, maintaining a discharge capacity of 147.58 mAh g-1 after 100 cycles at 0.5 A g-1, with an impressive capacity retention rate of 82.72%.

2.
Small ; : e2405379, 2024 Oct 04.
Artigo em Inglês | MEDLINE | ID: mdl-39363823

RESUMO

Aqueous zinc-ion batteries (AZIBs) are considered as a promising energy storage system because of good safety, low cost, abundant resources, and environmental friendliness. However, the bottlenecks including dendrite growth, hydrogen evolution, and corrosion seriously limit their practical application. Herein, a novel ZnSn(OH)6 coating layer with rich hydroxyl groups is employed to achieve highly stable Zn anode. The hydroxyl groups can feasibly interact with H2O molecules, contributing to the desolvation of hydrated Zn2+ and the inhibition of side reactions on Zn anode surface. Furthermore, according to the DFT calculation, the adsorption energy of Zn2+ among various sites on the surface of ZnSn(OH)6 coating layer is relatively large, which helps the uniform distribution of Zn2+ flux and the prevention of dendrite growth. Consequently, the ZnSn(OH)6@Zn anode delivers ultra-long cycle life (6770 h), low polarization voltage (27 mV), and high Coulombic efficiency (99.2% over 800 cycles) at 1 mA cm-2, 1 mAh cm-2. Besides, the assembled NaV3O8·xH2O//ZnSn(OH)6@Zn full cell can operate stably for 1500 cycles at 2 A g-1 with a high specific capacity of 144.9 mAh g-1, demonstrating an excellent application potential. This simple and effective coating layer with high electrochemical performance provides an appealing strategy for the development of rechargeable AZIBs.

3.
ChemSusChem ; : e202401139, 2024 Sep 06.
Artigo em Inglês | MEDLINE | ID: mdl-39239772

RESUMO

Solid-state lithium-metal batteries (SSLMBs) have attracted great attention due to their outstanding advantages in safety, electrochemical stability and interfacial compatibility. However, the low ionic conductivity and narrow electrochemical window restrict their practical application. Herein, in-situ polymerization electrolytes (IPEs) crosslinked by acrylonitrile (AN) and ethylene glycol dimethacrylate (EGDMA) exhibit the superior ionic conductivity of 1.77×10-3 S cm-1 at 25 °C, the ultrahigh lithium transference number (tLi+) of 0.784 and the wider electrochemical stable window (ESW) of 5.65 V. The IPEs make the symmetrical Li||Li cells achieve the highly stable lithium stripping/plating cycling for over 3000 h at 0.1 mA cm-2. Meanwhile, IPE endows the solid-state LiFePO4||Li batteries with an excellent long-cycle performance over 700 cycles at 2.5 C with a capacity retention ratio over 95 %, as well as 1000 cycles at 1 C and superior capacity retention of 85 %. More importantly, the in-situ polymerized electrolytes containing polyacrylonitrile (PAN) open up a new frontier to promote the practical application of solid-state batteries with high safety and high energy density via in-situ solidification technology.

4.
Physiol Int ; 111(3): 242-257, 2024 Sep 18.
Artigo em Inglês | MEDLINE | ID: mdl-39186388

RESUMO

Kettlebell as a sport has gained recognition worldwide. We characterized the physiological responses induced by a simulated kettlebell competition routine in experienced kettlebell athletes (n = 26) in a two-group, pre-post plus short-term follow-up, non-randomized experiment. The experimental group (EXP) included 13 kettlebell athletes, while the control group (CON) consisted of 13 individuals with prior recreational exposure to kettlebell activities. EXP performed a 10-minute-long, long-cycle kettlebell routine, whereas CON engaged in seated rest. Cardiovascular and neuromuscular outcomes were measured at rest, after warm-up, during exercise, at 0 (immediately post), 5 and 15 min into recovery. Group-by-time interactions revealed that the 10-minute-long, long-cycle kettlebell routine increased (P < 0.05) the levels of all outcomes (e.g. heart rate, blood pressure, blood lactate) (range of effect sizes: -0.9-8.9) with many outcomes remaining well above baseline at 5 and 15 min into recovery. A notable exception was a lack of change in maximal squat strength. Kettlebell experience and mass correlated with changes in oxygen uptake (ΔVO2) and in ventilation (ΔVT) (r = -0.70, 0.64, -0.87, and 0.73, respectively, P < 0.05) in EXP. Kettlebell routine evoked significant changes in all physiological variables (respiratory and cardiovascular), out of which the heart rate (HR), diastolic blood pressure (DBP), rate pressure product (RPP), and blood lactate (BL) outlasted the routine for at least 15 min. Future studies should longitudinally examine physiological responses to kettlebell training throughout a season. Long-cycle kettlebell routine adds to the repertoire of evidence-based exercise options for high-intensity exercise.


Assuntos
Atletas , Frequência Cardíaca , Humanos , Masculino , Frequência Cardíaca/fisiologia , Adulto , Consumo de Oxigênio/fisiologia , Adulto Jovem , Feminino , Pressão Sanguínea/fisiologia , Ácido Láctico/sangue , Desempenho Atlético/fisiologia , Exercício Físico/fisiologia , Força Muscular/fisiologia
5.
Small ; : e2404135, 2024 Aug 01.
Artigo em Inglês | MEDLINE | ID: mdl-39087389

RESUMO

To effectively solve the challenges of rapid capacity decay and electrode crushing of silicon-carbon (Si-C) anodes, it is crucial to carefully optimize the structure of Si-C active materials and enhance their electron/ion transport dynamic in the electrode. Herein, a unique hybrid structure microsphere of Si/C/CNTs/Cu with surface wrinkles is prepared through a simple ultrasonic atomization pyrolysis and calcination method. Low-cost nanoscale Si waste is embedded into the pyrolysis carbon matrix, cleverly combined with the flexible electrical conductivity carbon nanotubes (CNTs) and copper (Cu) particles, enhancing both the crack resistance and transport kinetics of the entire electrode material. Remarkably, as a lithium-ion battery anode, the fabricated Si/C/CNTs/Cu electrode exhibits stable cycling for up to 2300 cycles even at a current of 2.0 A g-1, retaining a capacity of ≈700 mAh g-1, with a retention rate of 100% compared to the cycling started at a current of 2.0 A g-1. Additionally, when paired with an NCM523 cathode, the full cell exhibits a capacity of 135 mAh g-1 after 100 cycles at 1.0 C. Therefore, this synthesis strategy provides insights into the design of long-life, practical anode electrode materials with micro/nano-spherical hybrid structures.

6.
Adv Mater ; 36(41): e2407233, 2024 Oct.
Artigo em Inglês | MEDLINE | ID: mdl-39152942

RESUMO

Aqueous Mn-ion batteries (MIBs) exhibit a promising development potential due to their cost-effectiveness, high safety, and potential for high energy density. However, the development of MIBs is hindered by the lack of electrode materials capable of storing Mn2+ ions due to acidic manganese salt electrolytes and large ion radius. Herein, the tunnel-type structure of monoclinic VO2 nanorods to effectively store Mn2+ ions via a reversible (de)insertion chemistry for the first time is reported. Utilizing exhaustive in situ/ex situ multi-scale characterization techniques and theoretical calculations, the co-insertion process of Mn2+/proton is revealed, elucidating the capacity decay mechanism wherein high proton activity leads to irreversible dissolution loss of vanadium species. Further, the Grotthuss transfer mechanism of protons is broken via a hydrogen bond reconstruction strategy while achieving the modulation of the electric double-layer structure, which effectively suppresses the electrode interface proton activity. Consequently, the VO2 demonstrates excellent electrochemical performance at both ambient temperatures and -20 °C, especially maintaining a high capacity of 162 mAh g-1 at 5 A g-1 after a record-breaking 20 000 cycles. Notably, the all-vanadium symmetric pouch cells are successfully assembled for the first time based on the "rocking-chair" Mn2+/proton hybrid mechanism, demonstrating the practical application potential.

7.
Small ; 20(37): e2401922, 2024 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-38721984

RESUMO

Introducing N atoms in vanadium oxides (VOx) of aqueous Zn-ion batteries (ZIBs) can reduce their bandgap energy and enhance their electronic conductivity, thereby promoting the diffusion of Zn2+. The close-packed vanadium oxynitride (VON) generated often necessitates the intercalation of water molecules for restructuring, rendering it more conducive for zinc ion intercalation. However, its dense structure often causes structural strain and the formation of by-products during this process, resulting in decreased electrochemical performance. Herein, carbon-coated porous V2O3/VN nanosheets (p-VON@C) are constructed by annealing vanadium metal-organic framework in an ammonia-contained environment. The designed p-VON@C nanosheets are efficiently converted to low-crystalline hydrated N-doped VOx during subsequent activation while maintaining structural stability. This is because the V2O3/VN heterojunction and abundant oxygen vacancies in p-VON@C alleviate the structural strain during water molecule intercalation, and accelerate the intercalation rate. Carbon coating is beneficial to prevent p-VON@C from sliding or falling off during the activation and cycling process. Profiting from these advantages, the activated p-VON@C cathode delivers a high specific capacity of 518 mAh g-1 at 0.2 A g-1 and maintains a capacity retention rate of 80.9% after 2000 cycles at 10 A g-1. This work provides a pathway to designing high-quality aqueous ZIB cathodes.

8.
J Colloid Interface Sci ; 670: 385-394, 2024 Sep 15.
Artigo em Inglês | MEDLINE | ID: mdl-38772255

RESUMO

Solid-state lithium metal batteries (SSLMBs) are promising candidates for safe and high-energy-density next-generation applications. However, harmful interfacial decomposition and uneven Li deposition lead to poor ion transport, a short cycle life, and battery failure. Herein, we propose a novel poly(ethylene oxide) (PEO)-based composite solid electrolyte (CSE) containing succinonitrile (SN) and zinc oxide (ZnO) nanoparticles (NPs), which improves interface stability through a dual mechanism. (1) By anchoring bis(trifluoromethanesulfonyl)imide (TFSI) anions to ZnO, a reliable solid electrolyte interface (SEI) later with abundant LiF can be obtained to inhibit interface decomposition. (2) The immobilization of escaping SN molecules in the SEI layer by ZnO NPs promotes the self-polymerization of SN and facilitates charge transfer through the interface. As a result, the ion conductivity of the stainless steel-symmetrical battery reaches 1.1 × 10-4 S cm-1 at room temperature, and a LiFePO4 (LFP) full battery exhibits ultrahigh stability (800 cycles) at 0.5 C. Thus, the present study provides valuable insights for the development of advanced PEO-based SSLMBs.

9.
ACS Appl Mater Interfaces ; 16(20): 26121-26129, 2024 May 22.
Artigo em Inglês | MEDLINE | ID: mdl-38728577

RESUMO

The design of aqueous zinc-ion batteries (ZIBs) that have high specific capacity and long-term stability is essential for future large-scale energy storage systems. Cathode materials with extended π-conjugation and abundant active sites are desirable to enhance the charge storage performance and the cycling stability of the aqueous ZIB. Based on this concept, 6,9-dihydropyrazino[2,3-g]quinoxaline-2,3,7,8(1H,4H)-tetrone was chosen as the monomer to be electropolymerized onto carbon cloth (PDHPQ-Tetrone/CC). When used as the cathode material for aqueous ZIBs, an exceptional cycling life (>20,000 cycles) at a current density of 10 A g-1 was achieved, with the specific capacity maintained at 82.8% and with the Coulombic efficiency at around 100% throughout cycling. At the charge-discharge current density of 0.1 A g-1, the ZIB with PDHPQ-Tetrone/CC achieved a high specific capacity of 248 mAh g-1. Kinetic analyses showed that both surface-capacitive-controlled processes and semi-infinite diffusion-controlled processes contribute to the stored charge. The charge storage mechanism was investigated with ex situ characterizations and involves the redox processes of carbonyl/hydroxyl and amino/imino groups coupled with insertion and extraction of both Zn2+ and H+.

10.
ACS Appl Mater Interfaces ; 16(20): 26217-26225, 2024 May 22.
Artigo em Inglês | MEDLINE | ID: mdl-38733352

RESUMO

Among various anode materials, SiOx is regarded as the next generation of promising anode due to its advantages of high theoretical capacity with 2680 mA h g-1, low lithium voltage platform, and rich natural resources. However, the pure SiOx-based materials have slow lithium storage kinetics attributed to their low electron/ion conductive properties and the large volume change during lithiation/delithiation, restricting their practical application. Optimizing the SiOx material structures and the fabricating methods to mitigate these fatal defects and adapt to the market demand for energy density is critical. Hence, SiOx material with TiO1-xNx phase modification has been prepared by simple, low-cost, and scalable ball milling and then combined with nitridation. Consequently, based on the TiO1-xNx modified layer, which boosts high ionic/electronic conductivity, chemical stability, and excellent mechanical properties, the SiOx@TON-10 electrode shows highly stable lithium-ion storage performance for lithium-ion half/full batteries due to a stable solid-electrolyte interface layer, fast Li+ transport channel, and alleviative volumetric expansion, further verifying its practical feasibility and universal applicability.

11.
Artigo em Inglês | MEDLINE | ID: mdl-38655816

RESUMO

In this study, we present a strategic approach for the structural design and composite modification of one-dimensional Sn-based nanocomposites to enhance the overall electrochemical performance of hybrid magnesium-lithium batteries (MLIBs), which are emerging as promising successors to lithium-ion batteries. By using electrospinning technology, we successfully synthesized NST-SnO2, NST-SnO2-NiO, Sn-CNF, and Ni3Sn2-CNF composite cathodes, as well as analyzed the synthesis mechanism of the four Sn-based cathodes. The 100-cycle testing at a current density of 500 mA·g-1 revealed that NST-SnO2 maintained a discharge specific capacity of 129.8 mA h·g-1 with a retention rate of 90.76%, while NST-SnO2-NiO achieved a higher capacity of 147.4 mA h·g-1 and an 88.05% retention rate. Notably, Sn-CNF and Ni3Sn2-CNF exhibited initial discharge capacities of 66.7 and 79.6 mA h·g-1, respectively, coupled with exceptional cycle stability, evidenced by retention rates of 104.19 and 102.38%. The remarkable cycling stability observed in these novel cathodes is attributed to their robust structural integrity, thus demonstrating the potential for an extended cycle life in MLIBs. This work provides significant advancement in the development of high-performance electrode materials for next-generation hybrid magnesium-lithium energy storage systems.

12.
Adv Mater ; 36(26): e2400737, 2024 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-38572792

RESUMO

Electrode crosstalk between anode and cathode at elevated temperatures is identified as a real culprit triggering the thermal runaway of lithium-ion batteries. Herein, to address this challenge, a novel smart polymer electrolyte is prepared through in situ polymerization of methyl methacrylate and acrylic anhydride monomers within a succinonitrile-based dual-anion deep eutectic solvent. Owing to the abundant active unsaturated double bonds on the as-obtained polymer matrix end, this smart polymer electrolyte can spontaneously form a dense crosslinked polymer network under elevated temperatures, effectively slowing down the crosstalk diffusion kinetics of lithium ions and active gases. Impressively, LiCoO2/graphite pouch cells employing this smart polymer electrolyte demonstrate no thermal runaway even at the temperature up to 250 °C via accelerating rate calorimeter testing. Meanwhile, because of its abundance of functional motifs, this smart polymer electrolyte can facilitate the formation of stable and thermally robust electrode/electrolyte interface on both electrodes, ensuring the long cycle life and high safety of LIBs. In specific, this smart polymer electrolyte endows 1.1 Ah LiCoO2/graphite pouch cell with a capacity retention of 96% after 398 cycles at 0.2 C.

13.
Small ; 20(33): e2400709, 2024 Aug.
Artigo em Inglês | MEDLINE | ID: mdl-38552228

RESUMO

Prussian white (PW) is one of the most promising candidates as a cathode for sodium-ion batteries (SIBs) because of its high theoretical capacity, excellent rate performance, and low production cost. However, PW materials suffer severe capacity decay during long-term cycling. In this work, a robust cathode electrolyte interface (CEI) is designed on the PW cathode by employing cresyl diphenyl phosphate (CDP) and adiponitrile (ADN) as electrolyte additives. CDP and ADN possess higher highest occupied molecular orbital energy levels (HOMO) than other solvents, leading to the preferential decomposition of CDP and ADN to construct an inorganics-rich CEI layer in situ on the PW cathode. Benefiting from this CEI layer, the degradation of PW is effectively inhibited during the long cycling. The Na||PW cell achieves an excellent cycling performance with a capacity retention of 85.62% after 1400 cycles. This work presented here provides a feasible strategy for improving the cycling performance of PW by electrolyte modification.

14.
Angew Chem Int Ed Engl ; 63(31): e202403424, 2024 Jul 29.
Artigo em Inglês | MEDLINE | ID: mdl-38545934

RESUMO

Rechargeable aluminum batteries (RABs) are a promising candidate for large-scale energy storage, attributing to the abundant reserves, low cost, intrinsic safety, and high theoretical capacity of Al. However, the cathode materials reported thus far still face challenges such as limited capacity, sluggish kinetics, and undesirable cycle life. Herein, we propose an organic cathode benzo[i] benzo[6,7] quinoxalino [2,3-a] benzo [6,7] quinoxalino [2,3-c] phenazine-5,8,13,16,21,24-hexaone (BQQPH) for RABs. The six C=O and six C=N redox active sites in each molecule enable BQQPH to deliver a record ultra-high capacity of 413 mAh g-1 at 0.2 A g-1. Encouragingly, the intermolecular hydrogen bonding network and π-π stacking interactions endow BQQPH with robust structural stability and minimal solubility, enabling an ultra-long lifetime of 100,000 cycles. Moreover, the electron-withdrawing carbonyl group induces a reduction in the energy level of the lowest unoccupied molecular orbital and expands the π-conjugated system, which considerably enhances both the discharge voltage and redox kinetics of BQQPH. In situ and ex situ characterizations combined with theoretical calculations unveil that the charge storage mechanism is reversible coordination/dissociation of AlCl2 + with the N and O sites in BQQPH accompanied by 12-electron transfer. This work provides valuable insights into the design of high-performance organic cathode materials for RABs.

15.
Angew Chem Int Ed Engl ; 63(23): e202404400, 2024 Jun 03.
Artigo em Inglês | MEDLINE | ID: mdl-38517342

RESUMO

The practical application of lithium metal batteries (LMBs) has been hindered by limited cycle-life and safety concerns. To solve these problems, we develop a novel fluorinated phosphate cross-linker for gel polymer electrolyte in high-voltage LMBs, achieving superior electrochemical performance and high safety simultaneously. The fluorinated phosphate cross-linked gel polymer electrolyte (FP-GPE) by in-situ polymerization method not only demonstrates high oxidation stability but also exhibits excellent compatibility with lithium metal anode. LMBs utilizing FP-GPE realize stable cycling even at a high cut-off voltage of 4.6 V (vs Li/Li+) with various high-voltage cathode materials. The LiNi0.6Co0.2Mn0.2O2|FP-GPE|Li battery exhibits an ultralong cycle-life of 1200 cycles with an impressive capacity retention of 80.1 %. Furthermore, the FP-GPE-based batteries display excellent electrochemical performance even at practical conditions, such as high cathode mass loading (20.84 mg cm-2), ultrathin Li (20 µm), and a wide temperature range of -25 to 80 °C. Moreover, the first reported solid-state 18650 cylindrical LMBs have been successfully fabricated and demonstrate exceptional safety under mechanical abuse. Additionally, the industry-level 18650 cylindrical LiMn2O4|FP-GPE|Li4Ti5O12 cells demonstrate a remarkable cycle-life of 1400 cycles. Therefore, the impressive electrochemical performance and high safety in practical batteries demonstrate a substantial potential of well-designed FP-GPE for large-scale industrial applications.

16.
J Colloid Interface Sci ; 664: 790-800, 2024 Jun 15.
Artigo em Inglês | MEDLINE | ID: mdl-38492380

RESUMO

Deleterious volumetric expansion and poor electrical conductivity seriously hinder the application of Si-based anode materials in lithium-ion batteries (LIBs). Herein, boron-doped three-dimensional (3D) porous carbon framework/carbon shell encapsulated silicon (B-3DCF/Si@C) hybrid composites are successfully prepared by two coating and thermal treatment processes. The presence of 3D porous carbon skeleton and carbon shell effectively improves the mechanical properties of the B-3DCF/Si@C electrode during the cycling process, ensures the stability of the electrical contacts of the silicon particles and stabilizes the solid electrolyte interface (SEI) layer, thus enhancing the electronic conductivity and ion migration efficiency of the anode. The developed B-3DCF/Si@C anode has a high reversible capacity, excellent cycling stability and outstanding rate performance. A reversible capacity of 1288.5 mAh/g is maintained after 600 cycles at a current density of 400 mA g-1. The improved electrochemical performance is demonstrated in a full cell using a LiFePO4-based cathode. This study presents a novel approach that not only mitigates the large volume expansion effects in LIB anode materials, but also provides a reference model for the preparation of porous composites with various functionalities.

17.
J Colloid Interface Sci ; 663: 801-809, 2024 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-38442521

RESUMO

Sodium-selenium (Na-Se) batteries have gained attention due to their high energy density and power density, resulting from the liquid-liquid reaction at the interface in the dimethoxyethane electrolyte. Nevertheless, the pronounced shuttle effect of polyselenides causes low coulomb efficiency and inadequate cycling stability for Na-Se batteries. Herein, the iron nanoparticles surface modified accordion-like Ti3C2Tx MXene (MXene/Fe) synthesized via the molten salt etching is utilized as the host of Se species for high-performance Na-Se battery cathode. Benefiting from the layered structure and chemical adsorption of accordion-like MXene, the shuttle effect of the cathode is effectively inhibited. Simultaneously, electrochemical kinetics is boosted due to the catalytic effect of Fe nanoparticles, which facilitate the transformation of polyselenide from long-chain to short-chain, contributing to pseudocapacitive capacity. Consequently, the Se-based cathode delivers a steady capacity of 575.0 mA h g-1 at 0.2 A/g, and even a high capacity of 500 mAh/g at 50 A/g based on the mass of Se@MXene/Fe electrode, indicating the ultrafast Na+ ion storage. Most notably, this structure demonstrated remarkable long-term cycling stability for 5000 cycles with a high capacity retention of 97.4 %. The electrochemical energy storage mechanism is further revealed by in situ Raman. Herein, the confinement-catalysis structure shines light on inhibiting shuttling and facilitating ultrafast ion storage.

18.
Adv Mater ; 36(21): e2312486, 2024 May.
Artigo em Inglês | MEDLINE | ID: mdl-38332711

RESUMO

Compared with conventional inorganic materials, organic electrodes are competitive candidates for secondary battery cathodes due to their resourcefulness, environmental friendliness, and cost-effectiveness. Much effort is devoted at the level of chemical structure, while ignoring the impact of molecular aggregation on battery behavior. Herein, this work designs a series of organic molecules with two electrochemically active phenothiazine groups linked by different lengths of alkyl chain to regulate molecular symmetry and crystallinity. The results emphasize the equally important role of molecular aggregation and chemical structure for battery performance. Among them, 2PTZ-C7H14|Li cell exhibits the most impressive cycle and rate performance. At the high rate of 50 C, it can still deliver a capacity of 63.4 mA h g-1 and 74.5% capacity retention after 10 000 cycles. Besides, the dropout voltage of 2PTZ-C9H18|Li cell is only 52 mV, which is among the lowest reported for lithium-organic batteries to the best of the author's knowledge.

19.
Adv Sci (Weinh) ; 11(14): e2308258, 2024 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-38291813

RESUMO

Increasing the charging cut-off voltage (e.g., 4.6 V) to extract more Li ions are pushing the LiCoO2 (LCO) cathode to achieve a higher energy density. However, an inhomogeneous cycled bulk-to-surface Li distribution, which is closely associated with the enhanced extracted Li ions, is usually ignored, and severely restricts the design of long lifespan high voltage LCO. Here, a strategy by constructing an artificial solid-solid Li diffusion environment on LCO's surface is proposed to achieve a homogeneous bulk-to-surface Li distribution upon cycling. The diffusion optimized LCO not only shows a highly reversible capacity of 212 mA h g-1 but also an ultrahigh capacity retention of 80% over 600 cycles at 4.6 V. Combined in situ X-ray diffraction measurements and stress-evolution simulation analysis, it is revealed that the superior 4.6 V long-cycled stability is ascribed to a reduced structure stress leaded by the homogeneous bulk-to-surface Li diffusion. This work broadens approaches for the design of highly stable layered oxide cathodes with low ion-storage structure stress.

20.
ACS Appl Mater Interfaces ; 16(4): 4661-4670, 2024 Jan 31.
Artigo em Inglês | MEDLINE | ID: mdl-38232753

RESUMO

The recently developed advanced electrolytes possess many crucial qualities, including robust stability, Li dendrite-free, and comparable interface compatibility, for the manufacturing of Li metal batteries with a high energy density. In this study, lithium bis(trifluoromethane)sulfonimide, acrylamide, and succinonitrile were first used to design a polymerizable monomer. Then, it went through in situ thermal polymerization to attain a new solid polymer electrolyte [named poly(PDES)]. The synthesized poly(PDES) electrolyte achieved higher ionic conductivity (∼1.89 × 10-3 S cm-1), oxidation potential (∼5.10 V versus Li+/Li), and a larger lithium-ion transfer number (∼0.63). Moreover, poly(PDES) was nonflammable and could effectively inhibit the formation of Li dendrites. As a result, the assembled batteries using the poly(PDES) electrolyte for both Li||LiFePO4 and Li||LiNi0.8Co0.1Mn0.1O2 exhibited excellent interface compatibility and electrochemical performances. This poly(PDES) electrolyte has promising potential for broad application in lithium-metal batteries with elevated energy density and safety performance in the near future.

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