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1.
Small ; : e2403084, 2024 Jul 03.
Artigo em Inglês | MEDLINE | ID: mdl-38958079

RESUMO

Residual alkali is one of the biggest challenges for the commercialization of sodium-based layered transition metal oxide cathode materials since it can even inevitably appear during the production process. Herein, taking O3-type Na0.9Ni0.25Mn0.4Fe0.2Mg0.1Ti0.05O2 as an example, an active strategy is proposed to reduce residual alkali by slowing the cooling rate, which can be achieved in one-step preparation method. It is suggested that slow cooling can significantly enhance the internal uniformity of the material, facilitating the reintegration of Na+ into the bulk material during the calcination cooling phase, therefore substantially reducing residual alkali. The strategy can remarkably suppress the slurry gelation and gas evolution and enhance the structural stability. Compared to naturally cooled cathode materials, the capacity retention of the slowly cooled electrode material increases from 76.2% to 85.7% after 300 cycles at 1 C. This work offers a versatile approach to the development of advanced cathode materials toward practical applications.

2.
Chem Sci ; 15(25): 9775-9783, 2024 Jun 26.
Artigo em Inglês | MEDLINE | ID: mdl-38939152

RESUMO

Transition-metal compounds (TMCs) have recently become promising candidates as lithium-sulfur (Li-S) battery cathode materials because they have unique adsorption and catalytic properties. However, the relationship between the anionic species and performance has not been sufficiently revealed. Herein, using FeCoNiX (X = O, S, and P) compounds as examples, we systematically studied the effects of the anion composition of FeCoNiX compounds on the adsorption and catalytic abilities of sulfur cathodes in Li-S batteries. Adsorption tests and density functional theory calculations showed that the adsorption ability toward lithium polysulfides follows the order: FeCoNiP > FeCoNiO > FeCoNiS, while in situ ultraviolet-visible spectroscopy and cyclic voltammetry revealed that the catalytic ability for lithium polysulfide conversion follows the order: FeCoNiP > FeCoNiS > FeCoNiO. These results indicate that FeCoNiP is an excellent polysulfide immobilizer and catalyst that restricts shuttling and improves reaction kinetics. Electrochemical tests further demonstrated that the FeCoNiP cathode delivered superior cycling performance to FeCoNiO or FeCoNiS. In addition, the battery performance order is consistent with that of catalytic ability, which suggests that catalytic ability plays a key influencing role in batteries. This study provides new insight into the use of O-, S-, and P-doped TMCs as functional sulfur carriers.

3.
Fish Shellfish Immunol ; 151: 109707, 2024 Jun 15.
Artigo em Inglês | MEDLINE | ID: mdl-38885802

RESUMO

Infection with Vibrio mimicus in the Siluriformes has demonstrated a rapid and high infectivity and mortality rate, distinct from other hosts. Our earlier investigations identified necrosis, an inflammatory storm, and tissue remodeling as crucial pathological responses in yellow catfish (Pelteobagrus fulvidraco) infected with V. mimicus. The objective of this study was to further elucidate the impact linking these pathological responses within the host during V. mimicus infection. Employing metabolomics and transcriptomics, we uncovered infection-induced dense vacuolization of perimysium; Several genes related to nucleosidase and peptidase activities were significantly upregulated in the skin and muscles of infected fish. Concurrently, the translation processes of host cells were impaired. Further investigation revealed that V. mimicus completes its infection process by enhancing its metabolism, including the utilization of oligopeptides and nucleotides. The high susceptibility of yellow catfish to V. mimicus infection was associated with the composition of its body surface, which provided a microenvironment rich in various nucleotides such as dIMP, dAMP, deoxyguanosine, and ADP, in addition to several amino acids and peptides. Some of these metabolites significantly boost V. mimicus growth and motility, thus influencing its biological functions. Furthermore, we uncovered an elevated expression of gangliosides on the surface of yellow catfish, aiding V. mimicus adhesion and increasing its infection risk. Notably, we observed that the skin and muscles of yellow catfish were deficient in over 25 polyunsaturated fatty acids, such as Eicosapentaenoic acid, 12-oxo-ETE, and 13-Oxo-ODE. These substances play a role in anti-inflammatory mechanisms, possibly contributing to the immune dysregulation observed in yellow catfish. In summary, our study reveals a host immune deviation phenomenon that promotes bacterial colonization by increasing nutrient supply. It underscores the crucial factors rendering yellow catfish highly susceptible to V. mimicus, indicating that host nutritional sources not only enable the establishment and maintenance of infection within the host but also aid bacterial survival under immune pressure, ultimately completing its lifecycle.

4.
ACS Appl Mater Interfaces ; 16(22): 28473-28481, 2024 Jun 05.
Artigo em Inglês | MEDLINE | ID: mdl-38785067

RESUMO

Metallic iron (Fe) typically demonstrates the unfavorable catalytic activity for the CO2 reduction reaction (CO2RR), mainly attributed to the excessively strong binding of CO products on Fe sites. Toward this end, we employed an effective approach involving electronic structure modulation through nitrogen (N) integration to enhance the performance of the CO2RR. Here, an efficient catalyst has been developed, composed of N-doped metallic iron (Fe) nanoparticles encapsulated in a porous N-doped carbon framework. Notably, this N-integrated Fe catalyst displays significantly enhanced performance in the electrocatalytic reduction of CO2, yielding the highest CO Faradaic efficiency of 97.5% with a current density of 6.68 mA cm-2 at -0.7 V versus the reversible hydrogen electrode. The theoretical calculations, combined with the in situ attenuated total reflection surface-enhanced infrared absorption spectroscopy study, reveal that N integration modulates the electron density around Fe, resulting in the weakening of the binding strength between the Fe active sites and *CO intermediates, consequently promoting the desorption of CO and the overall CO2RR process.

5.
Adv Sci (Weinh) ; : e2401514, 2024 May 02.
Artigo em Inglês | MEDLINE | ID: mdl-38696613

RESUMO

Layered oxides of sodium-ion batteries suffer from severe side reactions on the electrode/electrolyte interface, leading to fast capacity degradation. Although surface reconstruction strategies are widely used to solve the above issues, the utilization of the low-cost wet chemical method is extremely challenging for moisture-sensitive Na-based oxide materials. Here, the solvation tuning strategy is proposed to overcome the deterioration of NaNi1/3Mn1/3Fe1/3O2 in water-based solution and conduct the surface reconstruction. When capturing the water molecules by the solvation structure of cations, here is Li+, the structural collapse and degradation of layered oxides in water-based solvents are greatly mitigated. Furthermore, Li(H2O)3EA+ promotes the profitable Li+/Na+ exchange to build a robust surface, which hampers the decomposition of electrolytes and the structural evolution upon cycling. Accordingly, the lifespan of Li-reinforced materials is prolonged to three times that of the pristine one. This work represents a step forward in understanding the surface reconstruction operated in a water-based solution for high-performance sodium layered oxide cathodes.

6.
Water Res ; 254: 121355, 2024 May 01.
Artigo em Inglês | MEDLINE | ID: mdl-38430755

RESUMO

Stormwater harvesting (SWH) addresses the UN's Sustainable Development Goals (SDGs). Conventional stormwater control measures (SCMs) effectively remove particulate and colloidal contaminants from urban runoff; however, they fail to retain dissolved contaminants, particularly substances of concern like polycyclic aromatic hydrocarbons (PAHs) and heavy metals (HMs), thereby hindering the SWH applicability. Here, inspired by protein folding in nature, we reported a novel biomimetic SCM for the efficient removal of dissolved PAHs and HMs from urban runoff. Lab-scale tests were conducted together with a more mechanistic investigation on how the contaminants were removed. By integrating hydrophobic organic chains with low-cost hydrophilic flocculant matrixes, our biomimetic flocculants achieved a 1.4-9.5 times removal of all detected dissolved PAHs and HMs, while enhancing the removal of a wide-spectrum of particulate and colloidal contaminants, compared to existing SCMs. Ecotoxicity, as indicated by newborn Daphnia magna as experimental organisms, was reduced from "acute toxicity" of the original runoff sample (toxic unit of ∼2.6) to "non-toxicity" (toxic unit < 0.4) of the treated water. The improved performance is attributed to the protein-folding-like features of the bioinspired flocculants providing: (i) stronger binding to PAHs (via hydrophobic association) and HMs (via coordination), and (ii) the ability of spontaneous aggregation. The bio-inspired approach in this work holds strong promise as an alternative or supplementary component in SCM systems, and is expected to contribute to sustainable water management practices in relation to SDGs.


Assuntos
Metais Pesados , Hidrocarbonetos Policíclicos Aromáticos , Poluentes Químicos da Água , Hidrocarbonetos Policíclicos Aromáticos/análise , Poluentes Químicos da Água/química , Monitoramento Ambiental , Metais Pesados/análise
8.
Nanomaterials (Basel) ; 14(3)2024 Jan 23.
Artigo em Inglês | MEDLINE | ID: mdl-38334510

RESUMO

The utilization of renewable energy for hydrogen production presents a promising pathway towards achieving carbon neutrality in energy consumption. Water electrolysis, utilizing pure water, has proven to be a robust technology for clean hydrogen production. Recently, seawater electrolysis has emerged as an attractive alternative due to the limitations of deep-sea regions imposed by the transmission capacity of long-distance undersea cables. However, seawater electrolysis faces several challenges, including the slow kinetics of the oxygen evolution reaction (OER), the competing chlorine evolution reaction (CER) processes, electrode degradation caused by chloride ions, and the formation of precipitates on the cathode. The electrode and catalyst materials are corroded by the Cl- under long-term operations. Numerous efforts have been made to address these issues arising from impurities in the seawater. This review focuses on recent progress in developing high-performance electrodes and electrolyser designs for efficient seawater electrolysis. Its aim is to provide a systematic and insightful introduction and discussion on seawater electrolysers and electrodes with the hope of promoting the utilization of offshore renewable energy sources through seawater electrolysis.

9.
Animals (Basel) ; 14(3)2024 Jan 29.
Artigo em Inglês | MEDLINE | ID: mdl-38338079

RESUMO

Vibrio mimicus is a serious pathogen in aquatic animals, resulting in significant economic losses. The cAMP receptor protein (CRP) often acts as a central regulator in highly pathogenic pathogens. V. mimicus SCCF01 is a highly pathogenic strain isolated from yellow catfish; the crp gene deletion strain (Δcrp) was constructed by natural transformation to determine whether this deletion affects the virulence phenotypes. Their potential molecular connections were revealed by qRT-PCR analysis. Our results showed that the absence of the crp gene resulted in bacterial and colony morphological changes alongside decreases in bacterial growth, hemolytic activity, biofilm formation, enzymatic activity, motility, and cell adhesion. A cell cytotoxicity assay and animal experiments confirmed that crp contributes to V. mimicus pathogenicity, as the LD50 of the Δcrp strain was 73.1-fold lower compared to the WT strain. Moreover, qRT-PCR analysis revealed the inhibition of type II secretion system genes, flagellum genes, adhesion genes, and metalloproteinase genes in the deletion strain. This resulted in the virulence phenotype differences described above. Together, these data demonstrate that the crp gene plays a core regulatory role in V. mimicus virulence and pathogenicity.

10.
Adv Mater ; : e2311322, 2024 Jan 25.
Artigo em Inglês | MEDLINE | ID: mdl-38299450

RESUMO

Seawater electrolysis for hydrogen production is a sustainable and economical approach that can mitigate the energy crisis and global warming issues. Although various catalysts/electrodes with excellent activities have been developed for high-efficiency seawater electrolysis, their unsatisfactory durability, especially for anodes, severely impedes their industrial applications. In this review, attention is paid to the factors that affect the stability of anodes and the corresponding strategies for designing catalytic materials to prolong the anode's lifetime. In addition, two important aspects-electrolyte optimization and electrolyzer design-with respect to anode stability improvement are summarized. Furthermore, several methods for rapid stability assessment are proposed for the fast screening of both highly active and stable catalysts/electrodes. Finally, perspectives on future investigations aimed at improving the stability of seawater electrolysis systems are outlined.

11.
Phys Chem Chem Phys ; 26(5): 4505-4510, 2024 Jan 31.
Artigo em Inglês | MEDLINE | ID: mdl-38240530

RESUMO

There is a growing demand for high purity ethanol as an electronic chemical. The conventional distillation process is effective for separating ethanol from water but consumes a significant amount of energy. Selective membrane separation using the LTA-type molecular sieve has been introduced as an alternative. The density functional theory simulation indicates that aluminum (Al) sites are evenly distributed throughout the framework, while sodium (Na+) ions are preferentially located in the six-membered ring. The movement of ethanol molecules can cause Na+ ions to be transported towards the eight-membered ring, hindering the passage of ethanol through the channel. In contrast, the energy barrier for water molecules passing through the channel occupied by Na+ ions is significantly lower, leading to a high level of selectivity for ethanol-water separation.

12.
Adv Mater ; 36(2): e2306062, 2024 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-37907201

RESUMO

Although hydrogen gas (H2 ) storage might enable offshore renewable energy to be stored at scale, the commercialization of technology for H2 generation by seawater electrolysis depends upon the development of methods that avoid the severe corrosion of anodes by chloride (Cl- ) ions. Here, it is revealed that the stability of an anode used for seawater splitting can be increased by more than an order of magnitude by loading Ag nanoparticles on the catalyst surface. In experiments, an optimized NiFe-layered double hydroxide (LDH)@Ag electrode displays stable operation at 400 mA cm-2 in alkaline saline electrolyte and seawater for over 5000 and 2500 h, respectively. The impressive long-term durability is more than 20 times that of an unmodified NiFe-LDH anode. Meticulous characterization and simulation reveals that in the presence of an applied electric field, free Cl- ions react with oxidized Ag nanoparticles to form stable AgCl species, giving rise to the formation of a Cl- -free layer near the anode surface. Because of its simplicity and effectiveness, it is anticipated that the proposed strategy to immobilize chloride ions on the surface of an anode has the potential to become a crucial technology to control corrosion during large-scale electrolysis of seawater to produce hydrogen.

13.
Braz J Microbiol ; 55(1): 901-910, 2024 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-37999911

RESUMO

Sichuan is a significant aquaculture province in China, with a total aquaculture output of 1.72 × 106 tons in 2022. One of the most significant microorganisms hurting the Sichuan aquaculture is Aeromonas hydrophila, whose genotype and antibiotic resistance are yet unknown. This study isolated a total of 64 strains of A. hydrophila from various regions during September 2019 to June 2021 within Sichuan province, China. The technique of Multi-Locus Sequence Typing (MLST) was used for the purpose of molecular typing. Meanwhile, identification of antibiotic resistance phenotype and antibiotic resistance gene was performed. The findings of the study revealed that 64 isolates exhibited 29 sequence types (ST) throughout different regions in Sichuan, with 25 of these ST types being newly identified. Notably, the ST251 emerged as the predominant sequence type responsible for the pandemic. The resistance rate of isolated strains to roxithromycin was as high as 98.3%, followed by co-trimoxazole (87.5%), sulfafurazole (87.5%), imipenem (80%), amoxicillin (60%), and clindamycin (57.8%). Fifteen strains of A. hydrophila exhibited resistance to medicines across a minimum of three categories, suggesting the development of multidrug resistance in these isolates. A total of 63 ARGs were detected from the isolates, which mediated a range of antibiotic resistance mechanisms, with deactivation and efflux potentially serving as the primary mechanisms of antibiotic resistance. This study revealed the diversity of A. hydrophila genotypes and the risk of antibiotic resistance in Sichuan, providing reference for scientific and effective control of A. hydrophila infection.


Assuntos
Aeromonas hydrophila , Aeromonas , Aeromonas hydrophila/genética , Tipagem de Sequências Multilocus , Resistência Microbiana a Medicamentos , Genótipo , Fenótipo , Antibacterianos/farmacologia , China , Aeromonas/genética
14.
ACS Nano ; 17(14): 13948-13960, 2023 Jul 25.
Artigo em Inglês | MEDLINE | ID: mdl-37428219

RESUMO

Hydrogels with strong yet reversible mechanical and adhesive properties fabricated in a facile and friendly manner are important for engineering and intelligent electronics applications but are challenging to create and control. Existing approaches for preparing hydrogels involve complicated pretreatments and produce hydrogels that suffer from limited skin applicability. Copolymerized hydrogels are expected to present an intriguing target in this field by means of thermoresponsive features, while the perceived intrinsic flaws of brittleness, easy fracture, and weak adhesion enervate the development prospects. Herein, we report a hydrogel with strong yet reversible mechanical and adhesive properties using cellulose nanofibrils to simultaneously address multiple dilemmas inspired by a temperature-mediated phase separation strategy. This strategy applies temperature-driven formation and dissociation of hydrogen bonds between common copolymers and cellulose nanofibrils to trigger the onset and termination of phase separation for dynamically reversible on-demand properties. The resulting hydrogel exhibits up to 96.0% (117.2 J/m2 vs 4.8 J/m2 for interfacial toughness) and 85.7% (0.02 MPa vs 0.14 MPa for mechanical stiffness) adhesive and mechanical tunability when worked on skin, respectively. Our strategy offers a promising, simple, and efficient way to directly achieve robust adhesion performance in one step using common copolymers and biomass resources, with implications that could go beyond strong yet adhesive hydrogels.

15.
Biomed Pharmacother ; 165: 115026, 2023 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-37336148

RESUMO

This study sought to investigate the anti-amyloid ß (Aß) and anti-neuroinflammatory effects of catalpol in an Alzheimer's disease (AD) mouse model. METHODS: The effects of catalpol on Aß formation were investigated by thioflavin T assay. The effect of catalpol on generating inflammatory cytokines from microglial cells and the cytotoxicity of microglial cells on HT22 hippocampal cells were assessed by real-time quantitative PCR, ELISA, redox reactions, and cell viability. APPswe/PS1ΔE9 mice were treated with catalpol, and their cognitive ability was investigated using the water maze and novel object recognition tests. Immunohistochemistry and immunofluorescence were used to probe for protein markers of microglia and astrocyte, Aß deposits, and NF-κB pathway activity. Aß peptides, neuroinflammation, and nitric oxide production were examined using ELISA and redox reactions. RESULTS: Catalpol potently inhibited Aß fibril and oligomer formation. In microglial cells stimulated by Aß, catalpol alleviated the expression of the proinflammatory cytokines tumor necrosis factor-α (TNF-α), interleukin (IL)-6, and inducible nitric oxide synthase (iNOS) but promoted the expression of the anti-inflammatory cytokine IL-10. Catalpol alleviated the cytotoxic effects of Aß-exposed microglia on HT22 cells. Treatment with catalpol in APPswe/PS1ΔE9 mice downregulated neuroinflammation production, decreased Aß deposits in the brains and alleviated cognitive impairment. Catalpol treatment decreased the number of IBA-positive microglia and GFAP-positive astrocytes and their activities of the NF-κB pathway in the hippocampus of APPswe/PS1ΔE9 mice. CONCLUSION: The administration of catalpol protected neurons by preventing neuroinflammation and Aß deposits in an AD mouse model. Therefore, catalpol may be a promising strategy for treating AD.


Assuntos
Peptídeos beta-Amiloides , Disfunção Cognitiva , Medicamentos de Ervas Chinesas , Glucosídeos Iridoides , Doenças Neuroinflamatórias , Fármacos Neuroprotetores , Placa Amiloide , Medicamentos de Ervas Chinesas/farmacologia , Medicamentos de Ervas Chinesas/uso terapêutico , Glucosídeos Iridoides/farmacologia , Glucosídeos Iridoides/uso terapêutico , Disfunção Cognitiva/tratamento farmacológico , Placa Amiloide/tratamento farmacológico , Doenças Neuroinflamatórias/tratamento farmacológico , Animais , Camundongos , Modelos Animais de Doenças , Citocinas/metabolismo , Linhagem Celular , Fármacos Neuroprotetores/farmacologia , Fármacos Neuroprotetores/uso terapêutico , Peptídeos beta-Amiloides/antagonistas & inibidores , Camundongos Endogâmicos C57BL , Masculino , Feminino , Camundongos Transgênicos
16.
Small ; 19(38): e2302055, 2023 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-37222116

RESUMO

Heteroatoms Fe, F co-doped NiO hollow spheres (Fe, F-NiO) are designed, which simultaneously integrate promoted thermodynamics by electronic structure modulation with boosted reaction kinetics by nano-architectonics. Benefiting from the electronic structure co-regulation of Ni sites by introducing Fe and F atoms in NiO , as the rate-determined step (RDS), the Gibbs free energy of OH* intermediates (ΔGOH* ) for Fe, F-NiO catalyst is significantly decreased to 1.87 eV for oxygen evolution reaction (OER) compared with pristine NiO (2.23 eV), which reduces the energy barrier and improves the reaction activity. Besides, densities of states (DOS) result verifies the bandgap of Fe, F-NiO(100) is significantly decreased compared with pristine NiO(100), which is beneficial to promote electrons transfer efficiency in electrochemical system. Profiting by the synergistic effect, the Fe, F-NiO hollow spheres only require the overpotential of 215 mV for OER at 10 mA cm-2 and extraordinary durability under alkaline condition. The assembled Fe, F-NiO||Fe-Ni2 P system only needs 1.51 V to reach 10 mA cm-2 , also exhibits outstanding electrocatalytic durability for continuous operation. More importantly, replacing the sluggish OER by advanced sulfion oxidation reaction (SOR) not only can realize the energy saving H2 production and toxic substances degradation, but also bring additional economic benefits.

17.
Water Res ; 236: 119942, 2023 Jun 01.
Artigo em Inglês | MEDLINE | ID: mdl-37031529

RESUMO

Hydrophobic-modified flocculants have demonstrated considerable promise in the removal of emerging contaminants by flocculation. However, there is a lack of information about the impacts of dosing such flocculants on the performance of subsequent treatment unit(s) in the overall water treatment process. In this work, inspired by the ubiquitous protein folding phenomenon, an innovative approach using an elevated membrane cleaning temperature as the means to induce residual hydrophobic-modified chitosan flocculant (TRC), after flocculation-sedimentation, to reduce membrane fouling in a subsequent ultrafiltration was proposed; this was evaluated in a continuous flocculation-sedimentation-ultrafiltration (FSUF) process treating samples of the Yangtze River. The hydrophobic chains of TRC had similar temperature-dependent hydrophobicity to those of natural proteins. In the 40-day operation of the FSUF system with combined dosing of alum and TRC, a moderately elevated cleaning water temperature (45 °C) of both backwash with air-bubbling and soaking with sponge-scrubbing cleaning, significantly reduced reversible and irreversible fouling resistance by 49.8%∼61.3% and 73.9%∼83.3%, respectively, compared to the system using cleaning water at 25 °C. Material flow analysis, statistical analysis, instrumental characterizations, and computational simulations, showed that the enhanced fouling mitigation originated from three factors: the reduced contaminant accumulation onto membranes, the strengthened membrane-surface-modification role of TRC, and the weakened structure of the fouling material containing TRC, at the elevated cleaning temperature. Other measures of the performance, these being water purification, membrane stability and economic aspects, also confirmed the potential and feasibility of the proposed approach. This work has provided new insights into the role of hydrophobic-modified flocculants in membrane fouling control, in addition to emerging contaminant removal, in a FSUF surface water treatment process.


Assuntos
Membranas Artificiais , Purificação da Água , Floculação , Temperatura , Ultrafiltração , Interações Hidrofóbicas e Hidrofílicas , Dobramento de Proteína
18.
Chem Commun (Camb) ; 59(39): 5874-5877, 2023 May 11.
Artigo em Inglês | MEDLINE | ID: mdl-37089054

RESUMO

We synthesized three soluble perinone isomers as electron transport materials in p-i-n perovskite solar cells. The cis-isomer BBIN-2 possesses higher LUMO level and electron mobility than the trans-isomers. The BBIN-2 devices showed the highest power conversion efficiency of 19.36%, demonstrating the potential of perinone dyes in perovskite solar cells.

19.
Artigo em Inglês | MEDLINE | ID: mdl-36762445

RESUMO

Ni-rich layered LiNixCoyAlzO2 (NCA, x ≥ 0.8) oxides have attracted wide attention as cathode materials for lithium-ion batteries due to their higher energy density and lower cost. However, the increase in the capacity for Ni-rich cathodes can cause faster capacity decay and increase sensitivity to ambient air exposure during the storage process. Especially, the residual lithium on the surface of Ni-rich cathodes will cause severe flatulence during cycling which greatly reduces the safety performance of the battery. Washing is an effective method to reduce residual lithium, but it will seriously damage the surface phase structure of Ni-rich materials. Here, we introduce a designed method involving two steps, washing and high-temperature annealing, which can ingeniously modify the surface phase structure of Ni-rich cathodes. The results show that the residual lithium content can be significantly reduced. The thin NiO-like rock-salt phase formed on the surface of Ni-rich cathode annealed at 600 °C improves the diffusion kinetics of Li+, reduces the polarization, and improves the electrochemical performance of Ni-rich materials, while the thick spinel-like phase formed at 400 °C hinders the diffusion kinetics of Li+, significantly increases the polarization, and eventually leads to the structural degradation of Ni-rich materials. As a result, the discharge capacity of the cathode annealed at 600 °C still retains 174.48 mA h g-1 after 100 cycles, with a capacity retention of 92.04%, much larger than the cathode annealed at 400 °C, for which the discharge capacity drops to 107.77 mA h g-1, with a capacity retention of 65.78%.

20.
Nano Lett ; 23(1): 227-234, 2023 Jan 11.
Artigo em Inglês | MEDLINE | ID: mdl-36535024

RESUMO

Sulfide solid electrolyte membranes employed in all-solid-state lithium batteries generally show high thickness and poor chemical stability, which limit the cell-level energy density and cycle life. In this work, Li9.88GeP1.96Sb0.04S11.88Cl0.12 solid electrolyte is synthesized with Sb, Cl partial substitution of P, S, possessing excellent toluene tolerance and stability to lithium. The formed SbS43- group in Li9.88GeP1.96Sb0.04S11.88Cl0.12 exhibits low adsorption energy and reactivity for toluene molecules, confirmed by first-principles density functional theory calculation. Using toluene as the solvent, ultrathin Li9.88GeP1.96Sb0.04S11.88Cl0.12 membranes with adjustable thicknesses can be well prepared by the wet coating method, and an 8 µm thick membrane exhibits an ionic conductivity of 1.9 mS cm-1 with ultrahigh ionic conductance of 1860 mS and ultralow areal resistance of 0.68 Ω cm-2 at 25 °C. The obtained LiCoO2|Li9.88GeP1.96Sb0.04S11.88Cl0.12 membrane|Li all-solid-state lithium battery shows an initial reversible capacity of 125.6 mAh g-1 with a capacity retention of 86.3% after 250 cycles at 0.1 C under 60 °C.

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