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1.
Sci Immunol ; 9(99): eadp3475, 2024 Sep 20.
Artigo em Inglês | MEDLINE | ID: mdl-39303018

RESUMO

Heat is a cardinal feature of inflammation, yet its impacts on immune cells remain uncertain. We show that moderate-grade fever temperatures (39°C) increased murine CD4 T cell metabolism, proliferation, and inflammatory effector activity while decreasing regulatory T cell suppressive capacity. However, heat-exposed T helper 1 (TH1) cells selectively developed mitochondrial stress and DNA damage that activated Trp53 and stimulator of interferon genes pathways. Although many TH1 cells subjected to such temperatures died, surviving TH1 cells exhibited increased mitochondrial mass and enhanced activity. Electron transport chain complex 1 (ETC1) was rapidly impaired under fever-range temperatures, a phenomenon that was specifically detrimental to TH1 cells. TH1 cells with elevated DNA damage and ETC1 signatures were also detected in human chronic inflammation. Thus, fever-relevant temperatures disrupt ETC1 to selectively drive apoptosis or adaptation of TH1 cells to maintain genomic integrity and enhance effector functions.


Assuntos
Dano ao DNA , Febre , Inflamação , Mitocôndrias , Animais , Dano ao DNA/imunologia , Camundongos , Inflamação/imunologia , Febre/imunologia , Humanos , Mitocôndrias/imunologia , Camundongos Endogâmicos C57BL , Células Th1/imunologia , Feminino , Masculino
2.
Nanomicro Lett ; 17(1): 22, 2024 Sep 27.
Artigo em Inglês | MEDLINE | ID: mdl-39331215

RESUMO

High-entropy materials represent a new category of high-performance materials, first proposed in 2004 and extensively investigated by researchers over the past two decades. The definition of high-entropy materials has continuously evolved. In the last ten years, the discovery of an increasing number of high-entropy materials has led to significant advancements in their utilization in energy storage, electrocatalysis, and related domains, accompanied by a rise in techniques for fabricating high-entropy electrode materials. Recently, the research emphasis has shifted from solely improving the performance of high-entropy materials toward exploring their reaction mechanisms and adopting cleaner preparation approaches. However, the current definition of high-entropy materials remains relatively vague, and the preparation method of high-entropy materials is based on the preparation method of single metal/low- or medium-entropy materials. It should be noted that not all methods applicable to single metal/low- or medium-entropy materials can be directly applied to high-entropy materials. In this review, the definition and development of high-entropy materials are briefly reviewed. Subsequently, the classification of high-entropy electrode materials is presented, followed by a discussion of their applications in energy storage and catalysis from the perspective of synthesis methods. Finally, an evaluation of the advantages and disadvantages of various synthesis methods in the production process of different high-entropy materials is provided, along with a proposal for potential future development directions for high-entropy materials.

3.
Nat Methods ; 2024 Sep 25.
Artigo em Inglês | MEDLINE | ID: mdl-39322753

RESUMO

The development of single-cell multi-omics technology has greatly enhanced our understanding of biology, and in parallel, numerous algorithms have been proposed to predict the protein abundance and/or chromatin accessibility of cells from single-cell transcriptomic information and to integrate various types of single-cell multi-omics data. However, few studies have systematically compared and evaluated the performance of these algorithms. Here, we present a benchmark study of 14 protein abundance/chromatin accessibility prediction algorithms and 18 single-cell multi-omics integration algorithms using 47 single-cell multi-omics datasets. Our benchmark study showed overall totalVI and scArches outperformed the other algorithms for predicting protein abundance, and LS_Lab was the top-performing algorithm for the prediction of chromatin accessibility in most cases. Seurat, MOJITOO and scAI emerge as leading algorithms for vertical integration, whereas totalVI and UINMF excel beyond their counterparts in both horizontal and mosaic integration scenarios. Additionally, we provide a pipeline to assist researchers in selecting the optimal multi-omics prediction and integration algorithm.

4.
Int J Mol Sci ; 25(17)2024 Sep 09.
Artigo em Inglês | MEDLINE | ID: mdl-39273690

RESUMO

Cytoplasmic male sterility (CMS) is important for commercial hybrid seed production. However, it is still not used in eggplant (Solanum melongena L.), and corresponding regulatory genes and mechanisms of action have not been reported. We report CMS line 327A, which was derived from the hybridization between cultivated and wild eggplants. By looking at different stages of anther development under a microscope, we saw that the 327A anther's tapetum layer vacuolized during meiosis, which caused abortion. To investigate the 327A CMS regulatory genes, the mitochondrial genomes of 327A and its maintainer line 327B were assembled de novo. It was found that 15 unique ORFs (Open Reading Frame) were identified in 327A. RT-PCR and RT-QPCAR tests confirmed that orf312a and orf172a, 327A-specific ORFs with a transmembrane domain, were strongly expressed in sterile anthers of 327A. In addition, orf312a has a chimeric structure with the ribosomal protein subunit rpl16. Therefore, orf312a and orf172a can be considered strong candidate genes for CMS. Concurrently, we analyzed the characteristics of CMS to develop a functional molecular marker, CMS312, targeting a future theoretical basis for eggplant CMS three-line molecular breeding.


Assuntos
Genoma Mitocondrial , Infertilidade das Plantas , Solanum melongena , Solanum melongena/genética , Infertilidade das Plantas/genética , Fases de Leitura Aberta/genética , Regulação da Expressão Gênica de Plantas , Citoplasma/genética , Citoplasma/metabolismo , Genes de Plantas
5.
Inorg Chem ; 63(37): 17166-17175, 2024 Sep 16.
Artigo em Inglês | MEDLINE | ID: mdl-39221868

RESUMO

Recycling spent lithium-ion batteries (LIBs) in a green and economical way is vital for maintaining the sustainability of the LIB industry. However, given the low content of high-value components in olivine-type lithium iron phosphate (LFP), traditional metallurgical processes are economically unfeasible for recycling due to high chemical/energy consumption and labor-intensive procedures. This study proposes a facile electrochemistry strategy to directly regenerate the spent LFP material by an electrically driven lithiation process as a spent LFP slurry (200 g/L) rather than as electrodes. Minimal energy and chemical consumption are achieved by enabling the healing of spent LFP without destroying the original olivine-type crystal structure. The proposed method utilizes mild healing conditions (25 °C for 2 h) and LiCl solution as the only reagent in the regeneration process, significantly lowering the expenses associated with producing cathode electrodes. The electrochemical performance of the regenerated LFP have been dramatically recovered after regeneration, exhibiting a capacity of 151.5 mA h g-1 at 0.1 C and 96.6% capacity retention over 400 cycles at 1 C. This approach demonstrates a high processing capability and offers considerable economic and environmental benefits, making it an eco-friendly option and supporting the sustainable development of the LFP industry.

6.
J Phys Chem Lett ; 15(33): 8434-8443, 2024 Aug 22.
Artigo em Inglês | MEDLINE | ID: mdl-39119908

RESUMO

Metallic zinc has been regarded as an ideal anode material for aqueous batteries due to its high capacity, abundance, and low toxicity. Numerous strategies have been proposed for anode protection to address its intrinsic deficiencies. However, existing methods can only suppress dendrite growth at limited current densities, and achieving stable cycling at high rates remains a great challenge. Herein, density functional theory (DFT) reveals that Mn-MOF, with a distinctive π-π stacking structure (π-MOF), can induce accelerated ion transfer dynamics, providing high-speed pathways for Zn2+ flux, which can enable stable deposition even at high rates. As anticipated, the π-MOF@Zn anode exhibits remarkable stability for over 1900 h with the lowest voltage hysteresis (71 mV) at a current density of 10 mA cm-2. This study presents a viable approach to enhance the interface stability of high-rate metal anodes by modulating charge or ion behavior at the interface.

7.
ACS Nano ; 18(36): 25053-25068, 2024 Sep 10.
Artigo em Inglês | MEDLINE | ID: mdl-39177338

RESUMO

The carbon coating strategy has emerged as an indispensable approach to improve the conductivity of polyanionic cathodes. However, owing to the complex reaction process between precursors of carbon and cathode, establishing a unified screening principle for carbonaceous precursors remains a technical challenge. Herein, we reveal that carbonaceous precursor pyrolysis chemistry undeniably influences the formation process and performance of Na3V2(PO4)3 (NVP) cathodes from in situ insights. By investigating three types of carbonaceous precursors, it is found that O/H-containing functional groups can provide more bonding sites for cathode precursors and generate a reducing atmosphere by pyrolysis, which is beneficial to the formation of polyanionic materials and a uniform carbon coating layer. Conversely, excessive pyrolysis of functional groups leads to a significant amount of gas, which is detrimental to the compactness of the carbon layer. Furthermore, the substantial presence of residual heteroatoms diminishes graphitization. In this case, it is demonstrated that carbon dots (CDs) precursors with suitable functional groups can comprehensively enhance the Na+ migration rate, reversibility, and interface stability of the cathode material. As a result, the NVP/CDs cathode displays outstanding capacity retention, maintaining 92% after 10,000 cycles at a high rate of 50 C. Altogether, these findings provide a valuable benchmark for carbon source selection for polyanionic cathodes.

8.
Chem Commun (Camb) ; 60(70): 9384-9387, 2024 Aug 27.
Artigo em Inglês | MEDLINE | ID: mdl-39132718

RESUMO

Direct regeneration is an effective strategy of spent lithium iron phosphate (S-LFP), with the principal aspect being the selection of the lithium source and reductant. Here, assisted with a thermodynamically favourable reaction involving a bifunctional organic lithium salt (lithium citrate), the single-step regeneration of S-LFP is successfully achieved. The structure and composition of the regenerated LFP are significantly restored, demonstrating excellent electrochemical performance (142.7 mA h g-1) with no degradation after 200 cycles.

9.
ACS Nano ; 18(34): 23773-23784, 2024 Aug 27.
Artigo em Inglês | MEDLINE | ID: mdl-39141003

RESUMO

Al impurity is among the most likely components to enter the spent lithium-ion battery (LIB) cathode powder due to the strong adhesion between the cathode material and the Al current collector. However, high-value metal elements tend to be lost during the deep removal of Al impurities to obtain high-purity metal salt products in the conventional hydrometallurgical process. In this work, the harmful Al impurity is designed as a beneficial ingredient to upcycle high-voltage LiCoO2 by incorporating robust Al-O covalent bonds into the bulk of the cathode assisted with Ti modification. Benefiting from the strong Al-O and Ti-O bonds in the bulk, the irreversible phase transitions of the upcycled R-LCO-AT have been significantly suppressed at high voltages, as revealed by in situ XRD. Moreover, a Li+-conductive Li2TiO3 protective layer is constructed on the surface of R-LCO-AT by pinning slow-diffusion Ti on the grain boundaries, resulting in improved Li+ diffusion kinetics and restrained interface side reactions. Consequently, the cycle stability and rate performance of R-LCO-AT were significantly enhanced at a high cutoff voltage of 4.6 V, with a discharge capacity of 189.5 mAhg-1 at 1 C and capacity retention of 92.9% over 100 cycles at 4.6 V. This study utilizes the detrimental impurity element to upcycle high-voltage LCO cathodes through an elaborate bulk/surface structural design, offering a strategy for the high-value utilization of spent LIBs.

10.
J Phys Chem Lett ; 15(34): 8628-8635, 2024 Aug 29.
Artigo em Inglês | MEDLINE | ID: mdl-39150409

RESUMO

Polycrystalline lithium manganese oxide (LMO) is known to suffer from severe surface structure degradation and electrochemical polarization due to its mixed crystal plane orientations. A hexagonal prism single-crystal LMO (LMOS-HP), engineered through the SrO-induced preferential growth effect, features the most stable {111} top surfaces and the fastest Li+ diffusion {110} side surfaces, effectively addressing these challenges. Consequently, LMOS-HP exhibits superior electrochemical capability, with only 0.021% capacity fading per cycle after 500 cycles and achieves a discharge capacity of 81.9 mAh g-1 at 20C. This innovative design offers a promising approach for tuning surface crystal orientation to improve performance.

11.
Angew Chem Int Ed Engl ; 63(40): e202410420, 2024 Oct 01.
Artigo em Inglês | MEDLINE | ID: mdl-38961660

RESUMO

The structural failure of Na2Mn[Fe(CN)6] could not be alleviated with traditional modification strategies through the adjustable composition property of Prussian blue analogues (PBAs), considering that the accumulation and release of stress derived from the MnN6 octahedrons are unilaterally restrained. Herein, a novel application of adjustable composition property, through constructing a coordination competition relationship between chelators and [Fe(CN)6]4- to directionally tune the enrichment of elements, is proposed to restrain structural degradation and induce unconventional energy coupling phenomenon. The non-uniform distribution of elements at the M1 site of PBAs (NFM-PB) is manipulated by the sequentially precipitated Ni, Fe, and Mn according to the Irving-William order. Electrochemically active Fe is operated to accompany Mn, and zero-strain Ni is modulated to enrich at the surface, synergistically mitigating with the enrichment and release of stress and then significantly improving the structural stability. Furthermore, unconventional energy coupling effect, a fusion of the electrochemical behavior between FeLS and MnHS, is triggered by the confined element distribution, leading to the enhanced electrochemical stability and anti-polarization ability. Consequently, the NFM-PB demonstrates superior rate performance and cycling stability. These findings further exploit potentialities of the adjustable composition property and provide new insights into the component design engineering for advanced PBAs.

12.
Angew Chem Int Ed Engl ; 63(41): e202409044, 2024 Oct 07.
Artigo em Inglês | MEDLINE | ID: mdl-39005168

RESUMO

The practical application of solid polymer electrolyte is hindered by the small transference number of Li+, low ionic conductivity and poor interfacial stability, which are seriously determined by the microenvironment in polymer electrolyte. The introduction of functional fillers is an effective solution to these problems. In this work, based on density functional theory (DFT) calculations, it is demonstrated that the anion vacancy of filler can anchor anions of lithium salt, thereby significantly increasing the transference number of Li+ in the electrolyte. Therefore, flower-like SnS2-based filler with abundant sulfur vacancies is prepared under the regulation of functionalized carbon dots (CDs). It is worth mentioning that the CDs dotted on the surface of SnS2 have rich organic functional groups, which can serve as the bridging agent to enhance the compatibility of filler and polymer, leading to superior mechanical performance and fast ion transport pathway. Additionally, the in situ formed Li2S/Li3N at the interface of Li metal and electrolyte facilitate the fast Li+ diffusion and uniform Li deposition, effectively mitigating the growth of lithium dendrites. As a result, the assembled lithium metal batteries exhibit excellent cycling stability, reflecting the superiority of the carbon dots derived vacancy-rich inorganic filler modification strategy.

13.
Small ; : e2403736, 2024 Jul 11.
Artigo em Inglês | MEDLINE | ID: mdl-38990899

RESUMO

Transition metal selenides (TMSs) are receiving considerable interest as improved anode materials for sodium-ion batteries (SIBs) and lithium-ion batteries (LIBs) due to their considerable theoretical capacity and excellent redox reversibility. Herein, ZIF-12 (zeolitic imidazolate framework) structure is used for the synthesis of Cu2Se/Co3Se4@NPC anode material by pyrolysis of ZIF-12/Se mixture. When Cu2Se/Co3Se4@NPC composite is utilized as an anode electrode material in LIB and SIB half cells, the material demonstrates excellent electrochemical performance and remarkable cycle stability with retaining high capacities. In LIB and SIB half cells, the Cu2Se/Co3Se4@NPC anode material shows the ultralong lifespan at 2000 mAg-1, retaining a capacity of 543 mAhg-1 after 750 cycles, and retaining a capacity of 251 mAhg-1 after 200 cycles at 100 mAg-1, respectively. The porous structure of the Cu2Se/Co3Se4@NPC anode material can not only effectively tolerate the volume expansion of the electrode during discharging and charging, but also facilitate the penetration of electrolyte and efficiently prevents the clustering of active particles. In situ X-ray difraction (XRD) analysis results reveal the high potential of Cu2Se/Co3Se4@NPC composite in building efficient LIBs and SIBs due to reversible conversion reactions of Cu2Se/Co3Se4@NPC for lithium-ion and sodium-ion storage.

14.
ACS Nano ; 2024 Jul 29.
Artigo em Inglês | MEDLINE | ID: mdl-39074061

RESUMO

On the basis of the sustainable concept, organic compounds and carbon materials both mainly composed of light C element have been regarded as powerful candidates for advanced electrochemical energy storage (EES) systems, due to theie merits of low cost, eco-friendliness, renewability, and structural versatility. It is investigated that the carbonyl functionality as the most common constituent part serves a crucial role, which manifests respective different mechanisms in the various aspects of EES systems. Notably, a systematical review about the concept and progress for carbonyl chemistry is beneficial for ensuring in-depth comprehending of carbonyl functionality. Hence, a comprehensive review about carbonyl chemistry has been summarized based on state-of-the-art developments. Moreover, the working principles and fundamental properties of the carbonyl unit have been discussed, which has been generalized in three aspects, including redox activity, the interaction effect, and compensation characteristic. Meanwhile, the pivotal characterization technologies have also been illustrated for purposefully studying the related structure, redox mechanism, and electrochemical performance to profitably understand the carbonyl chemistry. Finally, the current challenges and promising directions are concluded, aiming to afford significant guidance for the optimal utilization of carbonyl moiety and propel practicality in EES systems.

15.
Adv Mater ; : e2406905, 2024 Jul 31.
Artigo em Inglês | MEDLINE | ID: mdl-39081118

RESUMO

Lithium carbon dioxide (Li-CO2) batteries, noted for their high discharge voltage of approximately 2.8 V and substantial theoretical specific energy of 1876 Wh kg-1, represent a promising avenue for new energy sources and CO2 emission reduction. However, the practical application of these batteries faces significant hurdles, particularly at high current densities and over extended cycle lives, due to their complex reaction mechanisms and slow kinetics. This paper delves into the recent advancements in cathode catalysts for Li-CO2 batteries, with a specific focus on the designing philosophy from composition, geometry, and homogeneity of the catalysts to the proper test conditions and real-world application. It surveys the possible catalytic mechanisms, giving readers a brief introduction of how the energy is stored and released as well as the critical exploration of the relationship between material properties and performances. Specifically, optimization and standardization of test conditions for Li-CO2 battery research is highlighted to enhance data comparability, which is also critical to facilitate the practical application of Li-CO2 batteries. This review aims to bring up inspiration from previous work to advance the design of more effective and sustainable cathode catalysts, tailored to meet the practical demands of Li-CO2 batteries.

16.
J Phys Chem Lett ; 15(26): 6743-6749, 2024 Jul 04.
Artigo em Inglês | MEDLINE | ID: mdl-38912658

RESUMO

Layered sodium transition-metal oxides generally encounter severe capacity decay and inferior rate performance during cycling, especially at a high state of charge. Herein, defect concentration is rationally modulated to explore the impact on electrochemical behavior in NaNi1/3Fe1/3Mn1/3O2 layered oxides. Bulk vacancies are increased through annealing in an oxygen-rich atmosphere, demonstrated by electron paramagnetic resonance measurement. It is found that the cathode with enriched oxygen vacancies exhibits significantly enhanced reversibility of redox reactions with a higher initial Coulombic efficiency of 90.0%. Furthermore, the reduced volume variations during the initial charge/discharge process are also confirmed by in situ X-ray diffraction. As a result, the oxygen-vacancy-rich cathode shows great cycling stability and superior rate performances. Also, full cells deliver a specific capacity of approximately 145.2 mAh g-1 at 0.5 C, with a high capacity retention of 78.3% after 100 cycles. This work presents a viable strategy for designing Na+ intercalated cathodes with a high-energy density.

17.
ACS Nano ; 18(26): 16468-16488, 2024 Jul 02.
Artigo em Inglês | MEDLINE | ID: mdl-38900494

RESUMO

Sodium-ion batteries (SIBs) have significant potential for applications in portable electric vehicles and intermittent renewable energy storage due to their relatively low cost. Currently, hard carbon (HC) materials are considered commercially viable anode materials for SIBs due to their advantages, including larger capacity, low cost, low operating voltage, and inimitable microstructure. Among these materials, renewable biomass-derived hard carbon anodes are commonly used in SIBs. However, the reports about biomass hard carbon from basic research to industrial applications are very rare. In this paper, we focus on the research progress of biomass-derived hard carbon materials from the following perspectives: (1) sodium storage mechanisms in hard carbon; (2) optimization strategies for hard carbon materials encompassing design, synthesis, heteroatom doping, material compounding, electrolyte modulation, and presodiation; (3) classification of different biomass-derived hard carbon materials based on precursor source, a comparison of their properties, and a discussion on the effects of different biomass sources on hard carbon material properties; (4) challenges and strategies for practical of biomass-derived hard carbon anode in SIBs; and (5) an overview of the current industrialization of biomass-derived hard carbon anodes. Finally, we present the challenges, strategies, and prospects for the future development of biomass-derived hard carbon materials.

18.
Chem Commun (Camb) ; 60(57): 7370-7373, 2024 Jul 11.
Artigo em Inglês | MEDLINE | ID: mdl-38920095

RESUMO

A separator modification strategy was proposed by placing nitrogen-doped carbon fibers (NCF700) in the middle of the separator to prevent direct contact between the coating and the rigid zinc metal anode, resulting in coating cracks. The NCF700 coating can homogenize the electric field distribution and increase the transference number of zinc ions. Therefore, the battery assembled with the NCF700 coated separator exhibits superior cycling stability compared to the bare separator.

19.
Angew Chem Int Ed Engl ; 63(36): e202410016, 2024 Sep 02.
Artigo em Inglês | MEDLINE | ID: mdl-38896116

RESUMO

Garnet solid-state electrolyte Li6.5La3Zr1.5Ta0.5O12 (LLZTO) holds significant promise. However, the practical utilization has been seriously impeded by the poor contact of Li|garnet and electron leakage. Herein, one new type of garnet-based solid-state battery is proposed with high performance through the disparity in interfacial energy, induced by the reaction between trace fluorinated carbon dots (FCDs) and Li. The work of adhesion of Li|garnet is increased by the acquired Li-FCD composite, which facilitates an intimate Li|garnet interface with the promoted uniform Li+ deposition, revealed by density functional theory (DFT) calculations. It is further validated that a concentrated C-Li2O-LiF component at the Li|garnet interface is spontaneously constructed, due to the significant disparity in interfacial energy between C-Li2O-LiF|LLZTO and C-Li2O-LiF|Li. Furthermore, The electron transport and Li dendrites penetration are effectively hindered by the formed Li2O and LiF. The Li-FCD|LLZTO|Li-FCD symmetrical cells demonstrate stable cycling performance for over 3000 hours at 0.3 mA cm-2 and 800 hours at 0.5 mA cm-2. Furthermore, the LFP|garnet|Li-FCD full cell exhibits remarkable cycling performance (91.6 % capacity retention after 500 cycles at 1 C). Our research has revealed a novel approach to establish a dendrite-free Li|garnet interface, laying the groundwork for future advancements in garnet-based solid-state batteries.

20.
ACS Nano ; 18(20): 13150-13163, 2024 May 21.
Artigo em Inglês | MEDLINE | ID: mdl-38726816

RESUMO

Layered sodium transition-metal (TM) oxides generally suffer from severe capacity decay and poor rate performance during cycling, especially at a high state of charge (SoC). Herein, an insight into failure mechanisms within high-voltage layered cathodes is unveiled, while a two-in-one tactic of charge localization and coherent structures is devised to improve structural integrity and Na+ transport kinetics, elucidated by density functional theory calculations. Elevated Jahn-Teller [Mn3+O6] concentration on the particle surface during sodiation, coupled with intense interlayer repulsion and adverse oxygen instability, leads to irreversible damage to the near-surface structure, as demonstrated by X-ray absorption spectroscopy and in situ characterization techniques. It is further validated that the structural skeleton is substantially strengthened through the electronic structure modulation surrounding oxygen. Furthermore, optimized Na+ diffusion is effectively attainable via regulating intergrown structures, successfully achieved by the Zn2+ inducer. Greatly, good redox reversibility with an initial Coulombic efficiency of 92.6%, impressive rate capability (86.5 mAh g-1 with 70.4% retention at 10C), and enhanced cycling stability (71.6% retention after 300 cycles at 5C) are exhibited in the P2/O3 biphasic cathode. It is believed that a profound comprehension of layered oxides will herald fresh perspectives to develop high-voltage cathode materials for sodium-ion batteries.

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