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1.
Nature ; 616(7956): 300-305, 2023 04.
Artículo en Inglés | MEDLINE | ID: mdl-36927804

RESUMEN

Achieving food-system sustainability is a multidimensional challenge. In China, a doubling of crop production since 1990 has compromised other dimensions of sustainability1,2. Although the country is promoting various interventions to enhance production efficiency and reduce environmental impacts3, there is little understanding of whether crop switching can achieve more sustainable cropping systems and whether coordinated action is needed to avoid tradeoffs. Here we combine high-resolution data on crop-specific yields, harvested areas, environmental footprints and farmer incomes to first quantify the current state of crop-production sustainability. Under varying levels of inter-ministerial and central coordination, we perform spatial optimizations that redistribute crops to meet a suite of agricultural sustainable development targets. With a siloed approach-in which each government ministry seeks to improve a single sustainability outcome in isolation-crop switching could realize large individual benefits but produce tradeoffs for other dimensions and between regions. In cases of central coordination-in which tradeoffs are prevented-we find marked co-benefits for environmental-impact reductions (blue water (-4.5% to -18.5%), green water (-4.4% to -9.5%), greenhouse gases (GHGs) (-1.7% to -7.7%), fertilizers (-5.2% to -10.9%), pesticides (-4.3% to -10.8%)) and increased farmer incomes (+2.9% to +7.5%). These outcomes of centrally coordinated crop switching can contribute substantially (23-40% across dimensions) towards China's 2030 agricultural sustainable development targets and potentially produce global resource savings. This integrated approach can inform feasible targeted agricultural interventions that achieve sustainability co-benefits across several dimensions.


Asunto(s)
Producción de Cultivos , Ambiente , Agricultores , Renta , Desarrollo Sostenible , China , Producción de Cultivos/economía , Producción de Cultivos/métodos , Fertilizantes/análisis , Desarrollo Sostenible/economía , Desarrollo Sostenible/tendencias , Plaguicidas , Gases de Efecto Invernadero
2.
Hum Mol Genet ; 2024 Sep 06.
Artículo en Inglés | MEDLINE | ID: mdl-39239972

RESUMEN

Makorin RING finger protein 3 (MKRN3) is a key inhibitor of the hypothalamic-pituitary-gonadal (HPG) axis. The association between MKRN3 gene variants and central precocious puberty (CPP) has been repeatedly examined. In a recent study, MKRN3 has been assigned a role of tumor suppressor in lung carcinogenesis. Therefore, it is hypothesized that MKRN3 may be the link between CPP and lung cancer (LC), and certain MKRN3 gene variants may affect individuals' susceptibility to CPP and LC. The rs12441287, rs6576457 and rs2239669 in the MKRN3 gene were selected as the target variants. Sanger sequencing was applied to genotype them in two sets of case-control cohorts, namely 384 CPP girls and 422 healthy girls, 550 LC patients and 800 healthy controls. The results showed that rs6576457 but not rs12441287 or rs2239669 was significantly associated with the risk of CPP and LC. Their association with CPP risk was further confirmed in the following meta-analysis. Subsequent functional assays revealed that the rs6576457 genotypes were correlated with differentially expressed MKRN3, and the rs6576457 alleles affected the transcription repressor Oct-1 binding affinity to the MKRN3 promoter. Collectively, the MKRN3 gene rs6576457 may participate in the CPP pathology and LC tumorigenesis in the Hubei Chinese population. However, the present findings should be validated in additional investigations with larger samples from different ethnic populations.

3.
Cell Mol Life Sci ; 81(1): 344, 2024 Aug 12.
Artículo en Inglés | MEDLINE | ID: mdl-39133273

RESUMEN

Osteogenesis is tightly coupled with angiogenesis spatiotemporally. Previous studies have demonstrated that type H blood vessel formed by endothelial cells with high expression of CD31 and Emcn (CD31hi Emcnhi ECs) play a crucial role in bone regeneration. The mechanism of the molecular communication around CD31hi Emcnhi ECs and bone mesenchymal stem cells (BMSCs) in the osteogenic microenvironment is unclear. This study indicates that exosomes from bone mesenchymal stem cells with 7 days osteogenic differentiation (7D-BMSCs-exo) may promote CD31hi Emcnhi ECs angiogenesis, which was verified by tube formation assay, qRT-PCR, Western blot, immunofluorescence staining and µCT assays etc. in vitro and in vivo. Furthermore, by exosomal miRNA microarray and WGCNA assays, we identified downregulated miR-150-5p as the most relative hub gene coupling osteogenic differentiation and type H blood vessel angiogenesis. With bioinformatics assays, dual luciferase reporter experiments, qRT-PCR and Western blot assays, SOX2(SRY-Box Transcription Factor 2) was confirmed as a novel downstream target gene of miR-150-5p in exosomes, which might be a pivotal mechanism regulating CD31hi Emcnhi ECs formation. Additionally, JC-1 immunofluorescence staining, Western blot and seahorse assay results showed that the overexpression of SOX2 could shift metabolic reprogramming from oxidative phosphorylation (OXPHOS) to glycolysis to enhance the CD31hi Emcnhi ECs formation. The PI3k/Akt signaling pathway might play a key role in this process. In summary, BMSCs in osteogenic differentiation might secrete exosomes with low miR-150-5p expression to induce type H blood vessel formation by mediating SOX2 overexpression in ECs. These findings might reveal a molecular mechanism of osteogenesis coupled with type H blood vessel angiogenesis in the osteogenic microenvironment and provide a new therapeutic target or cell-free remedy for osteogenesis impaired diseases.


Asunto(s)
Diferenciación Celular , Células Endoteliales , Exosomas , Células Madre Mesenquimatosas , MicroARNs , Neovascularización Fisiológica , Osteogénesis , MicroARNs/genética , MicroARNs/metabolismo , Exosomas/metabolismo , Osteogénesis/genética , Células Madre Mesenquimatosas/metabolismo , Células Madre Mesenquimatosas/citología , Diferenciación Celular/genética , Neovascularización Fisiológica/genética , Animales , Células Endoteliales/metabolismo , Células Endoteliales/citología , Ratones , Humanos , Células Cultivadas , Transducción de Señal , Molécula-1 de Adhesión Celular Endotelial de Plaqueta/metabolismo , Molécula-1 de Adhesión Celular Endotelial de Plaqueta/genética , Factores de Transcripción SOXB1/metabolismo , Factores de Transcripción SOXB1/genética , Reprogramación Metabólica , Angiogénesis
4.
Nano Lett ; 24(27): 8427-8435, 2024 Jul 10.
Artículo en Inglés | MEDLINE | ID: mdl-38920280

RESUMEN

Metal selenides show outstanding sodium-ion storage performance when matched with an ether-based electrolyte. However, the intrinsic origin of improvement and deterministic interface characteristics have not been systematically elucidated. Herein, employing FeSe2 anode as the model system, the electrochemical kinetics of metal selenides in ether and ester-based electrolytes and associated solid electrolyte interphase (SEI) are investigated in detail. Based on the galvanostatic intermittent titration technique and in situ electrochemical impedance spectroscopy, it is found that the ether-based electrolyte can ensure fast Na+ transfer and low interface impedance. Additionally, the ether-derived thin and smooth double-layer SEI, which is critical in facilitating ion transport, maintaining structural stability, and inhibiting electrolyte overdecomposition, is concretely visualized by transmission electron microscopy, atomic force microscopy, and depth-profiling X-ray photoelectron spectroscopy. This work provides a deep understanding of the optimization mechanism of electrolytes, which can guide available inspiration for the design of practical electrode materials.

5.
Nano Lett ; 2024 Oct 23.
Artículo en Inglés | MEDLINE | ID: mdl-39440864

RESUMEN

Lithium (Li) metal batteries face challenges, such as dendrite growth and electrolyte interface instability. Artificial interface layers alleviate these issues. Here, cellulose nanocrystal (CNC) nanomembranes, with excellent mechanical properties and high specific surface areas, combine with polyvinylidene-hexafluoropropylene (PVDF-HFP) porous membranes to form an artificial solid electrolyte interphase (SEI) layer. The porous structure of PVDF-HFP equalizes the electric field near metallic lithium surfaces. The high mechanical modulus of CNC (6.2 GPa) effectively inhibits dendrite growth, ensures the uniform flow of lithium ions to the lithium metal electrode, and inhibits the growth of lithium dendrites during cycling. The synergy of high polarity ß-phase poly(vinylidene fluoride) (PVDF) and CNC provides over 1000 h of stability for Li//Li batteries. Moreover, Li//LiFePO4 (LFP) full cells with this artificial protective layer perform well at 5 C, showcasing the potential of this film in lithium metal batteries.

6.
Nano Lett ; 24(25): 7698-7705, 2024 Jun 26.
Artículo en Inglés | MEDLINE | ID: mdl-38869496

RESUMEN

Highly efficient recognition of cancer cells by immune cells is important for successful therapeutic-cell-based cancer immunotherapy. Herein, we present a facile NIR-II nanoadaptor [hyaluronic acid (HA)/dibenzocyclooctyne (DBCO)-Au:Ag2Te quantum dots (QDs)] for enhancing the tumor recognition and binding ability of natural killer (NK) cells via a bio-orthogonal click reaction in vivo. The Nanoadaptor possesses superior tumor-targeting capacity, facilitating the accumulation of the chemical receptor DBCO at the tumor sites. Subsequently, the enrichment of DBCO on tumor cell surfaces provides multivalent recognition sites for capturing pretreated azide engineered NK92 cells (NK92-N3) through an efficient click reaction, thereby significantly enhancing the therapeutical efficiency. The dynamic process of nanoadaptor-mediated recognition of NK cells to tumor cells could be vividly observed using multiplexed NIR-II fluorescence imaging in a mouse model of lung cancer. Such a nanoadaptor strategy can be extended to other therapeutic cellular systems and holds promise for future clinical applications.


Asunto(s)
Química Clic , Células Asesinas Naturales , Células Asesinas Naturales/inmunología , Animales , Ratones , Humanos , Puntos Cuánticos/química , Ácido Hialurónico/química , Línea Celular Tumoral , Neoplasias Pulmonares/inmunología , Neoplasias Pulmonares/patología , Oro/química , Inmunoterapia
7.
Nano Lett ; 24(28): 8525-8534, 2024 Jul 17.
Artículo en Inglés | MEDLINE | ID: mdl-38954769

RESUMEN

Cr2(NCN)3 is a potentially high-capacity and fast-charge Li-ion anode owing to its abundant and broad tunnels. However, high intrinsic chemical instability severely restricts its capacity output and electrochemical reversibility. Herein we report an effective crystalline engineering method for optimizing its phase and crystallinity. Systematic studies reveal the relevancy between electrochemical performance and crystalline structure; an optimal Cr2(NCN)3 with high phase purity and uniform crystallinity exhibits a high reversible capacity of 590 mAh g-1 and a stable cycling performance of 478 mAh g-1 after 500 cycles. In-operando heating XRD reveals its high thermodynamical stability over 600 °C, and in-operando electrochemical XRD proves its electrochemical Li storage mechanism, consisting of the primary Li-ion intercalation and subsequent conversion reactions. This study introduces a facile and low-cost method for fabricating high-purity Cr2(NCN)3, and it also confirms that the Li storage of Cr2(NCN)3 can be further improved by tuning its phase and crystallinity.

8.
Nano Lett ; 24(39): 12027-12035, 2024 Oct 02.
Artículo en Inglés | MEDLINE | ID: mdl-39311392

RESUMEN

S-redox involving solvated polysulfides is accompanied by volumetric change and structural decay of the S-based cathodes. Here, we propose a synchronous construction strategy for consolidating Li, Se, S, and C elements within a composite cathode via a paradigm reaction of 8Li+2Se+CS2 = 2Li4SeS+C. The obtained composite features crystalline Li4SeS encapsulated in a carbon nanocage (Li4SeS@C), exhibiting ultrahigh electrical conductivity, ultralow activation barrier, and excellent structural integrity, accordingly enabling large specific capacity (615 mAh g-1) and high capacity retention (87.3% after 350 cycles) at 10 A g-1. TOF-SIMS demonstrates its superior volumetric efficiency to a similar derivative SeS@C (2Se+CS2 = 2SeS+C), and DFT reveals its lower activation barrier than Li2S@C and Li2Se@C. This consolidation design significantly improves the electrochemical performance of S-based cathodes, and the paradigm reaction guarantees structural diversity and flexibility. Moreover, employing a synchronous construction mechanism to maximize the synergistic effect between element consolidation and carbon encapsulation opens up a new approach for developing robust S or chalcogenide cathodes.

9.
Nano Lett ; 24(11): 3421-3431, 2024 Mar 20.
Artículo en Inglés | MEDLINE | ID: mdl-38377170

RESUMEN

Natural killer (NK) cell-based adoptive immunotherapy has demonstrated encouraging therapeutic effects in clinical trials for hematological cancers. However, the effectiveness of treatment for solid tumors remains a challenge due to insufficient recruitment and infiltration of NK cells into tumor tissues. Herein, a programmed nanoremodeler (DAS@P/H/pp) is designed to remodel dense physical stromal barriers and for dysregulation of the chemokine of the tumor environment to enhance the recruitment and infiltration of NK cells in tumors. The DAS@P/H/pp is triggered by the acidic tumor environment, resulting in charge reversal and subsequent hyaluronidase (HAase) release. HAase effectively degrades the extracellular matrix, promoting the delivery of immunoregulatory molecules and chemotherapy drugs into deep tumor tissues. In mouse models of pancreatic cancer, this nanomediated strategy for the programmed remodeling of the tumor microenvironment significantly boosts the recruitment of NK92 cells and their tumor cell-killing capabilities under the supervision of multiplexed near-infrared-II fluorescence.


Asunto(s)
Neoplasias , Neoplasias Pancreáticas , Animales , Ratones , Línea Celular Tumoral , Neoplasias/patología , Inmunoterapia/métodos , Inmunoterapia Adoptiva/métodos , Neoplasias Pancreáticas/patología , Células Asesinas Naturales , Microambiente Tumoral
10.
Nano Lett ; 24(40): 12620-12627, 2024 Oct 09.
Artículo en Inglés | MEDLINE | ID: mdl-39324698

RESUMEN

TexSe1-x shortwave infrared (SWIR) photodetectors show promise for monolithic integration with readout integrated circuits (ROIC), making it a potential alternative to conventional expensive SWIR photodetectors. However, challenges such as a high dark current density and insufficient detection performance hinder their application in large-scale monolithic integration. Herein, we develop a ZnO/TexSe1-x heterojunction photodiode and synergistically address the interfacial elemental diffusion and dangling bonds via inserting a well-selected 0.3 nm amorphous TeO2 interfacial layer. The optimized device achieves a reduced dark current density of -3.5 × 10-5 A cm-2 at -10 mV, a broad response from 300 to 1700 nm, a room-temperature detectivity exceeding 2.03 × 1011 Jones, and a 3 dB bandwidth of 173 kHz. Furthermore, for the first time, we monolithically integrate the TexSe1-x photodiodes on ROIC (64 × 64 pixels) with the largest-scale array among all TexSe1-x-based detectors. Finally, we demonstrate its applications in transmission imaging and substance identification.

11.
J Proteome Res ; 23(2): 550-559, 2024 02 02.
Artículo en Inglés | MEDLINE | ID: mdl-38153036

RESUMEN

In bottom-up proteomics, peptide-spectrum matching is critical for peptide and protein identification. Recently, deep learning models have been used to predict tandem mass spectra of peptides, enabling the calculation of similarity scores between the predicted and experimental spectra for peptide-spectrum matching. These models follow the supervised learning paradigm, which trains a general model using paired peptides and spectra from standard data sets and directly employs the model on experimental data. However, this approach can lead to inaccurate predictions due to differences between the training data and the experimental data, such as sample types, enzyme specificity, and instrument calibration. To tackle this problem, we developed a test-time training paradigm that adapts the pretrained model to generate experimental data-specific models, namely, PepT3. PepT3 yields a 10-40% increase in peptide identification depending on the variability in training and experimental data. Intriguingly, when applied to a patient-derived immunopeptidomic sample, PepT3 increases the identification of tumor-specific immunopeptide candidates by 60%. Two-thirds of the newly identified candidates are predicted to bind to the patient's human leukocyte antigen isoforms. To facilitate access of the model and all the results, we have archived all the intermediate files in Zenodo.org with identifier 8231084.


Asunto(s)
Péptidos , Espectrometría de Masas en Tándem , Humanos , Espectrometría de Masas en Tándem/métodos , Proteínas , Modelos Teóricos , Proteómica/métodos , Algoritmos
12.
J Biol Chem ; 299(10): 105142, 2023 Oct.
Artículo en Inglés | MEDLINE | ID: mdl-37553040

RESUMEN

Nuclear magnetic resonance studies of many physiologically important proteins have long been impeded by the necessity to express such proteins in isotope-labeled form in higher eukaryotic cells and the concomitant high costs of providing isotope-labeled amino acids in the growth medium. Economical routes use isotope-labeled yeast or algae extracts but still require expensive isotope-labeled glutamine. Here, we have systematically quantified the effect of 15N2-glutamine on the expression and isotope labeling of different proteins in insect cells. Sufficient levels of glutamine in the medium increase the protein expression by four to five times relative to deprived conditions. 1H-15N nuclear magnetic resonance spectroscopy shows that the 15N atoms from 15N2-glutamine are scrambled with surprisingly high (60-70%) efficiency into the three amino acids alanine, aspartate, and glutamate. This phenomenon gives direct evidence that the high energy demand of insect cells during baculovirus infection and concomitant heterologous protein expression is predominantly satisfied by glutamine feeding the tricarboxylic acid cycle. To overcome the high costs of supplementing isotope-labeled glutamine, we have developed a robust method for the large-scale synthesis of 15N2-glutamine and partially deuterated 15N2-glutamine-α,ß,ß-d3 from inexpensive precursors. An application is shown for the effective large-scale expression of the isotope-labeled ß1-adrenergic receptor using the synthesized 15N2-glutamine-α,ß,ß-d3.

13.
Small ; 20(12): e2307042, 2024 Mar.
Artículo en Inglés | MEDLINE | ID: mdl-37946682

RESUMEN

Water stability is a crucial issue always addressed for commercial practical application of perovskite quantum dots (QDs). Recent advances in ligand engineering for in situ synthesis of water-stable perovskite QDs have attracted growing interest. However, the exact mechanism remains unclear. Here, the function of 4-bromobutyric acid (BBA) and oleylamine (OLA) is systematically studied in water-stable CsPbX3 (X = Br and I) QDs and confirms that the zwitterionic ligands generated in situ by BBA and OLA are anchored on the QDs surface, thus preventing water from penetrating into the QDs. Cs4PbBr6 intermediate crystal found in the crystal structure evolution process of CsPbX3 QD further reveals a complete crystallization process: PbX2 + CsX + Br- → Cs4PbBr6 crystals + X-→ CsPbX3 QDs + Br-. Furthermore, it is found that the solvent coordination of the precursor solution has a significant effect on the crystallinity of Cs4PbBr6 intermediate crystal, while the Rb+ doping can effectively passivate the surface defects of CsPbX3 QDs, thereby jointly achieving photoluminescence quantum yields (PLQY) of 94.6% for CsPbBr3 QDs (88.2% for CsPbI3 QDs). This work provides new insights and guiding ideas for the green synthesis of high-quality and water-stable perovskite QDs.

14.
Small ; 20(44): e2404065, 2024 Nov.
Artículo en Inglés | MEDLINE | ID: mdl-38949396

RESUMEN

Fe3O4 is barely taken into account as an electrocatalyst for oxygen reduction reaction (ORR), an important reaction for metal-air batteries and fuel cells, due to its sluggish catalytic kinetics and poor electron conductivity. Herein, how strain engineering can be employed to regulate the local electronic structure of Fe3O4 for high ORR activity is reported. Compressively strained Fe3O4 shells with 2.0% shortened Fe─O bond are gained on the Fe/Fe4N cores as a result of lattice mismatch at the interface. A downshift of the d-band center occurs for compressed Fe3O4, leading to weakened chemisorption energy of oxygenated intermediates, and lower reaction overpotential. The compressed Fe3O4 exhibits greatly enhanced electrocatalytic ORR activity with a kinetic current density of 27 times higher than that of pristine one at 0.80 V (vs reversible hydrogen electrode), as well as potential application in zinc-air batteries. The findings provide a new strategy for tuning electronic structures and improving the catalytic activity of other metal catalysts.

15.
Small ; 20(32): e2311650, 2024 Aug.
Artículo en Inglés | MEDLINE | ID: mdl-38764187

RESUMEN

Current lithium-ion batteries cannot meet the requirement of higher energy density with further large-scale application of electrical vehicles. Lithium metal batteries combined with Ni-rich layered oxides cathode are expected as the one of promising solutions, while the poor electrode and electrolyte interface impedes the commercial development of lithium metal batteries. A new double-salts super concentrated (DSSC) carbonate electrolyte is proposed to improve the electrochemical performance of LiNi0.90Co0.05Mn0.05O2 (NCM9055)||Li metal battery which exhibits stable cycling performance with the capacity retention of 93.04% and reversible capacity of 173.8 mAh g-1 after 100 cycles at 1 C, while cells with conventional 1 m diluted electrolyte remains only 60.55% and capacity of 114.2 mAh g-1. The double salts synergistic effect in super concentrated electrolyte promotes the formation for more balanced stable cathode electrolyte interface (CEI) inorganic compounds of CFx, LiNOx, SOF2, Li2SO4, and less LiF by X-ray photoelectron spectroscopy (XPS) test, and the uniform 2-3 nm rock-salt phase protection layer on the cathode surface by transmission electron microscope (TEM) characterization, improving the cycling performance of the Ni-rich NCM9055 layered oxide cathode. The DSSC electrolyte also can relief the Li dendrite growth on Li metal anode, as well as exhibit better flame retardance, promoting the application of more safety Ni-rich NCM9055||Li metal batteries.

16.
Small ; 20(31): e2310699, 2024 Aug.
Artículo en Inglés | MEDLINE | ID: mdl-38456384

RESUMEN

Na3V2(PO4)2F3 (NVPF) is emerging as a promising cathode material for high-voltage sodium-ion batteries. Whereas, the inferior intrinsic electrical conductivity leading to poor rate performance and cycling stability. To address this issue, a strategy of synthesizing unique yolk-shell structured NVPF with copper substitution via spray drying method is proposed. Besides, the synergistic modulation of both crystalline structure and interfacial properties results in significantly enhanced intrinsic and interfacial conductivity of NVPF. The optimized yolk-shell structured cathode materials can possess a high capacity of 117.4 mAh g-1 at 0.1 C, and remains a high-capacity retention of 91.3% after 5000 cycles. A detailed investigation of kinetic properties combined with in situ XRD technology and DFT calculations, has been implemented, particularly with regard to electron conduction and sodium ion diffusion. Consequently, the yolk-shell structured composition of Na3V1.94Cu0.06(PO4)2F3 with nitrogen-modified carbon coating layer shows the lowest polarization potential because of the effectively enhanced electronic conductivity and Na+ diffusion process in the bulk phase. The robust electrochemical performance suggests that developing the unique yolk-shell structure with the collaboration of interface and bulk crystal properties is a favorable strategy to design cathode material with a high performance for sodium-ion batteries.

17.
Small ; 20(1): e2305030, 2024 Jan.
Artículo en Inglés | MEDLINE | ID: mdl-37649169

RESUMEN

Vanadium-based oxides have attracted much attention because of their rich valences and adjustable structures. The high theoretical specific capacity contributed by the two-electron-transfer process (V5+ /V3+ ) makes it an ideal cathode material for aqueous zinc-ion batteries. However, slow diffusion kinetics and poor structural stability limit the application of vanadium-based oxides. Herein, a strategy for intercalating organic matter between vanadium-based oxide layers is proposed to attain high rate performance and long cycling life. The V3 O7 ·H2 O is synthesized in situ on the carbon cloth to form an open porous structure, which provides sufficient contact areas with electrolyte and facilitates zinc ion transport. On the molecular level, the added organic matter p-aminophenol (pAP) not only plays a supporting role in the V3 O7 ·H2 O layer, but also shows a regulatory effect on the V5+ /V4+ redox process due to the reducing functional group on pAP. The novel composite electrode with porous structure exhibits outstanding reversible specific capacity (386.7 mAh g-1 , 0.1 A g-1 ) at a high load of 6.5 mg cm-2 , and superior capacity retention of 80% at 3 A g-1 for 2100 cycles.

18.
Small ; 20(5): e2306595, 2024 Feb.
Artículo en Inglés | MEDLINE | ID: mdl-37732373

RESUMEN

Iron-based sulfate cathodes of alluaudite Na2+2 δ Fe2- δ (SO4 )3 (NFS) in sodium-ion batteries with low cost, steady cycling performance, and high voltage are promising for grid-scale energy storage systems. However, the poor electronic conductivity and the limited understanding of the phase-evolution of precursors hinder obtaining high-rate capacity and the pure phase. Distinctive NFS@C@n%CNTs (n = 1, 2, 5, 10) sphere-shell conductive networks composite cathode materials are constructed creatively, which exhibit superior reversible capacity and rate performance. In detail, the designed NFS@C@2%CNTs cathode delivers an initial discharge capacity of 95.9 mAh g-1 at 0.05 C and up to 60 mAh g-1 at a high rate of 10 C. The full NFS@C@2%CNTs//HC cell delivers a practical operating voltage of 3.5 V and mass-energy density of 140 Wh kg-1 at 0.1 C, and it can also retain 67.37 mAh g-1 with a capacity retention rate of 96.4% after 200 cycles at 2 C. On the other hand, a novel combination reaction mechanism is first revealed for forming NFS from the mixtures of Na2 Fe(SO4 )2 ·nH2 O (n = 2, 4) and FeSO4 ·H2 O during the sintering process. The inspiring results would provide a novel perspective to synthesize high-performance alluaudite sulfate and analogs by aqueous methods.

19.
Small ; 20(37): e2401465, 2024 Sep.
Artículo en Inglés | MEDLINE | ID: mdl-38750613

RESUMEN

Lithium (Li) metal batteries have attracted considerable research attention due to their exceptionally high theoretical capacity. However, the commercialization of Li metal batteries faces challenges, primarily attributed to uncontrolled growth of Li dendrites, which raises safety concerns and lowers coulombic efficiency. To mitigate Li dendrites growth and attain dense Li deposition, the hybrid SiO2-Cu2O lithiophilic film applied to a 3D copper foam current collector is developed to regulate the interfacial properties for achieving even and dense Li deposition. The SiO2-Cu2O possesses strong Li+ trapping capability through strong lithiophilicity from Cu2O. Additionally, the SiO2-Cu2O enables uniform ion diffusion through the domain-limiting effect of the holes in the SiO2 layer, inducing an even and dense Li plating/stripping behavior at a large capacity. Furthermore, the SiO2 layer promotes the formation of an initial high inorganic content Solid Electrolyte Interphase (SEI) through selective preferential binding with anion and solvent molecules. When the SiO2-Cu2O@Li anode is coupled with a LiFePO4 (LFP) cathode, the resulting full cell exhibits superior cycling stability and rate performance. These results provide a facile approach to construct a lithiophilic current collector for practical Li metal anodes.

20.
Small ; 20(23): e2307292, 2024 Jun.
Artículo en Inglés | MEDLINE | ID: mdl-38169091

RESUMEN

Layered Li-rich oxide cathode materials are capable of offering high energy density due to their cumulative cationic and anionic redox mechanism during (de)lithiation process. However, the structural instability of the layered Li-rich oxide cathode materials, especially in the deeply delitiated state, results in severe capacity and voltage degradation. Considering the minimal isotropic structural evolution of disordered rock salt oxide cathode during cycling, cation-disordered nano-domains have been controllably introduced into layered Li-rich oxides by co-doping of d0-TM and alkali ions. Combining electrochemical and synchrotron-based advanced characterizations, the incorporation of the phase-compatible cation-disordered domains can not only hinder the oxygen framework collapse along the c axis of layered Li-rich cathode under high operation voltage but also promote the Mn and anionic activities as well as Li+ (de)intercalation kinetics, leading to remarkable improvement in rate capability and mitigation of capacity and voltage decay. With this unique layered/rocksalt intergrown structure, the intergrown cathode yields an ultrahigh capacity of 288.4 mAh g-1 at 0.1 C, and outstanding capacity retention of ≈90.0% with obviously suppressed voltage decay after 100 cycles at 0.5, 1, and 2 C rate. This work provides a new direction toward advanced cathode materials for next-generation Li-ion batteries.

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