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1.
Cell Death Differ ; 2024 Jul 15.
Artigo em Inglês | MEDLINE | ID: mdl-39009653

RESUMO

Although deubiquitinases (DUBs) have been well described in liver tumorigenesis, their potential roles and mechanisms have not been fully understood. In this study, we identified ubiquitin-specific protease 1 (USP1) as an oncogene with essential roles during hepatocellular carcinoma (HCC) progression. USP1, with elevated expression levels and clinical significance, was identified as a hub DUB for HCC in multiple bioinformatics datasets. Functionally, USP1 overexpression significantly enhanced the malignant behaviors in HCC cell lines and spheroids in vitro, as well as the zebrafish model and the xenograft model in vivo. In contrast, genetic ablation or pharmacological inhibition of USP1 dramatically impaired the phenotypes of HCC cells. Specifically, ectopic USP1 enhanced aggressive properties and metabolic reprogramming of HCC cells by modulating mitochondrial dynamics. Mechanistically, USP1 induced mitochondrial fission by enhancing phosphorylation of Drp1 at Ser616 via deubiquitination and stabilization of cyclin-dependent kinase 5 (CDK5), which could be degraded by the E3 ligase NEDD4L. The USP1/CDK5 modulatory axis was activated in HCC tissues, which was correlated with poor prognosis of HCC patients. Furthermore, Prasugrel was identified as a candidate USP1 inhibitor for targeting the phenotypes of HCC by an extensive computational study combined with experimental validations. Taken together, USP1 induced malignant phenotypes and metabolic reprogramming by modulating mitochondrial dynamics in a CDK5-mediated Drp1 phosphorylation manner, thereby deteriorating HCC progression.

2.
J Am Chem Soc ; 146(28): 19537-19546, 2024 Jul 17.
Artigo em Inglês | MEDLINE | ID: mdl-38949461

RESUMO

It has been widely recognized that the pH environment influences the nanobubble dynamics and hydroxide ions adsorbed on the surface may be responsible for the long-term survival of the nanobubbles. However, understanding the distribution of hydronium and hydroxide ions in the vicinity of a bulk nanobubble surface at a microscopic scale and the consequent impact of these ions on the nanobubble behavior remains a challenging endeavor. In this study, we carried out deep potential molecular dynamics simulations to explore the behavior of a nitrogen nanobubble under neutral, acidic, and alkaline conditions and the inherent mechanism, and we also conducted a theoretical thermodynamic and dynamic analysis to address constraints related to simulation duration. Our simulations and theoretical analyses demonstrate a trend of nanobubble dissolution similar to that observed experimentally, emphasizing the limited dissolution of bulk nanobubbles in alkaline conditions, where hydroxide ions tend to reside slightly farther from the nanobubble surface than hydronium ions, forming more stable hydrogen bond networks that shield the nanobubble from dissolution. In acidic conditions, the hydronium ions preferentially accumulating at the nanobubble surface in an orderly manner drive nanobubble dissolution to increase the entropy of the system, and the dissolved nitrogen molecules further strengthen the hydrogen bond networks of systems by providing a hydrophobic environment for hydronium ions, suggesting both entropy and enthalpy effects contribute to the instability of nanobubbles under acidic conditions. These results offer fresh insights into the double-layer distribution of hydroxide and hydronium near the nitrogen-water interface that influences the dynamic behavior of bulk nanobubbles.

3.
Adv Mater ; : e2402947, 2024 May 14.
Artigo em Inglês | MEDLINE | ID: mdl-38743762

RESUMO

Tin (Sn) -based perovskite solar cells (PSCs) normally show low open circuit voltage due to serious carrier recombination in the devices, which can be attributed to the oxidation and the resultant high p-type doping of the perovskite active layers. Considering the grand challenge to completely prohibit the oxidation of Sn-based perovskites, a feasible way to improve the device performance is to counter-dope the oxidized Sn-based perovskites by replacing Sn2+ with trivalent cations in the crystal lattice, which however is rarely reported. Here, the introduction of Sb3+, which can effectively counter-dope the oxidized perovskite layer and improve the carrier lifetime, is presented. Meanwhile, Sb3+ can passivate deep-level defects and improve carrier mobility of the perovskite layer, which are all favorable for the photovoltaic performance of the devices. Consequently, the target devices yield a relative enhancement of the power conversion efficiency (PCE) of 31.4% as well as excellent shelf-storage stability. This work provides a novel strategy to improve the performance of Sn-based PSCs, which can be developed as a universal way to compensate for the oxidation of Sn-based perovskites in optoelectronic devices.

4.
J Am Chem Soc ; 146(22): 15219-15229, 2024 Jun 05.
Artigo em Inglês | MEDLINE | ID: mdl-38775440

RESUMO

Unraveling the catalyst surface structure and behavior during reactions is essential for both mechanistic understanding and performance optimization. Here we report a phenomenon of facet-dependent surface restructuring intrinsic to ß-Ni(OH)2 catalysts during oxygen evolution reaction (OER), discovered by the correlative ex situ and operando characterization. The ex situ study after OER reveals ß-Ni(OH)2 restructuring at the edge facets to form nanoporous Ni1-xO, which is Ni deficient containing Ni3+ species. Operando liquid transmission electron microscopy (TEM) and Raman spectroscopy further identify the active role of the intermediate ß-NiOOH phase in both the OER catalysis and Ni1-xO formation, pinpointing the complete surface restructuring pathway. Such surface restructuring is shown to effectively increase the exposed active sites, accelerate Ni oxidation kinetics, and optimize *OH intermediate bonding energy toward fast OER kinetics, which leads to an extraordinary activity enhancement of ∼16-fold. Facilitated by such a self-activation process, the specially prepared ß-Ni(OH)2 with larger edge facets exhibits a 470-fold current enhancement than that of the benchmark IrO2, demonstrating a promising way to optimize metal-(oxy)hydroxide-based catalysts.

5.
Nat Mater ; 2024 Apr 08.
Artigo em Inglês | MEDLINE | ID: mdl-38589543

RESUMO

Unconventional 1T'-phase transition metal dichalcogenides (TMDs) have aroused tremendous research interest due to their unique phase-dependent physicochemical properties and applications. However, due to the metastable nature of 1T'-TMDs, the controlled synthesis of 1T'-TMD monolayers (MLs) with high phase purity and stability still remains a challenge. Here we report that 4H-Au nanowires (NWs), when used as templates, can induce the quasi-epitaxial growth of high-phase-purity and stable 1T'-TMD MLs, including WS2, WSe2, MoS2 and MoSe2, via a facile and rapid wet-chemical method. The as-synthesized 4H-Au@1T'-TMD core-shell NWs can be used for ultrasensitive surface-enhanced Raman scattering (SERS) detection. For instance, the 4H-Au@1T'-WS2 NWs have achieved attomole-level SERS detections of Rhodamine 6G and a variety of severe acute respiratory syndrome coronavirus 2 (SARS-CoV-2) spike proteins. This work provides insights into the preparation of high-phase-purity and stable 1T'-TMD MLs on metal substrates or templates, showing great potential in various promising applications.

6.
Cardiovasc Res ; 2024 Apr 22.
Artigo em Inglês | MEDLINE | ID: mdl-38646676

RESUMO

BACKGROUND: In patients with diabetic microvascular complications, decreased perfusion or vascular occlusion, caused by reduced vascular diameter, is a common characteristic that will lead to insufficient blood supply. Yet, the regulatory mechanism and effective treatment approach remain elusive. METHODS AND RESULTS: Our initial findings revealed a notable decrease in the expression of human AQP1 in both diabetic human retina samples (49 healthy vs. 54 diabetic samples) and high-glucose-treated human retinal microvascular endothelial cells. Subsequently, our investigations unveiled a reduction in vascular diameter and compromised perfusion within zebrafish embryos subjected to high glucose treatment. Further analysis indicated a significant downregulation of two aquaporins, aqp1a.1 and aqp8a.1, which are highly enriched in ECs and are notably responsive to hyperglycemic conditions. Intriguingly, the loss of function of aqp1a.1 and/or aqp8a.1 resulted in a reduction of intersegmental vessel diameters, effectively mirroring the phenotype observed in the hyperglycemic zebrafish model.The overexpression of aqp1a.1/aqp8a.1 in zebrafish ECs led to notable enlargement of microvascular diameters. Moreover, the reduced vessel diameters resulting from high-glucose treatment were effectively rescued by the overexpression of these aquaporins. Additionally, both aqp1a.1 and apq8a.1 were localized in the intracellular vacuoles in cultured ECs as well as the ECs of sprouting ISVs, and the loss of Aqps caused the reduction of those vacuoles, which was required for lumenization. Notably, while the loss of AQP1 did not impact EC differentiation from human stem cells, it significantly inhibited vascular formation in differentiated ECs. CONCLUSION: EC-enriched aquaporins regulate the diameter of blood vessels through an intracellular vacuole-mediated process under hyperglycemic conditions. These findings collectively suggest that aquaporins expressed in ECs hold significant promise as potential targets for gene therapy aimed at addressing vascular perfusion defects associated with diabetes.

7.
ACS Appl Mater Interfaces ; 16(9): 11336-11348, 2024 Mar 06.
Artigo em Inglês | MEDLINE | ID: mdl-38407027

RESUMO

Articular cartilage injury is a common disease in clinical medicine. Because of its special physiological structure and lack of blood, lymph, and nerves, its ability to regenerate once damaged is very limited. In this study, we designed and synthesized a series of self- and coassembled cartilage-inducing functional peptide molecules and constructed a coassembled functional peptide hydrogel based on phenylboronic acid-o-dihydroxy "click chemistry" cross-linking to promote aggregation and signal transduction of mesenchymal stem cells (MSCs) in the early stage and differentiation toward cartilage, thereby promoting the repair of cartilage damage. Three functional peptide molecules were produced using solid-phase peptide synthesis technology, yielding a purity higher than 95%. DOPA-FEFEFEFEGHSNGLPL (DFP) and PBA-FKFKFKFKGHAVDI (BFP) were coassembled at near-neutral pH to form hydrogels (C Gels) based on phenylboronic acid-o-dihydroxy click chemistry cross-linking and effectively loaded transforming growth factor (TGF)-ß1 with a release period of up to 2 weeks. Furthermore, chondrocytes and bone marrow mesenchymal stem cells (BMSCs) were cocultured with functional peptide hydrogels, and the results displayed that the coassembled functional peptide hydrogel group C Gels significantly promoted the proliferation of chondrocytes and MSCs. The chondrocyte markers collagen type I, collagen type II, and glycosaminoglycan (GAG) in the coassembled functional peptide hydrogel group were significantly higher than those in the control group, indicating that it can induce the differentiation of MSCs into cartilage. In vivo experiments demonstrated that the size and thickness of the new cartilage in the compound gel group were the most beneficial to cartilage regeneration. These results indicated that peptide hydrogels are a promising therapeutic option for cartilage regeneration.


Assuntos
Ácidos Borônicos , Cartilagem Articular , Hidrogéis , Hidrogéis/química , Cartilagem Articular/metabolismo , Condrócitos , Diferenciação Celular , Peptídeos/farmacologia , Peptídeos/metabolismo , Fator de Crescimento Transformador beta1/farmacologia , Fator de Crescimento Transformador beta1/metabolismo , Condrogênese , Engenharia Tecidual/métodos
8.
Soft Matter ; 20(9): 2017-2023, 2024 Feb 28.
Artigo em Inglês | MEDLINE | ID: mdl-38334445

RESUMO

Surgical adhesives play a crucial role in tissue integration and repair, yet their application in wet conditions has been severely limited by inadequate adhesive strength and subpar biocompatibility. Furthermore, tissue adhesives have rarely been reported in cartilage tissue repair. In this study, a three-armed dopamine-modified hyaluronic acid derivative adhesive was prepared to function as a bio-inspired adhesive in moist environments. To meet the clinical requirements for cartilage tissue adhesion, we studied its chemical structure, including microscopic morphology, adhesion properties with materials and tissues, in vivo degradation rules, and biological evaluation. The OGMHA8-DOPA adhesive with the optimal aldehyde substitution degree and dopamine-grafting rate was determined by analyzing the experimental conditions. SEM results revealed that the cartilage tissue adhered to a porous interconnected structure. The excellent biocompatibility of the material not only facilitated chondrocyte adhesion but also supported their proliferation on its surface. Animal experiments have demonstrated that this material has no observable inflammatory response or incidence of fibrous capsule formation. The degradation timeline of the material extends beyond the duration of two weeks. The dopamine-modified adhesive exhibited a tight interfacial binding force between the biomaterial and cartilage tissue and excellent biocompatibility in watery tissue, revealing its potential for application in cartilage tissue repair and minimally invasive surgery.


Assuntos
Adesivos , Materiais Biocompatíveis , Animais , Materiais Biocompatíveis/farmacologia , Adesivos/química , Dopamina/química , Cartilagem , Condrócitos
9.
Nano Lett ; 24(5): 1539-1543, 2024 Feb 07.
Artigo em Inglês | MEDLINE | ID: mdl-38262042

RESUMO

Two-dimensional (2D) materials with competing polymorphs offer remarkable potential to switch the associated 2D functionalities for novel device applications. Probing their phase transition and competition mechanisms requires nanoscale characterization techniques that can sensitively detect the nucleation of secondary phases down to single-layer thickness. Here we demonstrate nanoscale phase identification on 2D In2Se3 polymorphs, utilizing their distinct plasmon energies that can be distinguished by electron energy-loss spectroscopy (EELS). The characteristic plasmon energies of In2Se3 polymorphs have been validated by first-principles calculations, and also been successfully applied to reveal phase transitions using in situ EELS. Correlating with in situ X-ray diffraction, we further derive a subtle difference in the valence electron density of In2Se3 polymorphs, consistent with their disparate electronic properties. The nanometer resolution and independence of orientation make plasmon-energy mapping a versatile technique for nanoscale phase identification on 2D materials.

10.
Adv Sci (Weinh) ; 11(13): e2305551, 2024 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-38263724

RESUMO

2D conjugated metal-organic frameworks (c-MOFs) have emerged as promising materials for (opto)electronic applications due to their excellent charge transport properties originating from the unique layered-stacked structures with extended in-plane conjugation. The further advancement of MOF-based (opto)electronics necessitates the development of novel 2D c-MOF thin films with high quality. Cu-HHHATN (HHHATN: hexahydroxyl-hexaazatrinaphthylene) is a recently reported 2D c-MOF featuring high in-plane conjugation, strong interlayer π-π stacking, and multiple coordination sites, while the production of its thin-film form has not yet been reported. Herein, large-area Cu-HHHATN thin films with preferential orientation, high uniformity, and smooth surfaces are realized by using a convenient layer-by-layer growth method. Flexible photodetectors are fabricated, showing broadband photoresponse ranging from UV to short-wave infrared (370 to 1450 nm). The relatively long relaxation time of photocurrent, which arises from the trapping of photocarriers, renders the device's synaptic plasticity similar to that of biological synapses, promising its use in neuromorphic visual systems. This work demonstrates the great potential of Cu-HHHATN thin films in flexible optoelectronic devices for various applications.

11.
Sci Rep ; 14(1): 2137, 2024 01 25.
Artigo em Inglês | MEDLINE | ID: mdl-38272986

RESUMO

This study aimed to evaluate the causal effects of inflammatory bowel disease (IBD) and erectile dysfunction (ED) using Mendelian randomization (MR). All datasets were obtained from the public genome-wide association study database. In the exposure group, 12,882 IBD patients and 21,770 controls were included. A total of 1154 ED patients and 94,024 controls were included in the outcome group. Two-sample MR was conducted to estimate the causal effect of IBD on ED. Furthermore, Crohn's disease (CD) and ulcerative colitis (UC) were exposure factors in subgroup analyses. Weighted median, MR-egger, Inverse-variant weighted (IVW), weighted mode, and simple mode methods were used in MR analysis. Horizontal pleiotropy test, heterogeneity test, and leave-one-out method were utilized to evaluate the sensitivity and stability of results. After analysis, 62, 52, and 36 single nucleotide polymorphisms (SNPs) that IBD-ED, CD-ED, and UC-ED were included, respectively. The incidence of ED was increased by IBD (IVW: OR = 1.110, 95% CI = 1.017-1.211, P = 0.019; P-heterogeneity > 0.05) and, in addition, ED was affected by CD (IVW: OR = 1.085, 95% CI = 1.015-1.160, P = 0.016; P-heterogeneity > 0.05). However, there was no causal effect of UC on ED (IVW: OR = 1.018, 95% CI = 0.917-1.129, P = 0.743; P-heterogeneity < 0.05). All SNPs showed no significant horizontal pleiotropy (P > 0.05). These results indicate that IBD and CD can cause ED; However, UC did not cause ED. Additional research was required to determine causality and potential mechanisms further.


Assuntos
Colite Ulcerativa , Doença de Crohn , Disfunção Erétil , Doenças Inflamatórias Intestinais , Masculino , Humanos , Disfunção Erétil/genética , Estudo de Associação Genômica Ampla , Análise da Randomização Mendeliana , Doenças Inflamatórias Intestinais/complicações , Doenças Inflamatórias Intestinais/genética , Colite Ulcerativa/complicações , Colite Ulcerativa/genética , Doença de Crohn/complicações , Doença de Crohn/genética
12.
J Org Chem ; 89(4): 2375-2396, 2024 Feb 16.
Artigo em Inglês | MEDLINE | ID: mdl-38288704

RESUMO

A universal glycosylation strategy could significantly simplify glycoside synthesis. One approach to achieving this goal is through acyl group direction for the corresponding 1,2-, 1,3-, 1,4-, or 1,6-trans glycosylation; however, this approach has been challenging for glycosidic bonds that require distal equatorial-acyl group direction. We developed an approach in weakly nucleophilic environments for selective 1,4-trans glycosylation directed by the equatorial-4-O-acyl group. Here, we explored this condition in other distal acyl groups and found that, besides 1,n-trans direction, acyl groups also mediated hydrogen bonding between acyl groups and alcohols. The latter showed a diverse effect and classified the acyl group direction into axial and equatorial categories. Corresponding glycosylation conditions were distinguished as guidance for acyl group direction from either category. Hence, acyl group direction may serve as a general glycosylation strategy.

13.
Nano Lett ; 23(23): 10765-10771, 2023 Dec 13.
Artigo em Inglês | MEDLINE | ID: mdl-37963268

RESUMO

High-entropy alloy (HEA) nanoparticles (NPs) have been emerging with superior compositional tunability and multielemental synergy, presenting a unique platform for material discovery and performance optimization. Here we report a synthetic approach utilizing hollow-carbon confinement in the ordinary furnace annealing to achieve the nonequilibrium HEA-NPs such as Pt0.45Fe0.18Co0.12Ni0.15Mn0.10 with uniform size ∼5.9 nm. The facile temperature control allows us not only to reveal the detailed reaction pathway through ex situ characterization but also to tailor the HEA-NP structure from the crystalline solid solution to intermetallic. The preconfinement of metal precursors is the key to ensure the uniform distribution of metal nanoparticles with confined volume, which is essential to prevent the thermodynamically favored phase separation even during the ordinary furnace annealing. Besides, the synthesized HEA-NPs exhibit remarkable activity and stability in oxygen reduction catalysis. The demonstrated synthetic approach may significantly expand the scope of HEA-NPs with uncharted composition and performance.

14.
JMIR Med Inform ; 11: e47833, 2023 Nov 20.
Artigo em Inglês | MEDLINE | ID: mdl-37983072

RESUMO

BACKGROUND: Machine learning (ML) models provide more choices to patients with diabetes mellitus (DM) to more properly manage blood glucose (BG) levels. However, because of numerous types of ML algorithms, choosing an appropriate model is vitally important. OBJECTIVE: In a systematic review and network meta-analysis, this study aimed to comprehensively assess the performance of ML models in predicting BG levels. In addition, we assessed ML models used to detect and predict adverse BG (hypoglycemia) events by calculating pooled estimates of sensitivity and specificity. METHODS: PubMed, Embase, Web of Science, and Institute of Electrical and Electronics Engineers Explore databases were systematically searched for studies on predicting BG levels and predicting or detecting adverse BG events using ML models, from inception to November 2022. Studies that assessed the performance of different ML models in predicting or detecting BG levels or adverse BG events of patients with DM were included. Studies with no derivation or performance metrics of ML models were excluded. The Quality Assessment of Diagnostic Accuracy Studies tool was applied to assess the quality of included studies. Primary outcomes were the relative ranking of ML models for predicting BG levels in different prediction horizons (PHs) and pooled estimates of the sensitivity and specificity of ML models in detecting or predicting adverse BG events. RESULTS: In total, 46 eligible studies were included for meta-analysis. Regarding ML models for predicting BG levels, the means of the absolute root mean square error (RMSE) in a PH of 15, 30, 45, and 60 minutes were 18.88 (SD 19.71), 21.40 (SD 12.56), 21.27 (SD 5.17), and 30.01 (SD 7.23) mg/dL, respectively. The neural network model (NNM) showed the highest relative performance in different PHs. Furthermore, the pooled estimates of the positive likelihood ratio and the negative likelihood ratio of ML models were 8.3 (95% CI 5.7-12.0) and 0.31 (95% CI 0.22-0.44), respectively, for predicting hypoglycemia and 2.4 (95% CI 1.6-3.7) and 0.37 (95% CI 0.29-0.46), respectively, for detecting hypoglycemia. CONCLUSIONS: Statistically significant high heterogeneity was detected in all subgroups, with different sources of heterogeneity. For predicting precise BG levels, the RMSE increases with a rise in the PH, and the NNM shows the highest relative performance among all the ML models. Meanwhile, current ML models have sufficient ability to predict adverse BG events, while their ability to detect adverse BG events needs to be enhanced. TRIAL REGISTRATION: PROSPERO CRD42022375250; https://www.crd.york.ac.uk/prospero/display_record.php?RecordID=375250.

15.
Org Lett ; 25(39): 7120-7125, 2023 Oct 06.
Artigo em Inglês | MEDLINE | ID: mdl-37738091

RESUMO

eq-4-O-Acyl group directed ß-rhamnosylation and ß-mannosylation are achieved in a carborane or BARF anion formed weakly nucleophilic environment with the assistance of a 2,3-orthocarbonate group. The 4-O-acyl group plays a critical role in directing the ß-selectivity, and the weakly coordinating anion is essential to amplify this direction. The orthocarbonate group could be readily removed with 1,3-propanediol in the presence of BF3·Et2O.

16.
Transplant Proc ; 55(9): 2085-2089, 2023 Nov.
Artigo em Inglês | MEDLINE | ID: mdl-37743190

RESUMO

BACKGROUND: The 2 main types of calcineurin inhibitors (CNI) are tacrolimus (TAC) and cyclosporine A (CsA); both are needed by patients who receive kidney transplants. A common adverse reaction of TAC is depression, which is listed in its instructions. However, depression occurred rarely, according to the instructions manual for CsA. METHODS: Scales measuring depression were sent to recipients who had taken TAC or CsA to observe whether there was a difference in depression between patients who consumed the 2 drugs. From September 23rd-December 8th 2022, a questionnaire was sent to kidney transplant recipients online to investigate depression by PHQ-9 score. Then, the questionnaires returned were divided into 2 groups: TAC group and CsA group. The difference of basic characteristics was made to equal by means of propensity score matching (PSM). The scores, degrees of depression, and prevalence of major depression between the 2 groups were compared. RESULTS: Of 259 questionnaires returned, 220 questionnaires were valid. Among them, 170 recipients used TAC and 50 recipients used CsA. There were no significant differences in baseline characteristics after PSM. After PSM, there was no statistically significant difference in PHQ-9 (0.8) score, degree of depression (P = .7), or rate of major depression between the 2 groups. CONCLUSIONS: There was no significant difference between kidney transplant recipients taking TAC or CsA in PHQ-9 score, degree of depression, or prevalence of major depression.


Assuntos
Ciclosporina , Transplante de Rim , Humanos , Ciclosporina/efeitos adversos , Tacrolimo/efeitos adversos , Imunossupressores/efeitos adversos , Transplante de Rim/efeitos adversos , Depressão/diagnóstico , Depressão/epidemiologia , Rejeição de Enxerto
17.
Innovation (Camb) ; 4(5): 100459, 2023 Sep 11.
Artigo em Inglês | MEDLINE | ID: mdl-37560333

RESUMO

The search of quantum spin liquid (QSL), an exotic magnetic state with strongly fluctuating and highly entangled spins down to zero temperature, is a main theme in current condensed matter physics. However, there is no smoking gun evidence for deconfined spinons in any QSL candidate so far. The disorders and competing exchange interactions may prevent the formation of an ideal QSL state on frustrated spin lattices. Here we report comprehensive and systematic measurements of the magnetic susceptibility, ultralow-temperature specific heat, muon spin relaxation (µSR), nuclear magnetic resonance (NMR), and thermal conductivity for NaYbSe2 single crystals, in which Yb3+ ions with effective spin-1/2 form a perfect triangular lattice. All these complementary techniques find no evidence of long-range magnetic order down to their respective base temperatures. Instead, specific heat, µSR, and NMR measurements suggest the coexistence of quasi-static and dynamic spins in NaYbSe2. The scattering from these quasi-static spins may cause the absence of magnetic thermal conductivity. Thus, we propose a scenario of fluctuating ferrimagnetic droplets immersed in a sea of QSL. This may be quite common on the way pursuing an ideal QSL, and provides a brand new platform to study how a QSL state survives impurities and coexists with other magnetically ordered states.

18.
Langmuir ; 39(33): 11828-11838, 2023 Aug 22.
Artigo em Inglês | MEDLINE | ID: mdl-37556484

RESUMO

Through employing molecular dynamics, in this work, we study how a two-component surfactant mixture cooperatively reduces the interfacial tension of a flat vapor-liquid interface. Our simulation results show that in the presence of a given insoluble surfactant, adding a secondary surfactant would either further reduce interfacial tension, indicating a positive synergistic effect, or increase the interfacial tension instead, indicating a negative synergistic effect. The synergism of the surfactant mixture in lowering surface tension is found to depend strongly on the structure complementary effect between different surfactant components. The synergistic mechanisms are then interpreted with minimization of the bending free energy of the composite surfactant monolayer via cooperatively changing the monolayer spontaneous curvature. By roughly describing the monolayer spontaneous curvature with the balanced distribution of surfactant heads and tails, we confirm that the positive synergistic effect in lowering surface tension is featured with the increasingly symmetric head-tail distributions, while the negative synergistic effect is featured with the increasingly asymmetric head-tail distributions. Furthermore, our simulation results indicate that minimal interfacial tension can only be observed when the spontaneous curvature is nearly zero.

19.
Angew Chem Int Ed Engl ; 62(28): e202303950, 2023 Jul 10.
Artigo em Inglês | MEDLINE | ID: mdl-37160760

RESUMO

Ether electrolytes are promising for lithium metal batteries. Despite the intensive research in recent years, most state-of-the-art ether electrolytes still cannot form reliable electrode-electrolyte interfaces in NCM811-Li batteries at diluted concentrations, especially in those operating at elevated temperatures. We report a simple but effective strategy to break this bottleneck and stabilize interfaces in high-temperature NCM811-Li batteries in ether electrolytes. We propose that by gradually extending the terminal groups of glycol diethers from methyl groups to n-butyl groups, the comprehensive stability of ether electrolytes is improved. An anion-dominated solvation structure is realized at a concentration of 1 M. Accordingly, the electrode-electrolyte interactions are suppressed, and a thinner, denser, and more inorganic-rich solid- /cathode-electrolyte interface is achieved. Additionally, the surface phase transition and structural degradation of NCM811 cathode are alleviated. Consequently, in the ethylene glycol dibutyl ether-based electrolyte, the Coulombic efficiency for Li-Cu cells working at 60 °C is boosted to 99.41 % with a cycling life of over 200 cycles. The lifespan of high-temperature NCM811-Li cells is prolonged by more than 400 % with a stable average Coulombic efficiency of 99.77 % at quasi-practical conditions of 50 µm Li, lean electrolyte of 10 µL mAh-1 , and medium-high cathode loading of >2.2 mAh cm-2 .

20.
Nat Commun ; 14(1): 2538, 2023 May 03.
Artigo em Inglês | MEDLINE | ID: mdl-37137913

RESUMO

Epitaxial growth is one of the most commonly used strategies to precisely tailor heterostructures with well-defined compositions, morphologies, crystal phases, and interfaces for various applications. However, as epitaxial growth requires a small interfacial lattice mismatch between the components, it remains a challenge for the epitaxial synthesis of heterostructures constructed by materials with large lattice mismatch and/or different chemical bonding, especially the noble metal-semiconductor heterostructures. Here, we develop a noble metal-seeded epitaxial growth strategy to prepare highly symmetrical noble metal-semiconductor branched heterostructures with desired spatial configurations, i.e., twenty CdS (or CdSe) nanorods epitaxially grown on twenty exposed (111) facets of Ag icosahedral nanocrystal, albeit a large lattice mismatch (more than 40%). Importantly, a high quantum yield (QY) of plasmon-induced hot-electron transferred from Ag to CdS was observed in epitaxial Ag-CdS icosapods (18.1%). This work demonstrates that epitaxial growth can be achieved in heterostructures composed of materials with large lattice mismatches. The constructed epitaxial noble metal-semiconductor interfaces could be an ideal platform for investigating the role of interfaces in various physicochemical processes.

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