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1.
Biomed Pharmacother ; 173: 116406, 2024 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-38460366

RESUMO

Sanguinarine is a quaternary ammonium benzophenanthine alkaloid found in traditional herbs such as Chelidonium, Corydalis, Sanguinarum, and Borovula. It has been proven to possess broad-spectrum biological activities, such as antitumor, anti-inflammatory, antiosteoporosis, neuroprotective, and antipathogenic microorganism activities. In this paper, recent progress on the biological activity and mechanism of action of sanguinarine and its derivatives over the past ten years is reviewed. The results showed that the biological activities of hematarginine and its derivatives are related mainly to the JAK/STAT, PI3K/Akt/mTOR, NF-κB, TGF-ß, MAPK and Wnt/ß-catenin signaling pathways. The limitations of using sanguinarine in clinical application are also discussed, and the research prospects of this subject are outlined. In general, sanguinarine, a natural medicine, has many pharmacological effects, but its toxicity and safety in clinical application still need to be further studied. This review provides useful information for the development of sanguinarine-based bioactive agents.


Assuntos
Alcaloides , Fosfatidilinositol 3-Quinases , Fosfatidilinositol 3-Quinases/metabolismo , Benzofenantridinas/farmacologia , Alcaloides/metabolismo , Isoquinolinas/farmacologia
2.
Adv Mater ; : e2403073, 2024 Mar 30.
Artigo em Inglês | MEDLINE | ID: mdl-38553938

RESUMO

Na-ion batteries (NIBs) are sustainable alternatives to Li-ion technologies due to the abundant and widely-distributed resources. However, the most promising cathode materials of NIBs so far, O3 layered oxides, suffer from serious air instability issues, which significantly increases the manufactural cost and carbon footprint because of the long-term use of dry rooms. While some feasible strategies are proposed via case studies, universal design strategies for air-stable cathodes are yet to be established. Herein, the air degradation mechanisms of O3 cathodes are investigated via combined first-principles and experimental approaches, with bond dissociation energy proposed as an effective descriptor for predicting air stability. Experimental validations in various unary, binary, and ternary O3 cathodes confirm that the air stability can indeed be effectively improved via simple compositional design. Guided by the predictive model, the designed material can sustain 30-day air-storage without structural or electrochemical degradation. It is calculated that such air-stable cathodes can significantly reduce both energy consumption (≈4 100 000 kWh) and carbon footprint (≈2200-ton CO2) annually for a 2 GWh NIBs manufactory. Therefore, the fundamental understandings and universal design strategy presented open an avenue for rational materials design of NIBs toward both elemental and manufactural sustainability.

3.
Biosci Trends ; 18(1): 94-104, 2024 Mar 19.
Artigo em Inglês | MEDLINE | ID: mdl-38325821

RESUMO

This study aimed to investigate the causal role of diabetes mellitus (DM), glycemic traits, and sodium-glucose cotransporter 2 (SGLT2) inhibition in pulmonary arterial hypertension (PAH). Utilizing a two-sample two-step Mendelian randomization (MR) approach, we determined the causal influence of DM and glycemic traits (including insulin resistance, glycated hemoglobin, and fasting insulin and glucose) on the risk of PAH. Moreover, we examined the causal effects of SGLT2 inhibition on the risk of PAH. Genetic proxies for SGLT2 inhibition were identified as variants in the SLC5A2 gene that were associated with both levels of gene expression and hemoglobin A1c. Results showed that genetically inferred DM demonstrated a causal correlation with an increased risk of PAH, exhibiting an odds ratio (OR) of 1.432, with a 95% confidence interval (CI) of 1.040-1.973, and a p-value of 0.028. The multivariate MR analysis revealed comparable outcomes after potential confounders (OR = 1.469, 95%CI = 1.021-2.115, p = 0.038). Moreover, genetically predicted SGLT2 inhibition was causally linked to a reduced risk of PAH (OR = 1.681*10-7, 95%CI = 7.059*10-12-0.004, p = 0.002). Therefore, our study identified the suggestively causal effect of DM on the risk of PAH, and SGLT2 inhibition may be a potential therapeutic target in patients with PAH.


Assuntos
Diabetes Mellitus Tipo 2 , Hipertensão Arterial Pulmonar , Humanos , Diabetes Mellitus Tipo 2/genética , Diabetes Mellitus Tipo 2/complicações , Glicemia , Hipertensão Arterial Pulmonar/complicações , Análise da Randomização Mendeliana , Transportador 2 de Glucose-Sódio/genética , Transportador 2 de Glucose-Sódio/uso terapêutico , Hemoglobinas Glicadas , Polimorfismo de Nucleotídeo Único
4.
Angew Chem Int Ed Engl ; 63(8): e202317942, 2024 Feb 19.
Artigo em Inglês | MEDLINE | ID: mdl-38179820

RESUMO

CO2 electroreduction (CO2 R) operating in acidic media circumvents the problems of carbonate formation and CO2 crossover in neutral/alkaline electrolyzers. Alkali cations have been universally recognized as indispensable components for acidic CO2 R, while they cause the inevitable issue of salt precipitation. It is therefore desirable to realize alkali-cation-free CO2 R in pure acid. However, without alkali cations, stabilizing *CO2 intermediates by catalyst itself at the acidic interface poses as a challenge. Herein, we first demonstrate that a carbon nanotube-supported molecularly dispersed cobalt phthalocyanine (CoPc@CNT) catalyst provides the Co single-atom active site with energetically localized d states to strengthen the adsorbate-surface interactions, which stabilizes *CO2 intermediates at the acidic interface (pH=1). As a result, we realize CO2 conversion to CO in pure acid with a faradaic efficiency of 60 % at pH=2 in flow cell. Furthermore, CO2 is successfully converted in cation exchanged membrane-based electrode assembly with a faradaic efficiency of 73 %. For CoPc@CNT, acidic conditions also promote the intrinsic activity of CO2 R compared to alkaline conditions, since the potential-limiting step, *CO2 to *COOH, is pH-dependent. This work provides a new understanding for the stabilization of reaction intermediates and facilitates the designs of catalysts and devices for acidic CO2 R.

5.
Science ; 383(6679): 212-219, 2024 Jan 12.
Artigo em Inglês | MEDLINE | ID: mdl-38207038

RESUMO

We expand the concept of epitaxy to a regime of "twisted epitaxy" with the epilayer crystal orientation between two substrates influenced by their relative orientation. We annealed nanometer-thick gold (Au) nanoparticles between two substrates of exfoliated hexagonal molybdenum disulfide (MoS2) with varying orientation of their basal planes with a mutual twist angle ranging from 0° to 60°. Transmission electron microscopy studies show that Au aligns midway between the top and bottom MoS2 when the twist angle of the bilayer is small (<~7°). For larger twist angles, Au has only a small misorientation with the bottom MoS2 that varies approximately sinusoidally with twist angle of the bilayer MoS2. Four-dimensional scanning transmission electron microscopy analysis further reveals a periodic strain variation (<|±0.5%|) in the Au nanodisks associated with the twisted epitaxy, consistent with the Moiré registry of the two MoS2 twisted layers.

6.
Chin Med J (Engl) ; 137(1): 82-86, 2024 Jan 05.
Artigo em Inglês | MEDLINE | ID: mdl-37646132

RESUMO

INTRODUCTION: Observational studies have revealed an association between waist circumference (WC) and atrial fibrillation (AF). However, it is difficult to infer a causal relationship from observational studies because the observed associations could be confounded by unknown risk factors. Therefore, the causal role of WC in AF is unclear. This study was designed to investigate the causal association between WC and AF using a two-sample Mendelian randomization (MR) analysis. METHODS: In our two-sample MR analysis, the genetic variation used as an instrumental variable for MR was acquired from a genome-wide association study (GWAS) of WC (42 single nucleotide polymorphisms with a genetic significance of P <5 × 10 -8 ). The data of WC (from the Genetic Investigation of ANthropometric Traits consortium, containing 232,101 participants) and the data of AF (from the European Bioinformatics Institute database, containing 55,114 AF cases and 482,295 controls) were used to assess the causal role of WC on AF. Three different approaches (inverse variance weighted [IVW], MR-Egger, and weighted median regression) were used to ensure that our results more reliable. RESULTS: All three MR analyses provided evidence of a positive causal association between high WC and AF. High WC was suggested to increase the risk of AF based on the IVW method (odds ratio [OR] = 1.43, 95% confidence interval [CI], 1.30-1.58, P = 2.51 × 10 -13 ). The results of MR-Egger and weighted median regression exhibited similar trends (MR-Egger OR = 1.40 [95% CI, 1.08-1.81], P = 1.61 × 10 -2 ; weighted median OR = 1.39 [95% CI, 1.21-1.61], P = 1.62 × 10 -6 ). MR-Egger intercepts and funnel plots showed no directional pleiotropic effects between high WC and AF. CONCLUSIONS: Our findings suggest that greater WC is associated with an increased risk of AF. Taking measures to reduce WC may help prevent the occurrence of AF.


Assuntos
Fibrilação Atrial , Humanos , Fibrilação Atrial/genética , Estudo de Associação Genômica Ampla , Circunferência da Cintura/genética , Biologia Computacional , Bases de Dados Factuais
7.
ACS Nano ; 18(1): 337-346, 2024 Jan 09.
Artigo em Inglês | MEDLINE | ID: mdl-38113246

RESUMO

Layered oxides are widely accepted to be promising cathode candidate materials for K-ion batteries (KIBs) in terms of their rich raw materials and low price, while their further applications are restricted by sluggish kinetics and poor structural stability. Here, the high-entropy design concept is introduced into layered KIB cathodes to address the above issues, and an example of high-entropy layered K0.45Mn0.60Ni0.075Fe0.075Co0.075Ti0.10Cu0.05Mg0.025O2 (HE-KMO) is successfully prepared. Benefiting from the high-entropy oxide with multielement doping, the developed HE-KMO exhibits half-metallic oxide features with a narrow bandgap of 0.19 eV. Increased entropy can also reduce the surface energy of the {010} active facets, resulting in about 2.6 times more exposure of the {010} active facets of HE-KMO than the low-entropy K0.45MnO2 (KMO). Both can effectively improve the kinetics in terms of electron conduction and K+ diffusion. Furthermore, high entropy can inhibit space charge ordering during K+ (de)insertion, and the transition metal-oxygen covalent interaction of HE-KMO is also enhanced, leading to suppressed phase transition of HE-KMO in 1.5-4.2 V and better electrochemical stability of HE-KMO (average capacity drop of 0.20%, 200 cycles) than the low-entropy KMO (average capacity drop of 0.41%, 200 cycles) in the wide voltage window.

9.
Ultrason Sonochem ; 101: 106683, 2023 Dec.
Artigo em Inglês | MEDLINE | ID: mdl-37948893

RESUMO

In this study, we aimed to investigate the impact of various ultrasound durations on the structure and bioactivity of sweet corncob polysaccharides treated with ultrasound-assisted degradation using hydrogen peroxide and ascorbic acid (H2O2-Vc). We subjected sweet corncob polysaccharides to ultrasound treatment for 0, 30, 60, and 90 min alongside the H2O2-Vc method. We then analyzed their chemical composition and structure. Additionally, we administered these polysaccharides to mice with type 2 diabetes (T2DM) through gavage at a dosage of 200 mg/kg/day. The results indicated a significant reduction in the molecular weight of the degraded sweet corncob polysaccharides, while their composition remained relatively stable. However, the basic structure of the polysaccharides was retained. In vivo experiments demonstrated that ultrasound-assisted degradation of these polysaccharides had a positive impact on T2DM, particularly the 60-minute ultrasound treatment (UH-DSCBP-60 min), which effectively controlled blood glucose levels by regulating glycolipid metabolism in the livers of mice with T2DM. This approach also reduced inflammation and oxidative stress levels and inhibited disaccharide activity in the small intestine. We demonstrated that ultrasound can positively affect the sweet corncob polysaccharides hypoglycemic activity. The findings of our study provide a theoretical foundation for the valuable utilization of sweet corncob polysaccharides.


Assuntos
Ácido Ascórbico , Diabetes Mellitus Tipo 2 , Animais , Camundongos , Ácido Ascórbico/química , Diabetes Mellitus Tipo 2/tratamento farmacológico , Peróxido de Hidrogênio/química , Zea mays/química , Polissacarídeos/química
10.
Nat Commun ; 14(1): 5210, 2023 Aug 25.
Artigo em Inglês | MEDLINE | ID: mdl-37626068

RESUMO

Na Super Ionic Conductor (NASICON) materials are an important class of solid-state electrolytes owing to their high ionic conductivity and superior chemical and electrochemical stability. In this paper, we combine first-principles calculations, experimental synthesis and testing, and natural language-driven text-mined historical data on NASICON ionic conductivity to achieve clear insights into how chemical composition influences the Na-ion conductivity. These insights, together with a high-throughput first-principles analysis of the compositional space over which NASICONs are expected to be stable, lead to the successful synthesis and electrochemical investigation of several new NASICONs solid-state conductors. Among these, a high ionic conductivity of 1.2 mS cm-1 could be achieved at 25 °C. We find that the ionic conductivity increases with average metal size up to a certain value and that the substitution of PO4 polyanions by SiO4 also enhances the ionic conductivity. While optimal ionic conductivity is found near a Na content of 3 per formula unit, the exact optimum depends on other compositional variables. Surprisingly, the Na content enhances the ionic conductivity mostly through its effect on the activation barrier, rather than through the carrier concentration. These deconvoluted design criteria may provide guidelines for the design of optimized NASICON conductors.

11.
Thromb Res ; 229: 243-251, 2023 09.
Artigo em Inglês | MEDLINE | ID: mdl-37591154

RESUMO

INTRODUCTION: The association between bleeding and subsequent major adverse cardiac and cerebrovascular events (MACCE) remains poorly characterized. We aimed to evaluate the impact of hemorrhagic events in patients with atrial fibrillation (AF) and acute coronary syndrome (ACS) or undergoing percutaneous coronary intervention (PCI). MATERIALS AND METHODS: A total of 1877 consecutive patients with AF and ACS or undergoing PCI were prospectively recruited. The primary endpoint was MACCE, including all-cause death, myocardial infarction, ischemic stroke, systemic embolism or ischemia-driven revascularization during follow-up. Post-discharge bleeding was graded according to TIMI criteria. Associations between bleeding and subsequent MACCE were examined using time-dependent multivariate Cox regression after adjusting for baseline covariates and the time from bleeding. RESULTS: During a median follow-up of 34.2 months, 341 (18.2 %) had TIMI major or minor bleeding events, of whom 86 (25.2 %) also experienced MACCE. The risk of MACCE was significantly higher in patients with bleeding than those without (8.85 % versus 6.99 % per patient-year; HR, 1.568, 95 % CI, 1.232-1.994). In patients who had both bleeding and MACCE, 65.1 % (56 of 86) bleeding events occurred first. Temporal gradients in MACCE risk after major bleeding was highest within 30 days (HRadj, 23.877; 95 % CI, 12.810-44.506) and remained significant beyond 1 year (HRadj, 3.640; 95 % CI, 1.278-10.366). Minor bleeding was associated with increased risk of MACCE within 1 year. CONCLUSIONS: In patients with AF and ACS or PCI, major and minor bleeding were associated with subsequent MACCE with time-dependency. Our findings may aid in better defining net clinical benefit of optimal antithrombotic therapy.


Assuntos
Síndrome Coronariana Aguda , Fibrilação Atrial , Intervenção Coronária Percutânea , Humanos , Fibrilação Atrial/complicações , Síndrome Coronariana Aguda/complicações , Assistência ao Convalescente , Intervenção Coronária Percutânea/efeitos adversos , Alta do Paciente , Hemorragia/etiologia
12.
Proc Natl Acad Sci U S A ; 120(31): e2301260120, 2023 Aug.
Artigo em Inglês | MEDLINE | ID: mdl-37487097

RESUMO

Lithium-sulfur (Li-S) batteries with high energy density and low cost are promising for next-generation energy storage. However, their cycling stability is plagued by the high solubility of lithium polysulfide (LiPS) intermediates, causing fast capacity decay and severe self-discharge. Exploring electrolytes with low LiPS solubility has shown promising results toward addressing these challenges. However, here, we report that electrolytes with moderate LiPS solubility are more effective for simultaneously limiting the shuttling effect and achieving good Li-S reaction kinetics. We explored a range of solubility from 37 to 1,100 mM (based on S atom, [S]) and found that a moderate solubility from 50 to 200 mM [S] performed the best. Using a series of electrolyte solvents with various degrees of fluorination, we formulated the Single-Solvent, Single-Salt, Standard Salt concentration with Moderate LiPSs solubility Electrolytes (termed S6MILE) for Li-S batteries. Among the designed electrolytes, Li-S cells using fluorinated-1,2-diethoxyethane S6MILE (F4DEE-S6MILE) showed the highest capacity of 1,160 mAh g-1 at 0.05 C at room temperature. At 60 °C, fluorinated-1,4-dimethoxybutane S6MILE (F4DMB-S6MILE) gave the highest capacity of 1,526 mAh g-1 at 0.05 C and an average CE of 99.89% for 150 cycles at 0.2 C under lean electrolyte conditions. This is a fivefold increase in cycle life compared with other conventional ether-based electrolytes. Moreover, we observed a long calendar aging life, with a capacity increase/recovery of 4.3% after resting for 30 d using F4DMB-S6MILE. Furthermore, the correlation between LiPS solubility, degree of fluorination of the electrolyte solvent, and battery performance was systematically investigated.

13.
Nano Lett ; 23(13): 5967-5974, 2023 Jul 12.
Artigo em Inglês | MEDLINE | ID: mdl-37350461

RESUMO

Lithium-sulfur (Li-S) batteries are promising candidates for next-generation energy storage systems due to their high theoretical energy density and the low cost of sulfur. However, slow conversion kinetics between the insulating S and lithium sulfide (Li2S) remains as a technical challenge. In this work, we report a catalyst featuring nickel (Ni) single atoms and clusters anchored to a porous hydrogen-substituted graphdiyne support (termed Ni@HGDY), which is incorporated in Li2S cathodes. The rapidly synthesized catalyst was found to enhance ionic and electronic conductivity, decrease the reaction overpotential, and promote more complete conversion between Li2S and sulfur. The addition of Ni@HGDY to commercial Li2S powder enabled a capacity of over 516 mAh gLi2S-1 at 1 C for over 125 cycles, whereas the control Li2S cathode managed to maintain just over 200 mAh gLi2S-1. These findings highlight the efficacy of Ni as a metal catalyst and demonstrate the promise of HGDY in energy storage devices.

14.
Nat Commun ; 14(1): 1275, 2023 Mar 08.
Artigo em Inglês | MEDLINE | ID: mdl-36882392

RESUMO

A key strategy to design environmental barrier coatings focuses on doping multiple rare-earth principal components into ß-type rare-earth disilicates (RE2Si2O7) to achieve versatile property optimization. However, controlling the phase formation capability of (nRExi)2Si2O7 remains a crucial challenge, due to the complex polymorphic phase competitions and evolutions led by different RE3+ combination. Herein, by fabricating twenty-one model (REI0.25REII0.25REIII0.25REIV0.25)2Si2O7 compounds, we find that their formation capability can be evaluated by the ability to accommodate configurational randomness of multiple RE3+ cations in ß-type lattice while preventing the ß-to-γ polymorphic transformation. The phase formation and stabilization are controlled by the average RE3+ radius and the deviations of different RE3+ combinations. Subsequently, based on high-throughput density-functional-theory calculations, we propose that the configurational entropy of mixing is a reliable descriptor to predict the phase formation of ß-type (nRExi)2Si2O7. The results may accelerate the design of (nRExi)2Si2O7 materials with tailored compositions and controlled polymorphic phases.

15.
ACS Omega ; 8(9): 8894-8909, 2023 Mar 07.
Artigo em Inglês | MEDLINE | ID: mdl-36910938

RESUMO

As an aprotic O-donor ligand, 4,4'-bipyridine N,N'-dioxide (DPO) shows good potential for the preparation of uranyl coordination compounds. In this work, by regulating reactant compositions and synthesis conditions, diverse coordination assembly between uranyl and DPO under different reaction conditions was achieved in the presence of other coexisting O-donors. A total of ten uranyl-DPO compounds, U-DPO-1 to U-DPO-10, have been synthesized by evaporation or hydro/solvothermal treatment, and the possible competition and cooperation of DPO with other O-donors for the formation of these uranyl-DPO compounds are discussed. Starting with an aqueous solution of uranyl nitrate, it is found that an anionic nitrate or hydroxyl group is involved in the coordination sphere of uranyl in U-DPO-1 ((UO2)(NO3)2(H2O)2·(DPO)), U-DPO-2 ((UO2)(NO3)2(DPO)), and U-DPO-3 ((UO2)(DPO)(µ2-OH)2), where DPO takes three different kinds of coordination modes, i.e. uncoordinated, monodentate, and biconnected. The utilization of UO2(CF3SO3)2 in acetonitrile, instead of an aqueous solution of uranyl nitrate, precludes the participation of nitrate and hydroxyl, and ensures the engagement of DPO ligands (4-5 DPO ligands for each uranyl) in a uranyl coordination sphere of U-DPO-4 ([(UO2)(CF3SO3)(DPO)2](CF3SO3)), U-DPO-5 ([UO2(H2O)(DPO)2](CF3SO3)2) and U-DPO-6 ([(UO2)(DPO)2.5](CF3SO3)2). Moreover, when combined with anionic carboxylate ligands, terephthalic acid (H2TPA), isophthalic acid (H2IPA), and succinic acid (H2SA), DPO works well with them to produce four mixed-ligand uranyl compounds with similar structures of two-dimensional (2D) networks or three-dimensional (3D) frameworks, U-DPO-7 ((UO2)(TPA)(DPO)), U-DPO-8 ((UO2)2(DPO)(IPA)2·0.5H2O), U-DPO-9 ((UO2)(SA)(DPO)·H2O), and U-DPO-10 ((UO2)2(µ2-OH)(SA)1.5(DPO)). Density functional theory (DFT) calculations conducted to probe the bonding features between uranyl ions and different O-donor ligands show that the bonding ability of DPO is better than that of anionic CF3SO3 -, nitrate, and a neutral H2O molecule and comparable to that of an anionic carboxylate group. Characterization of physicochemical properties of U-DPO-7 and U-DPO-10 with high phase purity including infrared (IR) spectroscopy, thermogravimetric analysis (TGA), and luminescence properties is also provided.

16.
Proc Natl Acad Sci U S A ; 120(10): e2214357120, 2023 Mar 07.
Artigo em Inglês | MEDLINE | ID: mdl-36848560

RESUMO

Improving Coulombic efficiency (CE) is key to the adoption of high energy density lithium metal batteries. Liquid electrolyte engineering has emerged as a promising strategy for improving the CE of lithium metal batteries, but its complexity renders the performance prediction and design of electrolytes challenging. Here, we develop machine learning (ML) models that assist and accelerate the design of high-performance electrolytes. Using the elemental composition of electrolytes as the features of our models, we apply linear regression, random forest, and bagging models to identify the critical features for predicting CE. Our models reveal that a reduction in the solvent oxygen content is critical for superior CE. We use the ML models to design electrolyte formulations with fluorine-free solvents that achieve a high CE of 99.70%. This work highlights the promise of data-driven approaches that can accelerate the design of high-performance electrolytes for lithium metal batteries.

17.
Sci Adv ; 9(2): eadc9721, 2023 Jan 13.
Artigo em Inglês | MEDLINE | ID: mdl-36638171

RESUMO

Determining the degree and the spatial extent of structural order in liquids is a grand challenge. Here, we are able to resolve the structural order in a model organic electrolyte of 1 M lithium hexafluorophosphate (LiPF6) dissolved in 1:1 (v/v) ethylene carbonate:diethylcarbonate by developing an integrated method of liquid-phase transmission electron microscopy (TEM), cryo-TEM operated at -30°C, four-dimensional scanning TEM, and data analysis based on deep learning. This study reveals the presence of short-range order (SRO) in the high-salt concentration domains of the liquid electrolyte from liquid phase separation at the low temperature. Molecular dynamics simulations suggest the SRO originates from the Li+-(PF6-)n (n > 2) local structural order induced by high LiPF6 salt concentration.

18.
ACS Nano ; 17(3): 3168-3180, 2023 Feb 14.
Artigo em Inglês | MEDLINE | ID: mdl-36700841

RESUMO

Inorganic-rich solid-electrolyte interphases (SEIs) on Li metal anodes improve the electrochemical performance of Li metal batteries (LMBs). Therefore, a fundamental understanding of the roles played by essential inorganic compounds in SEIs is critical to realizing and developing high-performance LMBs. Among the prevalent SEI inorganic compounds observed for Li metal anodes, Li3N is often found in the SEIs of high-performance LMBs. Herein, we elucidate new features of Li3N by utilizing a suspension electrolyte design that contributes to the improved electrochemical performance of the Li metal anode. Through empirical and computational studies, we show that Li3N guides Li electrodeposition along its surface, creates a weakly solvating environment by decreasing Li+-solvent coordination, induces organic-poor SEI on the Li metal anode, and facilitates Li+ transport in the electrolyte. Importantly, recognizing specific roles of SEI inorganics for Li metal anodes can serve as one of the rational guidelines to design and optimize SEIs through electrolyte engineering for LMBs.

19.
Nat Nanotechnol ; 18(2): 153-159, 2023 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-36585516

RESUMO

Metastable nanomaterials, such as single-atom and high-entropy systems, with exciting physical and chemical properties are increasingly important for next-generation technologies. Here, we developed a hydrogen-substituted graphdiyne-assisted ultrafast sparking synthesis (GAUSS) platform for the preparation of metastable nanomaterials. The GAUSS platform can reach an ultra-high reaction temperature of 3,286 K within 8 ms, a rate exceeding 105 K s-1. Controlling the composition and chemistry of the hydrogen-substituted graphdiyne aerogel framework, the reaction temperature can be tuned from 1,640 K to 3,286 K. We demonstrate the versatility of the GAUSS platform with the successful synthesis of single atoms, high-entropy alloys and high-entropy oxides. Electrochemical measurements and density functional theory show that single atoms synthesized by GAUSS enhance the lithium-sulfur redox reaction kinetics in all-solid-state lithium-sulfur batteries. Our design of the GAUSS platform offers a powerful way to synthesize a variety of metastable nanomaterials.

20.
J Cardiovasc Dev Dis ; 9(12)2022 Nov 30.
Artigo em Inglês | MEDLINE | ID: mdl-36547423

RESUMO

Aims: Patients with left ventricular noncompaction (LVNC) are at risk of thromboembolism. The relationship between left atrial diameter (LAD), a robust predictor for thrombosis, and LVNC is unclear. The purpose of this study was to explore the effect of LAD on the thrombotic risk in LVNC. Methods: In this retrospective cohort study, 320 patients with imaging characteristics of LVNC were included for statistical analysis. The primary endpoint was a composite event of intracardiac thrombi and stroke or transient ischemic attack (TIA). The secondary endpoints were intracardiac thrombi and stroke/TIA. Results: The 320 included patients (211 [65.9%] men, median age: 45 years [interquartile range: 30−57]) were divided into LAD1 (<43 mm, n = 157) and LAD2 (≥43 mm, n = 163) groups based on the median LAD. Throughout the median follow-up of 34 months, the incidence of thromboembolism among them was 7.2%: 11 (3.4%) patients had stroke/TIA and 14 (4.4%) had intracardiac thrombi. The rate of thromboembolism in the LAD2 group was higher than that of patients in the LAD1 group (11.0% vs. 3.2%, p = 0.007). Kaplan−Meier survival curves suggested that a LAD ≥ 43 mm was associated with a higher risk of thromboembolism and intracardiac thrombi (log-rank test, all p < 0.05). After adjusting for potential risk factors, LAD ≥ 43 mm was found to be an independent risk factor for thromboembolism (p = 0.013) and stroke (p = 0.024). The area under the receiver operating characteristic curve of LAD for predicting thromboembolism reached 0.696 at 1 year, 0.635 at 2 years, and 0.660 at 3 years. Conclusions: A larger LAD was related to a higher risk of thromboembolism in patients with LVNC. The LAD may be a useful predictor for thrombotic risk stratification among such patients.

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