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1.
J Colloid Interface Sci ; 677(Pt A): 655-664, 2025 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-39116563

RESUMO

Germanium based nanomaterials are very promising as the anodes for the lithium ion batteries since their large specific capacity, excellent lithium diffusivity and high conductivity. However, their controllable preparation is still very difficult to achieve. Herein, we facilely prepare a unique carbon coating Ge nanospheres with a cubic hollow structure (Ge@C) via a hydrothermal synthesis and subsequent pyrolysis using low-cost GeO2 as precursors. The hollow Ge@C nanostructure not only provides abundant interior space to alleviate the huge volumetric expansion of Ge upon lithiation, but also facilitates the transmission of lithium ions and electrons. Moreover, experiment analyses and density functional theory (DFT) calculations unveil the excellent lithium adsorption ability, high exchange current density, low activation energy for lithium diffusion of the hollow Ge@C electrode, thus exhibiting significant lithium storage advantages with a large charge capacity (1483 mAh/g under 200 mA g-1), distinguished rate ability (710 mAh/g under 8000 mA g-1) as well as long-term cycling stability (1130 mAh/g after 900 cycles under 1000 mA g-1). Therefore, this work offers new paths for controllable synthesis and fabrication of high-performance Ge based lithium storage nanomaterials.

2.
J Colloid Interface Sci ; 677(Pt B): 161-170, 2025 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-39142157

RESUMO

Two-dimensional nanosheets, with their distinct characteristics, are widely used in various applications such as water splitting, supercapacitors, catalysis etc. In this research, we produced Cu-BDC MOF nanosheets by using Cu2O nanotubes for metal ions and H2BDC as the organic linker. We combined these Cu-BDC MOF nanosheets with reduced graphene oxide (rGO) to form a nanocomposite. The collaboration between Cu-BDC MOF and rGO boosts both the catalytic reduction of 4-nitrophenol and the electrochemical capabilities. The conversion of 4-nitrophenol to 4-aminophenol is achieved using sodium borohydride as both a reducing agent and a catalyst. The study explores the impact of different concentrations of 4-nitrophenol and sodium borohydride on catalytic efficiency. The increase in sodium borohydride concentration enhances catalytic efficiency by providing more BH4- ions and electrons for the reduction process. The catalytic reduction process adheres to the Langmuir-Hinshelwood mechanism with apparent pseudo-first-order kinetics. Specifically, Cu-BDC MOF and rGO/Cu-BDC MOF exhibit specific capacities of 468.4 mA h/g and 656.4 mA h/g at a current density of 2 A/g, respectively, while also enhancing the operating voltage window. Therefore, electrodes based on rGO/Cu-BDC MOF nanosheets present a novel approach for environmental remediation and energy storage applications across various fields.

3.
J Colloid Interface Sci ; 677(Pt B): 312-322, 2025 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-39151224

RESUMO

Heteroatom-doped carbon has been widely investigated as anode materials for sodium-ion batteries (SIBs). However, simplifying the preparation process and precisely controlling their microstructure to achieve excellent Na+ storage performance remain significant challenges. Therefore, in this study, high-performance N, P co-doped Na+ storage carbon anode electrode materials were prepared by one-step carbonization using N, P-rich Eichhornia crassipes (EC) as raw materials and systematically tested for their Na+ storage performance. The doping levels of N and P atoms as well as the spatial structure of the carbon material were adjusted by changing the carbonization temperature during the pyrolysis process. Among them, the anode material corresponding to 1300 °C (EC-PN1300) showed an excellent Na+ storage capacity of 336 ± 4 mAh g-1 (50 mA g-1) and excellent cycling stability (99.8 % retention after 2000 cycles). In addition, the Na+ storage mechanism of EC-PN1300 was systematically analyzed using galvanostatic intermittent titration (GITT), ex-situ XPS and in-situ Raman spectroscopy, providing accurate research directions for developing carbon anode electrode materials with superior electrochemical performance. This study not only provides some insights into the preparation of carbon anode materials in alkali metal batteries and the development of carbon materials in other fields, but also realizes the interaction between environmental protection and new energy development.

4.
J Colloid Interface Sci ; 677(Pt B): 1034-1044, 2025 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-39178667

RESUMO

The interfacial effect is important for the tungsten trioxide (WO3)-based anode to achieve superior lithium-ion storage performance. Herein, the interfacial effect was constructed by in-situ surface direct nitridation reaction at 600 â„ƒ for 30 min of the as-synthesis WO3 nanoparticles (WO3/WN). X-ray photoelectron spectroscopy (XPS) analysis confirms evident chemical interaction between WO3 and WN via the interfacial covalent bond (WON). This WO3/WN anode shows a distinct interfacial effect for an efficient interatomic electron migration. Electrochemical kinetic analysis shows enhanced pseudocapacitance contribution. The galvanostatic intermittent titration technique (GITT) result demonstrates improved charge transfer kinetics. Ex-situ X-ray diffraction (XRD) analysis reveals the reversible oxidation and reduction reaction of the WO3/WN anode. The density functional theory (DFT) result shows that the evident interfacial bonding effect can enhance the electrochemical reaction kinetics of the WO3/WN anode. The discharge capacity can reach up to 546.9 mA h g-1 at 0.1 A g-1 after 200 cycles. After 2000 cycles, the capacity retention is approximately 85.97 % at 1.0 A g-1. In addition, the WO3/WN full cell (LiFePO4/C//WO3/WN) demonstrates excellent rate capability and capacity retention ratio. This in-situ surface nitridation strategy is an effective solution for designing an oxide-based anode with good electrochemical performance and beyond.

5.
Insect Sci ; 2024 Sep 30.
Artigo em Inglês | MEDLINE | ID: mdl-39350323

RESUMO

In the organisms with XX/XY sex chromosomes, Y chromosome is unique to males and plays an important role in male reproductive development. The study of Y chromosome genes will contribute to the development of pest genetic prevention and control technology. In this study, we identified 9 Y chromosome genes in Zeugodacus tau (Diptera: Tephritidae), including gene 16222. Protein structure analysis showed that 16222 was highly similar to odorant binding protein, and thus gene 16222 was named obp-Y. Obp-Y knockout (KO) significantly reduced hatching rate of offspring. Sperm detection results showed that obp-Y KO did not affect sperm number in the testes or sperm transfer during mating. We further examined the storage of sperms in females, and found that sperms in females mating with wild-type males began to transfer from spermathecal ducts to the spermathecae at hour 0 after the end of mating (AEM), and at 0-24 h AEM, the sperm count in the spermathecae gradually increased. However, no sperms were observed in spermathecae of females mating with mutant males at hours 0, 4, 8, 24 and 48 AEM. In summary, this study revealed that Y chromosome gene obp-Y was necessary for the storage of sperms in females. Our findings not only provide theoretical basis for elucidating the function of the Y chromosome, but also offer a molecular target for the genetic control over Z. tau.

6.
Plant Physiol ; 2024 Oct 01.
Artigo em Inglês | MEDLINE | ID: mdl-39351808

RESUMO

Coat protein complex II (COPII) vesicles play crucial roles in mediating the endoplasmic reticulum (ER) exit of newly synthesized proteins to the Golgi in eukaryotic cells. However, the molecular functions of COPII components and their functional diversifications in plant seeds remain obscure. Here, we showed that the rice (Oryza sativa) glutelin precursor accumulation12 (gpa12) mutant is defective in storage protein export from the ER, resulting in the formation of aggregated protein bodies. Map-based cloning revealed that GPA12 encodes a COPII outer layer protein, Sec13a, that mainly localizes to endoplasmic reticulum exit sites (ERES) and partially localizes to the Golgi. Biochemical experiments verified that Sec13a physically interacts with Sec31 and Sec16, and mutation in Sec13 compromises its interaction with Sec31 and Sec16, thereby affecting the membrane association of the inner complex components Sar1b and Sec23c. Apart from Sec13a, the rice genome encodes two other Sec13 isoforms, Sec13b and Sec13c. Notably, we observed an abnormal accumulation of globular ER structures in the sec13bc double mutant but not in the single mutants, suggesting a functional redundancy of Sec13b and Sec13c in modulating ER morphology. Taken together, our results substantiated that Sec13a plays an important role in regulating storage protein export from the ER, while Sec13b and Sec13c are required for maintaining ER morphology in rice endosperm cells. Our findings provide insights into the functional diversification of COPII components in plants.

7.
Adv Sci (Weinh) ; : e2407297, 2024 Oct 01.
Artigo em Inglês | MEDLINE | ID: mdl-39352306

RESUMO

Metal-organic frameworks (MOFs) deliver potential applications in electrochromism and energy storage. However, the poor intrinsic conductivity of MOFs in electrolytes seriously hampers the development of the above-mentioned electrochemical applications, especially in one MOF electrode. Herein, a new Ni-based MOF (denoted Ni-DPNDI) is proposed with enhanced conductivity by π-delocalized DPNDI connectors. Predictably, the obtained Ni-DPNDI MOF achieves a conductivity of up to 4.63 S∙m-1 at 300 K. Profiting from its unique electronic structure, the Ni-DPNDI MOF delivers excellent electrochromic and energy storage performance with a great optical modulation (60.8%), a fast switching speed (tc = 7.9 s and tb = 6.4 s), a moderate specific capacitance (25.3 mAh·g-1) and good cycle stability over 2000 times. Meanwhile, energy storage capacity is visual by the coloration states of Ni-DPNDI film. As a proof of the potential application, a large-area (100 cm2) electrochromic energy storage smart window is further designed and displayed. The strategy provides an interesting alternative to porous multifunctional materials for the new generation of electronic devices with diverse applications.

8.
Artigo em Inglês | MEDLINE | ID: mdl-39352577

RESUMO

Managing Inherited Metabolic Disorders (IMDs) at risk for hypoglycemia, such as Glycogen Storage Diseases (GSDs), Hereditary Fructose Metabolism Disorders (HFMDs) and Congenital Hyperinsulinism (CH), poses challenges in dietary treatments and blood glucose monitoring. The effectiveness of Continuous Glucose Monitoring (CGM) remains a subject of ongoing debate, with IMD guidelines maintaining caution. Therefore, a systematic evaluation is needed to understand the potential benefits of CGM during dietary interventions. A systematic literature review was conducted in PubMed according to the PICOS model and PRISMA recommendations on studies published from January 01, 2003, up to October 15, 2023 (PROSPERO CRD42024497744). The risk of bias was assessed using NIH Quality Assessment Tools. Twenty-four studies in GSDs (n = 13), CH (n = 10), and HFMDs (n = 1) were analyzed. In GSDs, Real-time CGM (Rt-CGM) was associated with metabolic benefits during nutritional interventions, proving to be an accurate system for hypoglycemia detection although with some concerns about reliability. Rt-CGM in CH, primarily involving children, also showed potential benefits for glycemic control and metabolic stability with acceptable accuracy, although its use during dietary changes was limited. Few experiences on Flash Glucose Monitoring (FGM) were reported, with some concerns about reliability. Overall, the studies analyzed presented different designs, and their quality was predominantly fair or poor. Heterogeneity and limited consensus on reliability and glycemic targets underscore the need for prospective studies and future recommendations for the use of CGM in optimizing nutritional status and providing personalized dietary education in individuals with IMDs prone to hypoglycemia.

9.
Natl Sci Rev ; 11(10): nwae309, 2024 Oct.
Artigo em Inglês | MEDLINE | ID: mdl-39355271

RESUMO

The significant volume of existing buildings and ongoing annual construction of infrastructure underscore the vast potential for integrating large-scale energy-storage solutions into these structures. Herein, we propose an innovative approach for developing structural and scalable energy-storage systems by integrating safe and cost-effective zinc-ion hybrid supercapacitors into cement mortar, which is the predominant material used for structural purposes. By performing air entrainment and leveraging the adverse reaction of the ZnSO4 electrolyte, we can engineer an aerated cement mortar with a multiscale pore structure that exhibits dual functionality: effective ion conductivity in the form of a cell separator and a robust load-bearing capacity that contributes to structural integrity. Consequently, a hybrid supercapacitor building block consisting of a tailored cement mortar, zinc metal anode and active carbon cathode demonstrates exceptional specific energy density (71.4 Wh kg-1 at 68.7 W kg-1), high areal energy density (2.0 Wh m-2 at 1.9 W m-2), favorable cycling stability (∼92% capacity retention after 1000 cycles) and exceptional safety (endurance in a 1-hour combustion test). By demonstrating the scalability of the structural energy-storage system coupled with solar energy generation, this new device exhibits great potential to revolutionize energy-storage systems.

10.
Nagoya J Med Sci ; 86(3): 361-369, 2024 Aug.
Artigo em Inglês | MEDLINE | ID: mdl-39355366

RESUMO

Despite recent advance in the study of the nature of storage iron turnover, a comprehensive analysis remains lacking. This study aimed to clarify the nature of storage iron turnover. Ferritin-hemosiderin iron transformation rate and the standard normal storage iron turnover rate were utilized in this study to describe the mechanism of iron absorption in relation to ferritin and hemosiderin iron turnover. The synchronization of radioiron uptake peaks by bone marrow and liver indicates that the distribution of radioiron is proportional to the pre-existing iron levels in organs at 24 h after radioiron injection. Moreover, the synchronization indicates the independence of iron mass from red cell precursors in acquiring plasma iron. Thus, the erythron does not dominate the radioiron uptake process. The inverse correlation between transformation rate and the amount of pre-existing iron storage implies that the intra-storage iron turnover is active in iron deficiency, but inactive in iron overload. The decreased ferritin/hemosiderin iron ratio in chronic hepatitis C (CHC) with normal iron storage suggests a trend of iron transformation from ferritin into hemosiderin. The correlation between the pretreatment iron storage and the speed of rebound in CHC implies that the vacant iron-storing rooms in iron-removed cells have a potential to increase iron absorption. This study presents new insights into the turnover of stored iron to enhance our understanding of iron metabolism in various hematologic disorders.


Assuntos
Ferritinas , Hemossiderina , Ferro , Fígado , Hemossiderina/metabolismo , Ferritinas/metabolismo , Ferro/metabolismo , Humanos , Fígado/metabolismo , Animais , Masculino , Medula Óssea/metabolismo , Radioisótopos de Ferro
11.
Food Chem ; 463(Pt 4): 141447, 2024 Sep 27.
Artigo em Inglês | MEDLINE | ID: mdl-39357308

RESUMO

This study investigated changes in the metabolome of fresh beef, lamb, and venison in relation to colour stability during display storage. Changes in meat colour and metabolites in loin muscles (Longissimus lumborum) of beef, lamb and venison were determined under a simulated retail display at 4 °C. Metabolite analysis was performed using nuclear magnetic resonance (NMR) spectroscopy, and 27 metabolites were identified. The stability of fresh meat colour was found to be in the following order: beef > lamb > venison. Several trends were observed, and amino acids and metabolites involved in ATP generation were found to be the most important. Leucine, isoleucine and valine were increased, whereas succinate, inosine monophosphate and choline were decreased over the storage time of all three meat types (p < 0.05). As a reduction in succinate, inosine monophosphate and choline during storage were found for all three meat types, these metabolites could potentially be associated with colour stability.

12.
Ann Pathol ; 2024 Oct 01.
Artigo em Francês | MEDLINE | ID: mdl-39358197

RESUMO

Thesaurismosis or storage diseases are rare genetic disorders due to an abnormal accumulation of an organic compound or its metabolite within cells. These conditions are either secondary to a defect in catabolism caused by enzymatic dysfunction or to a deficiency in transport proteins. They encompass lysosomal storage diseases, lipid storage diseases or dyslipidemias, and glycogen storage disorders or glycogenoses. Diagnosis is typically based on clinical and biological anomalies but may be made or suggested by the pathologist when symptoms are atypical or when biochemical or genetic tests are challenging to interpret. For accurate diagnosis, it is crucial to freeze a portion of the samples. Special staining and electronic microscopy can also aid in the diagnostic process. As the diagnosis is multidisciplinary, collaboration with clinicians, biochemists and geneticists is essential.

13.
J Esthet Restor Dent ; 2024 Oct 03.
Artigo em Inglês | MEDLINE | ID: mdl-39360391

RESUMO

OBJECTIVES: To evaluate the influence of preheating and water storage on color, whiteness, and translucency of one-shaded, group-shaded, and multi-shaded resin-based composites. MATERIALS AND METHODS: A total of 270 samples were fabricated from one-shaded (Omnichroma), group-shaded (Optishade MD), and multi-shaded (Enamel Plus HRI) resin-based composites and divided into six groups: no heating (control) and 1-5 heatings (test) (n = 15). The CIE L*, a*, b*, C*, and h° color coordinates were registered over white, black, and gray backgrounds with a spectrophotometer before and after 24, 72, 144 h water storage. Kruskal-Wallis test was used to evaluate differences in the color coordinates, whiteness index, and translucency parameter (α = 0.05). The Mann-Whitney U test was performed with a Bonferroni correction (p < 0.001) for pairwise comparisons. CIEDE2000 color, whiteness, and translucency differences between groups and subgroups were evaluated using their respective 50%:50% perceptibility and acceptability thresholds. RESULTS: Preheating influenced color coordinates, whiteness index, and relative translucency parameters (p < 0.001). Although color differences were below the acceptability threshold for all materials, translucency differences were above the acceptability threshold for Omnichroma. Water storage significantly influenced the whiteness index of Optishade MD (p < 0.001). CONCLUSIONS: Preheating had a more considerable effect on the color, whiteness, and translucency of one-shaded resin-based composite, while water storage influenced group-shaded resin-based composite more importantly. CLINICAL SIGNIFICANCE: Preheating influences the color, whiteness level, and translucency of the resin-based composites, but the variations remain generally clinically acceptable; however, practitioners should be aware that the modifications in translucency for one-shaded resin-based composites could be more important than for group-shaded and multi-shaded resin-based composites.

14.
Adv Sci (Weinh) ; : e2406216, 2024 Oct 03.
Artigo em Inglês | MEDLINE | ID: mdl-39360570

RESUMO

Shape memory alloys (SMAs) with large latent heat absorbed/released during phase transformation at elevated temperatures benefit their potential application on thermal energy storage (TES) in high temperature environment like power plants, etc. The desired alloys can be designed quickly by searching the vast component space of doped NiTi-based SMAs via data-driven method, while be challenging with the noisy experimental data. A noise-aware active learning strategy is proposed to accelerate the design of SMAs with large latent heat at elevated phase transformation temperatures based on noisy data. The optimal noise level is estimated by minimizing the model error with incorporation of a range of noise levels as noise hyper-parameters into the noise-aware Kriging model. The employment of this strategy leads to the discovery of the alloy with latent heat of -36.08 J g-1, 9.2% larger than the best value (-33.04 J g-1) in the original training dataset within another four experiments. Additionally, the alloy represents high austenite finish temperature (481.71°C) and relatively small hysteresis. This promotes the latent heat TES application of SMAs in high temperature circumstance. It is expected that the noise-aware approach can be convenient for the accelerated materials design via the data-driven method with noisy data.

15.
BMC Bioinformatics ; 25(1): 320, 2024 Oct 01.
Artigo em Inglês | MEDLINE | ID: mdl-39354338

RESUMO

BACKGROUND: Efficient DNA-based storage systems offer substantial capacity and longevity at reduced costs, addressing anticipated data growth. However, encoding data into DNA sequences is limited by two key constraints: 1) a maximum of h consecutive identical bases (homopolymer constraint h), and 2) a GC ratio between [ 0.5 - c GC , 0.5 + c GC ] (GC content constraint c GC ). Sequencing or synthesis errors tend to increase when these constraints are violated. RESULTS: In this research, we address a pure source coding problem in the context of DNA storage, considering both homopolymer and GC content constraints. We introduce a novel coding technique that adheres to these constraints while maintaining linear complexity for increased block lengths and achieving near-optimal rates. We demonstrate the effectiveness of the proposed method through experiments on both randomly generated data and existing files. For example, when h = 4 and c GC = 0.05 , the rate reached 1.988, close to the theoretical limit of 1.990. The associated code can be accessed at GitHub. CONCLUSION: We propose a variable-to-variable-length encoding method that does not rely on concatenating short predefined sequences, which achieves near-optimal rates.


Assuntos
Composição de Bases , DNA , DNA/química , Análise de Sequência de DNA/métodos , Algoritmos , Armazenamento e Recuperação da Informação/métodos
16.
Cureus ; 16(9): e68437, 2024 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-39360064

RESUMO

Introduction A frequency volume chart (FVC) or bladder diary (BD) is used to diagnose lower urinary tract symptoms and to determine the effectiveness of treatment. In outpatient practice, patients who use an FVC or BD may experience improvement in storage symptoms and not desire further treatment. The aim of this study was to determine the characteristics of patients who did not desire treatment after BD recording and to assess the changes in storage symptoms after BD recording. Methods This was a retrospective study. Patients who completed a three-day BD record were included. The patients were divided into two groups: those whose symptoms improved after using a BD and no longer desired treatment, and those who desired treatment. We compared endpoints including patient background, BD, Overactive Bladder Symptom Score (OABSS), and International Consultation on Incontinence Questionnaire-Urinary Incontinence Short Form (ICIQ-UI SF) score. Results We recruited 79 patients. Four patients were excluded (two were minors and two due to cognitive impairment). Thus, 75 patients were included in the analysis. Of these, 27 (36.0%) did not desire treatment for storage symptoms after BD recording. Compared with the group of patients who desired treatment, those who did not desire treatment had significantly lower daytime and nighttime frequency and number of leaks recorded in their BD, and there were fewer patients with nocturia and habitual caffeine consumption. Baseline OABSS and ICIQ-UI SF scores were lower and there were no significant changes in storage symptoms after BD recording. The cut-off value for the baseline total score of OABSS that did not desire treatment for storage symptoms after BD recording was 6 points. Conclusion In this study, 36.0% of patients no longer desired treatment for storage symptoms after using a BD. These patients initially exhibited a normal daily urinary frequency and mild storage symptoms. These findings suggest that among patients presenting to the outpatient clinic with storage symptoms, those with mild symptom severity and a total OABSS of 6 points or less may be able to avoid unnecessary treatment through BD recording.

17.
J Sci Food Agric ; 2024 Oct 02.
Artigo em Inglês | MEDLINE | ID: mdl-39354886

RESUMO

BACKGROUND: Nannochloropsis algae contain approximately 20% polyunsaturated fatty acids (PUFA) and hold significant potential for high-quality eicosapentaenoic acid (EPA) food industrialization. However, EPA in Nannochloropsis sp. is prone to oxidation, and microbial growth is a critical factor affecting the shelf life of fresh food. Storage composition and temperature are primary factors influencing microbial growth, yet these aspects are not fully understood. This study investigates the effects of temperature and encapsulation on EPA content in nano-products over time. Nano-powder and nanobeads derived from Nannochloropsis sp. served as raw materials. Additionally, changes in aerobic plate counts and coliform groups were monitored. RESULTS: The results indicated that nanobeads, due to their more complex processing and less mature packaging, were more susceptible to coliform contamination compared to nano-powder. In terms of EPA stability, nanobeads exhibited a longer storage life than nano-powder. The oxidation rate of both nano-powder and nanobeads was faster at 37 °C than at 25 °C. CONCLUSION: These findings can inform general shelf life estimation, rapid detection of total lipid content in nano-products and macro extraction of nano-oil. Moreover, they have significant implications for delaying EPA oxidation in nano-products and improving hygienic quality control for microbial detection. © 2024 Society of Chemical Industry.

18.
Chemistry ; : e202402597, 2024 Oct 02.
Artigo em Inglês | MEDLINE | ID: mdl-39355930

RESUMO

Biomass carbon has the advantages of wide source, low cost and environmental protection, and has been widely used in the field of electrochemical energy storage. In this work, N and S co-doped carbon materials were prepared by using peanut shell as carbon source and thiourea as activator. When the peanut shell and activator were 2 g and 4 g, respectively, the prepared NSPC-4 had the largest specific surface area and special pore structure. Elemental analysis showed that the activator introduced more N, S and O atoms to the carbon material, and more heteroatoms helped to improve the surface structure of the carbon material and provide additional pseudocapacitance. In addition, NSPC-4 contains a short-range ordered graphite structure, which can provide excellent electrical conductivity. The electrochemical test results show that NSPC-4 has the largest specific capacitance. When the mass of the activator is higher than or below 4 g, the electrochemical performance of the carbon material will be reduced. The symmetric supercapacitor (SSC) assembled by NSPC-4 has an energy density of 8.3 Wh kg-1 when the power density is 350 W kg-1. The synthesis method is not only simple, green and economical, but also has important application value.

19.
Artigo em Inglês | MEDLINE | ID: mdl-39356201

RESUMO

A machine learning (ML) model is developed for predicting useable methane (CH4) capacities in metal-organic frameworks (MOFs). The model applies to a wide variety of MOFs, including those with and without open metal sites, and predicts capacities for multiple pressure swing conditions. Despite its wider applicability, the model requires only 5 measurable structural features as input, yet achieves accuracies that surpass less-general models. Application of the model to a database of more than a million hypothetical MOFs identified several hundred whose capacities surpass that of the benchmark MOF, UMCM-152. Guided by the computational predictions, one of the promising candidates, UMCM-153, was synthesized and demonstrated to achieve superior volumetric capacity for CH4. Feature importance analyses reveal that pore volume and gravimetric surface area are the most important features for predicting CH4 capacity in MOFs. Finally, a reverse ML model is demonstrated. This model predicts the set of elementary MOF structural properties needed to achieve a desired CH4 capacity for a prescribed operating condition.

20.
Artigo em Inglês | MEDLINE | ID: mdl-39365083

RESUMO

Metal-organic frameworks (MOFs) have been widely studied for their ability to capture and store greenhouse gases. However, most computational discovery efforts study hypothetical MOFs without consideration of their stability, limiting the practical application of novel materials. We overcome this limitation by screening hypothetical ultrastable MOFs that have predicted high thermal and activation stability, as judged by machine learning (ML) models trained on experimental measures of stability. We enhance this set by computing the bulk modulus as a measure of mechanical stability and filter 1102 mechanically robust hypothetical MOFs from a database of ultrastable MOFs (USMOF DB). Grand Canonical Monte Carlo simulations are then employed to predict the gas adsorption properties of these hypothetical MOFs, alongside a database of experimental MOFs. We identify privileged building blocks that lead MOFs in USMOF DB to show exceptional working capacities compared to the experimental MOFs. We interpret these differences by training ML models on CO2 and CH4 adsorption in these databases, showing how poor model transferability between data sets indicates that novel design rules can be derived from USMOF DB that would not have been gathered through assessment of structurally characterized MOFs. We identify geometric features and node chemistry that will enable the rational design of MOFs with enhanced gas adsorption properties in synthetically realizable MOFs.

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