Your browser doesn't support javascript.
loading
Mostrar: 20 | 50 | 100
Resultados 1 - 20 de 144
Filtrar
1.
J Eur Acad Dermatol Venereol ; 38(1): 157-166, 2024 Jan.
Artículo en Inglés | MEDLINE | ID: mdl-37611262

RESUMEN

BACKGROUND: The German S2k guideline is the first to include a checklist that captures atopic dermatitis (AD) signs and symptoms as well as the lack of treatment response to identify patients eligible for systemic therapy. OBJECTIVES: Identifying candidates for a start/switch of systemic therapy in adult AD patients in Germany by applying the S2k guideline's checklist. METHODS: In this German multicentre, cross-sectional, non-interventional study (German Clinical Trials Register number: DRKS00023296), adult patients with mild to severe AD were enrolled at dermatological outpatient clinics and offices between April and October 2021. Demographics, clinical characteristics and quality of life were collected using questionnaires during one single visit. Eligibility for a start/switch of systemic AD therapy was evaluated according to the criteria of the German S2k guideline's checklist. RESULTS: Atopic dermatitis patients (575) were included in the analysis. One hundred and sixty-four patients (28.5%) received systemic (SYS) AD therapy and 411 patients (71.5%) did not (TOP). Of the TOP therapy patients, 38.7% were eligible to start systemic AD therapy, and about half of those (49.1%), were scheduled to start systemic AD therapy. The most frequent reason deciding against a systemic therapy was the patient's wish. Although 29.3% of SYS patients were eligible for a switch according to the criteria of the German S2k guideline's checklist, the majority (81.3%) did not switch AD therapy. CONCLUSIONS: This is the first study on the implementation of the German S2k guideline's checklist in everyday care of AD patients in Germany. More than one-third of the TOP patients were identified as eligible for systemic treatment. By applying the guideline's checklist criteria, another one-third of SYS patients may have benefited from a change of current systemic therapy. The use of the German S2k guideline's checklist in routine care represents an important tool to ensure effective patient care and identify inadequately treated patients.


Asunto(s)
Dermatitis Atópica , Adulto , Humanos , Dermatitis Atópica/terapia , Lista de Verificación , Estudios Transversales , Calidad de Vida , Alemania , Índice de Severidad de la Enfermedad
2.
Nano Lett ; 23(17): 7825-7830, 2023 Sep 13.
Artículo en Inglés | MEDLINE | ID: mdl-37638642

RESUMEN

Atomic layer deposition (ALD) is emerging as an efficient tool for the precise manufacture of catalysts, owing to its sophisticated surface tailoring capabilities. To overcome the techno-economic limitations of fuel cell electric vehicles (FCEVs), which are considered suitable alternatives to battery electric vehicles (BEVs), the development of cost-efficient high-performance catalysts is essential. In this study, we successfully fabricated a Pt-free cathode for a hydroxide exchange membrane fuel cell (HEMFC) with excellent oxygen reduction activity under extremely low loading of Ag electrocatalysts using ALD. Microstructural analysis confirmed that the surface modification by ALD-Ag nanoparticles exhibited excellent step coverage characteristics on porous carbon nanotubes (CNTs). An HEMFC comprising a CNT cathode surface-decorated with ALD-Ag nanoparticles delivered a high peak power density of 2154 mW mgAg-1 in an alkaline environment at 65 °C. This study demonstrates the applicability of ALD for the manufacture of highly active low-cost electrocatalysts for high-performance HEMFCs.

3.
J Dairy Sci ; 105(12): 9869-9881, 2022 Nov.
Artículo en Inglés | MEDLINE | ID: mdl-36207189

RESUMEN

The objectives of this descriptive study were to (1) describe the pharmacokinetics of salicylic acid (SA) in the milk and plasma of postpartum dairy cattle following oral administration of acetylsalicylic acid (ASA; aspirin), (2) to estimate a recommended milk withdrawal period for dairy cattle treated with ASA, and (3) to determine the effect of ASA administration on plasma prostaglandin E2 metabolite (PGEM) concentrations. Primiparous (n = 3) and multiparous (n = 7) postpartum Holstein dairy cows received 2 oral treatments with ASA at 200 mg/kg of body weight, 24 h apart. Concentrations of SA in plasma and milk from 0 h through 120 h after ASA administration were analyzed using ultra performance liquid chromatography triple quadrupole mass spectrometry and a milk withdrawal period was estimated using the United States Food and Drug Administration Milk Discard App in R. Two withdrawal periods were estimated: (1) a whole-herd treatment scenario with no dilution factor and (2) an individual animal treatment scenario with a bulk tank factor included in analysis. Plasma PGEM concentrations in samples from 0 h to 24 h after ASA administration were determined using a commercially available competitive ELISA. Milk SA concentrations were undetected in all cows by 48 h after the last ASA treatment. Secondary peaks were observed in plasma at 58 and 82 h after the last treatment and in milk at 87 h after the last treatment. In the absence of a tolerance for SA in milk, the estimated milk withdrawal periods were (1) 156 h for the whole-herd treatment scenario and (2) 120 h for the individual animal treatment scenario. Plasma PGEM concentrations were reduced compared with baseline for up to 12 h after ASA administration, with the greatest reduction observed at 2 h. Results from this study suggest that the current milk withhold recommendation for dairy cattle administered ASA may need revision to 120 h (5 d) and that ASA administration may mitigate postpartum inflammation through reduction in prostaglandin production for up to 12 h after treatment. Pharmacokinetic and milk withdrawal data from this study will inform future recommendations for extra-label use of aspirin in postpartum dairy cows. Further research is required to determine the basis for the secondary SA peaks and to elucidate the long-term effects of ASA administration on dairy cow health.


Asunto(s)
Aspirina , Leche , Femenino , Bovinos , Animales , Leche/química , Ácido Salicílico , Periodo Posparto/metabolismo , Prostaglandinas/metabolismo , Lactancia
4.
Phys Rev Lett ; 128(17): 176401, 2022 Apr 29.
Artículo en Inglés | MEDLINE | ID: mdl-35570444

RESUMEN

The "hydrogen atom" of magnetic Weyl semimetals, with the minimum number of Weyl points, has received growing attention recently due to the possible presence of Weyl-related phenomena. Here, we report a nontrivial electronic structure of the ferromagnetic alluaudite-type compound K_{2}Mn_{3}(AsO_{4})_{3}. It exhibits only a pair of Weyl points constrained in the z direction by the twofold rotation symmetry, leading to extremely long Fermi arc surface states. In addition, the study of its low-energy effective model results in the discovery of various topological superconducting states, such as the hydrogen atom of a Weyl superconductor. Our Letter provides a feasible platform to explore the intrinsic properties related to Weyl points, and the related device applications.

5.
Skeletal Radiol ; 51(7): 1453-1462, 2022 Jul.
Artículo en Inglés | MEDLINE | ID: mdl-35006279

RESUMEN

OBJECTIVE: The oblique orientation of the cervical neural foramina challenges the implementation of a short MRI protocol with concurrent excellent visualization of the spine. While sagittal oblique T2-weighted sequences permit good evaluation of the cervical neuroforamina, all segments may not be equally well depicted on a single sequence and conspicuity of foraminal stenosis may be limited. 3D T2-weighted sequences can be reformatted in arbitrary planes, including the sagittal oblique. We set out to compare 3D T2w SPACE sequences with sagittal oblique reformations and sagittal oblique 2D T2w TSE sequences for the evaluation of cervical foraminal visibility and stenosis. MATERIALS AND METHODS: Sixty consecutive patients who underwent MRI of the cervical spine with sagittal oblique 2D T2w TSE and 3D T2w SPACE sequences were included. Image homogeneity of the sequences was evaluated. Imaging sets were assessed for structure visibility and foraminal stenosis by two independent readers. Results of the sequences were compared by Wilcoxon matched-pairs tests. Interreader agreement was evaluated by weighted κ. RESULTS: Visibility of most structures was rated good to excellent on both sequences (mean visibility scores ≥ 4.5 of 5), though neuroforaminal contents were better seen on sagittal oblique T2w TSE (mean scores 4.1-4.6 vs. 3.1-4.1 on 3D T2w SPACE, p < 0.01). Stenosis grades were comparable between sequences (mean 1.1-2.6 of 4), with slightly higher values for 3D T2w SPACE at some levels (difference ≤ 0.3 points). CONCLUSION: 3D T2w SPACE is comparable with sagittal oblique 2D T2w TSE in the evaluation of cervical neural foramina.


Asunto(s)
Vértebras Cervicales , Imagen por Resonancia Magnética , Vértebras Cervicales/diagnóstico por imagen , Vértebras Cervicales/patología , Constricción Patológica/patología , Humanos , Imagenología Tridimensional/métodos , Imagen por Resonancia Magnética/métodos , Cuello
6.
J Occup Rehabil ; 32(1): 103-113, 2022 Mar.
Artículo en Inglés | MEDLINE | ID: mdl-34037926

RESUMEN

Purpose Chronic musculoskeletal pain can have a major impact on ability to work. The work ability score is a commonly used single-item question to assess work ability but has not been fully validated yet. The aim of the present study was to evaluate test-retest reliability, agreement, construct validity, and responsiveness of the work ability score among sick-listed workers with chronic musculoskeletal pain. Methods Data of sick-listed workers with chronic musculoskeletal pain was routinely collected at seven rehabilitation centres in the Netherlands. Assessments included a set of questionnaires, administered at admission and discharge from a fifteen-week vocational rehabilitation program. Test-retest reliability was determined with the intraclass correlation coefficient. For agreement, the standard error of measurement and smallest detectable changes were calculated. Construct validity was assessed by testing hypotheses regarding Spearman rank correlation coefficient. Area under the curve obtained from the receiver operating characteristic curve and minimal clinically important change were determined for the total sample and work ability score baseline tertile groups to assess responsiveness. Results In total, 34 workers were analyzed for reliability and agreement, 1291 workers for construct validity, and 590 responded to the responsiveness questionnaire. Reliability reached an intraclass correlation coefficient of 0.89; 95% CI 0.77-0.94, a standard error of measurement of 0.69 points, and the smallest detectable change of 1.92 points. For construct validity, six of the seven predefined hypotheses were not refuted. The area under the curve was 0.76 (95% CI 0.71-0.81) allowing for discrimination between stable and improved workers, with a minimal clinically important change of 2.0 points for the total sample. Conclusion The work ability score showed good measurement properties among sick-listed workers with chronic musculoskeletal pain.


Asunto(s)
Dolor Crónico , Dolor Musculoesquelético , Evaluación de la Discapacidad , Humanos , Dolor Musculoesquelético/rehabilitación , Reproducibilidad de los Resultados , Evaluación de Capacidad de Trabajo
7.
Osteoarthritis Cartilage ; 30(5): 671-680, 2022 05.
Artículo en Inglés | MEDLINE | ID: mdl-34883245

RESUMEN

OBJECTIVE: To compare computer-based 3D-analysis for quantification of the femorotibial joint space width (JSW) using weight-bearing cone beam CT (WB-CT), non-weight-bearing multi-detector CT (NWB-CT), and weight-bearing conventional radiographs (WB-XR). DESIGN: Twenty-six participants prospectively underwent NWB-CT, WB-CT, and WB-XR of the knee. For WB-CT and NWB-CT, the average and minimal JSW was quantified by 3D-analysis of the minimal distance of any point of the subchondral tibial bone surface and the femur. Associations with mechanical leg axes and osteoarthritis were evaluated. Minimal JSW of WB-CT was further compared to WB-XR. Two-tailed p-values of <0.05 were considered significant. RESULTS: Significant differences existed of the average medial and lateral JSW between WB-CT and NWB-CT (medial: 4.7 vs 5.1 mm [P = 0.028], lateral: 6.3 vs 6.8 mm [P = 0.008]). The minimal JSW on WB-XR (medial:3.1 mm, lateral:5.8 mm) were significantly wider compared to WB-CT and NWB-CT (both medial:1.8 mm, lateral:2.9 mm, all p < 0.001), but not significantly different between WB-CT and NWB-CT (all p ≥ 0.869). Significant differences between WB-CT and NWB-CT existed in participants with varus knee alignment for the average and the minimal medial JSW (p = 0.004 and p = 0.011) and for participants with valgus alignment for the average lateral JSW (p = 0.013). On WB-CT, 25% of the femorotibial compartments showed bone-on-bone apposition, which was significantly higher when compared to NWB-CT (10%,P = 0.008) and WB-XR (8%,P = 0.012). CONCLUSION: Combining WB-CT with 3D-based assessment allows detailed quantification of the femorotibial joint space and the effect of knee alignment on JSW. WB-CT demonstrates significantly more bone-on-bone appositions, which are underestimated or even undetectable on NWB-CT and WB-XR.


Asunto(s)
Articulación de la Rodilla , Osteoartritis de la Rodilla , Tomografía Computarizada de Haz Cónico , Humanos , Rodilla , Articulación de la Rodilla/diagnóstico por imagen , Osteoartritis de la Rodilla/diagnóstico por imagen , Radiografía , Soporte de Peso
8.
J Environ Radioact ; 237: 106715, 2021 Oct.
Artículo en Inglés | MEDLINE | ID: mdl-34371240

RESUMEN

Measurement of radioactive gas seepage from an underground nuclear explosion is one of the primary methods to confirm whether an event was nuclear in nature. Radioactive noble gas indicators that are commonly targeted by such measurements (e.g. 133Xe, 37Ar) have half-lives of 35 days or less. Argon-39, an activation product similar to 37Ar, is produced by the interaction between neutrons and potassium in the surrounding geology and has a half-life of 269 years. Measurements taken at three sites near three historic underground nuclear test locations at the Nevada National Security Site have all shown highly elevated levels of 39Ar in soil gas decades after the test events. Elevated levels of 39Ar were also detected in atmospheric air collected near two of these sites, and outside the entrance of the one tunnel site. These measurements demonstrate that 39Ar has the potential to be a long-term signature of an underground nuclear event which can be reliably detected at the surface or in the shallow subsurface. This radionuclide detection of an underground nuclear event decades after the event takes place is in contrast to the commonly held assumption that detecting underground nuclear events via radionuclides at the surface needs to be done in a matter of months. Depending upon what further studies show about the robustness of this signature in a variety of geological settings, it may in fact be easy to detect underground nuclear events at the surface for a very long time post-detonation.


Asunto(s)
Monitoreo de Radiación , Argón/análisis , Explosiones , Radioisótopos/análisis
9.
Adv Mater ; 33(30): e2007885, 2021 Jul.
Artículo en Inglés | MEDLINE | ID: mdl-34110653

RESUMEN

The design and fabrication of lattice-strained platinum catalysts achieved by removing a soluble core from a platinum shell synthesized via atomic layer deposition, is reported. The remarkable catalytic performance for the oxygen reduction reaction (ORR), measured in both half-cell and full-cell configurations, is attributed to the observed lattice strain. By further optimizing the nanoparticle geometry and ionomer/carbon interactions, mass activity close to 0.8 A mgPt -1 @0.9 V iR-free is achievable in the membrane electrode assembly. Nevertheless, active catalysts with high ORR activity do not necessarily lead to high performance in the high-current-density (HCD) region. More attention shall be directed toward HCD performance for enabling high-power-density hydrogen fuel cells.

10.
J Colloid Interface Sci ; 601: 843-852, 2021 Nov.
Artículo en Inglés | MEDLINE | ID: mdl-34118775

RESUMEN

Seed-mediated methods are widely used in industrial or academic laboratories for the synthesis of nanoparticles of controlled shape and size. In the natural medium, precipitation of secondary minerals also often take place on seeds. In this context, we have devised a formalism which accounts for the competition between seed growth and nucleation and growth of secondary particles in an initially over-saturated aqueous solution. Based on the classical nucleation theory, it involves a size-dependent growth law which accounts for Ostwald ripening effects, unlike most water-rock interaction codes. We find that, in such closed system, seed growth and nucleation/growth of secondary particles are strongly coupled. In the multi-dimensional parameter space, regions where one or the other process prevails are well-separated by a rather abrupt transition. In general, the value of the initial seed total surface area is insufficient to fully orientate the synthesis. Relying on this approach, we propose an alternative interpretation of recent experimental results on amorphous silica nanoparticle synthesis. Besides fundamental understanding of the kinetics of precipitation, the interest of the present approach is to serve as a guideline to experimentalists or industrialists working in seed-mediated syntheses and warn on the undesired formation of secondary particles when monodispersed distributions of nano- or micro-particles are searched.


Asunto(s)
Nanopartículas , Dióxido de Silicio , Cinética , Agua
11.
J Environ Radioact ; 233: 106590, 2021 Jul.
Artículo en Inglés | MEDLINE | ID: mdl-33798811

RESUMEN

Radioisotopes of the noble gases xenon and argon can be important indicators of underground nuclear explosions. The Comprehensive Nuclear-Test-Ban Treaty (CTBT) includes monitoring capabilities to identify potential nuclear explosions conducted in violation of the CTBT. This monitoring currently focuses on measurement of the xenon isotopes 131mXe, 133Xe, 133mXe, and 135Xe. However, it is predicted that within 100 days of an underground nuclear explosion (UNE) 37Ar would be released to the atmosphere at higher concentrations than xenon and with a higher signal to background ratio, depending on the radioxenon background levels. Therefore, inclusion of 37Ar measurement capabilities at atmospheric International Monitoring System (IMS) stations may represent an improvement in the capability to detect a nuclear explosion. At an IMS station location, an understanding of the expected range of background 37Ar activity concentrations is critical to determining what levels would constitute an elevated concentration. This work describes our analysis of atmospheric samples for 37Ar to evaluate the range of background concentrations. Samples were collected at multiple locations withing the United States, with approximately half coming from a sampler co-located with an IMS xenon monitoring station (RN75). The range of 37Ar concentrations measured in atmospheric air samples was relatively narrow; for samples considered detectable, the minimum and maximum measured concentrations were 0.56 and 2.3 mBq/m3, respectively. Comparison of 37Ar and 133Xe concentrations measured at the IMS station indicated some correlation between the measured concentrations. The results presented here demonstrate the capability to detect background concentrations of 37Ar in atmospheric air and provide a basis for potential implementation of 37Ar monitoring at IMS stations.


Asunto(s)
Contaminantes Radiactivos del Aire , Monitoreo de Radiación , Contaminantes Radiactivos del Aire/análisis , Argón , Atmósfera , Radioisótopos , Radioisótopos de Xenón/análisis
12.
Knee Surg Sports Traumatol Arthrosc ; 29(6): 1760-1768, 2021 Jun.
Artículo en Inglés | MEDLINE | ID: mdl-32785758

RESUMEN

PURPOSE: The role of increased femoral antetorsion (femAT) as a contributor to patellofemoral (PF) osteoarthritis (OA) is unknown. The purpose of this study was to investigate whether increased femAT was associated with advanced cartilage degeneration in the lateral PF joint. METHODS: Patients who underwent complete radiographic workup for surgical intervention due to OA in any knee joint compartment were included. Cartilage morphology according to the International Cartilage Repair Society (ICRS) cartilage lesion classification system in the PF joint, femoral and tibial torsion, frontal leg axis, and tibial tuberosity-trochlear groove (TT-TG) distance were assessed. Increased femAT was defined as > 20° according to previous reports. RESULTS: A total of 144 patients were included. Ninety-seven patients had a femAT of < 20° and 45 of > 20°. A significant odds ratio (OR) was found for lateral retropatellar (OR 3.5; p = 0.02) ICRS grade 3 and 4 cartilage degeneration and increased femAT ≥ 20°. In the medial PF compartment, increased femAT had an inverse effect (OR 0.16; p = 0.01). No significant ORs were found for TT-TG distance, tibial torsion, or leg axis. The lateral retropatellar ICRS grade showed a linear correlation to increased femAT values. In valgus knees, isolated lateral PF OA had an even more pronounced correlation to increased femAT (p = 0.004). CONCLUSION: Increased femAT showed higher grades of lateral retropatellar cartilage degeneration, which was even more pronounced in valgus knees. LEVEL OF EVIDENCE: Cohort study: Level III.


Asunto(s)
Enfermedades de los Cartílagos/epidemiología , Fémur/patología , Genu Valgum/epidemiología , Osteoartritis de la Rodilla/epidemiología , Articulación Patelofemoral/patología , Adulto , Anciano , Anciano de 80 o más Años , Cartílago/patología , Estudios de Cohortes , Femenino , Humanos , Articulación de la Rodilla/patología , Modelos Logísticos , Masculino , Persona de Mediana Edad , Oportunidad Relativa , Tibia/patología
13.
Knee Surg Sports Traumatol Arthrosc ; 29(10): 3254-3261, 2021 Oct.
Artículo en Inglés | MEDLINE | ID: mdl-32607816

RESUMEN

PURPOSE: The purpose of the present study was to compare total (TKA) and unicondylar (UKA) knee arthroplasty for spontaneous osteonecrosis of the knee (SONK), and to investigate potential correlations to radiographic parameters. METHODS: All consecutive patients with a magnetic resonance imaging (MRI) proven SONK treated with either TKA or UKA between 2002 and 2018 were analysed. The primary outcomes were postoperative complications and failure rates. Functional assessment included Knee Society Score (KSS), WOMAC Score, and range of motion. A novel three-dimensional measurement method was established to determine the size of the osteonecrotic lesion. All outcome parameters were correlated to the size of the necrotic lesion using Spearman's rank correlation. RESULTS: The two treatment groups (34 TKAs, 37 UKAs) did not differ regarding age, body mass index, and ratio of the volume of the necrotic lesion to the volume of the femoral condyle (n.s.). At a mean follow-up of 6.6 years, patients with UKA had better functional outcomes compared to patients with a TKA (WOMAC Score 1.0 vs. 1.6, p = 0.04; KSS pain 86 vs. 83, n.s), with a similar complication rate. No correlation was found between necrotic lesion size and failure rate (n.s.). CONCLUSION: UKA is a valuable treatment option for SONK leading to good functional results and a low failure rate. In case of a surgeon's concern regarding implant anchorage, TKA represents an equivalent solution. The MR-tomographic size of the osteonecrotic lesions seems to have no influence on the results. LEVEL OF EVIDENCE: III.


Asunto(s)
Artroplastia de Reemplazo de Rodilla , Osteoartritis de la Rodilla , Osteonecrosis , Humanos , Articulación de la Rodilla/diagnóstico por imagen , Articulación de la Rodilla/cirugía , Osteoartritis de la Rodilla/cirugía , Osteonecrosis/cirugía , Resultado del Tratamiento
14.
J Environ Radioact ; 228: 106513, 2021 Mar.
Artículo en Inglés | MEDLINE | ID: mdl-33360017

RESUMEN

While radioisotopes of noble gases are known to be indicators of underground nuclear explosions (UNE), McIntyre et al. (2017) was the first to report the presence of 39Ar in shallow soil gas in association with a decades old UNE. While this finding hinted at the potential application of 39Ar to be used as an indicator of a UNE, doing so would also require an understanding of the natural concentrations of 39Ar present in soil gas. Without knowing the expected range and variability of naturally occurring concentrations of 39Ar, it is difficult to determine what measured concentrations would be indicative of an elevated concentration. This paper presents results from 16 soil gas samples and three atmospheric air samples collected from various locations across the western United States. Shallow soil gas samples were collected into self-contained underwater breathing apparatus (SCUBA) tanks using a custom-built soil gas sampling system and then processed and analyzed for 39Ar. The measured concentrations of 39Ar varied from atmospheric air concentrations to about 3.5 times atmospheric air concentrations (58 mBq/m3). The results presented here represent the first measurements of natural background 39Ar concentrations in shallow soil gas. This data will be necessary if 39Ar is to be used as an indicator of UNE.


Asunto(s)
Argón , Radiación de Fondo , Monitoreo de Radiación , Radioisótopos , Contaminantes Radiactivos del Suelo/análisis , Argón/análisis , Radioisótopos/análisis , Suelo
15.
Proc Natl Acad Sci U S A ; 117(49): 30934-30941, 2020 12 08.
Artículo en Inglés | MEDLINE | ID: mdl-33229543

RESUMEN

It was previously shown [J. K. Lee et al., Proc. Natl. Acad. Sci. U.S.A, 116, 19294-19298 (2019)] that hydrogen peroxide (H2O2) is spontaneously produced in micrometer-sized water droplets (microdroplets), which are generated by atomizing bulk water using nebulization without the application of an external electric field. Here we report that H2O2 is spontaneously produced in water microdroplets formed by dropwise condensation of water vapor on low-temperature substrates. Because peroxide formation is induced by a strong electric field formed at the water-air interface of microdroplets, no catalysts or external electrical bias, as well as precursor chemicals, are necessary. Time-course observations of the H2O2 production in condensate microdroplets showed that H2O2 was generated from microdroplets with sizes typically less than ∼10 µm. The spontaneous production of H2O2 was commonly observed on various different substrates, including silicon, plastic, glass, and metal. Studies with substrates with different surface conditions showed that the nucleation and the growth processes of condensate water microdroplets govern H2O2 generation. We also found that the H2O2 production yield strongly depends on environmental conditions, including relative humidity and substrate temperature. These results show that the production of H2O2 occurs in water microdroplets formed by not only atomizing bulk water but also condensing water vapor, suggesting that spontaneous water oxidation to form H2O2 from water microdroplets is a general phenomenon. These findings provide innovative opportunities for green chemistry at heterogeneous interfaces, self-cleaning of surfaces, and safe and effective disinfection. They also may have important implications for prebiotic chemistry.

16.
ACS Appl Mater Interfaces ; 12(40): 44912-44918, 2020 Oct 07.
Artículo en Inglés | MEDLINE | ID: mdl-32915545

RESUMEN

The ability to control the properties of dielectric thin films on demand is of fundamental interest in nanoscale devices. Here, we modulate plasma characteristics at the surface of a substrate to tune both dielectric constant and thermal conductivity of amorphous thin films grown using plasma-enhanced atomic layer deposition. Specifically, we apply a substrate bias ranging from 0 to ∼117 V and demonstrate the systematic tunability of various material parameters of Al2O3. As a function of the substrate bias, we find a nonmonotonical evolution of intrinsic properties, including density, dielectric constant, and thermal conductivity. A key observation is that the maximum values in dielectric constant and effective thermal conductivity emerge at different substrate biases. The impact of density on both thermal conductivity and dielectric constant is further examined using a differential effective medium theory and the Clausius-Mossotti model, respectively. We find that the peak value in the dielectric constant deviates from the Clausius-Mossotti model, indicating the change of oxygen fraction in our thin films as a function of substrate bias. This finding suggests that the increased local strength of plasma sheath not only enhances material density but also controls the dynamics of microstructural defect formation beyond what is possible with conventional approaches. Based on our experimental observations and modeling, we further build a phenomenological relation between dielectric constant and thermal conductivity. Our results pave invaluable avenues for optimizing dielectric thin films at the atomic scale for a wide range of applications in nanoelectronics and energy devices.

17.
Phys Rev Lett ; 124(7): 076403, 2020 Feb 21.
Artículo en Inglés | MEDLINE | ID: mdl-32142316

RESUMEN

Exploration of the novel relationship between magnetic order and topological semimetals has received enormous interest in a wide range of both fundamental and applied research. Here we predict that "soft" ferromagnetic material EuB_{6} can achieve multiple topological semimetal phases by simply tuning the direction of the magnetic moment. Explicitly, EuB_{6} is a topological nodal-line semimetal when the moment is aligned along the [001] direction, and it evolves into a Weyl semimetal with three pairs of Weyl points by rotating the moment to the [111] direction. Interestingly, we identify a composite semimetal phase featuring the coexistence of a nodal line and Weyl points with the moment in the [110] direction. Topological surface states and anomalous Hall conductivity, which are sensitive to the magnetic order, have been computed and are expected to be experimentally observable. Large-Chern-number quantum anomalous Hall effect can be realized in its [111]-oriented quantum-well structures.

18.
ACS Appl Mater Interfaces ; 11(44): 41338-41346, 2019 Nov 06.
Artículo en Inglés | MEDLINE | ID: mdl-31603644

RESUMEN

In this Research Article, gadolinia-doped ceria (GDC), which is a highly catalyzed oxide ionic conductor, was explored to further improve oxygen surface reaction rates using a grain-controlled layer (GCL) concept. Typically, GDC materials have been used as a cathode functional layer by coating the GDC between the electrode and electrolyte to accelerate the oxygen reduction reaction (ORR). To further improve the oxygen surface kinetics of the GDC cathodic layer, we modified the grain boundary density and crystallinity developed in the GDC layer by adjusting RF power conditions during the sputtering process. This approach revealed that engineered nanograins of GDC thin films directly affected ORR kinetics by catalyzing the oxygen surface reaction rate, significantly enhancing the fuel cell performance. Using this innovative concept, the fuel cells fabricated with a GDC GCL demonstrated a peak power density of 240 mW/cm2 at 450 °C.

19.
J Environ Radioact ; 208-209: 106047, 2019 Nov.
Artículo en Inglés | MEDLINE | ID: mdl-31526956

RESUMEN

As part of an underground gas migration study, two radioactive noble gases (37Ar and 127Xe) and two stable tracer gases (SF6 and PFDMCH) were injected into a historic nuclear explosion test chimney and allowed to migrate naturally. The purpose of this experiment was to provide a bounding case (natural transport) for the flow of radioactive noble gases following an underground nuclear explosion. To accomplish this, soil gas samples were collected from a series of boreholes and a range of depths from the shallow subsurface (3 m) to deeper levels (~160 m) over a period of eleven months. These samples have provided insights into the development and evolution of the subsurface plume and constrained the relative migration rates of the radioactive and stable gas species in the case when the driving pressure from the cavity is low. Analysis of the samples concluded that the stable tracer SF6 was consistently enriched in the subsurface samples relative to the radiotracer 127Xe, but the ratios of SF6 and 37Ar remained similar throughout the samples.


Asunto(s)
Gases Nobles/análisis , Armas Nucleares , Monitoreo de Radiación , Radiactividad , Explosiones , Nevada , Medidas de Seguridad
20.
Proc Natl Acad Sci U S A ; 116(39): 19294-19298, 2019 09 24.
Artículo en Inglés | MEDLINE | ID: mdl-31451646

RESUMEN

We show H2O2 is spontaneously produced from pure water by atomizing bulk water into microdroplets (1 µm to 20 µm in diameter). Production of H2O2, as assayed by H2O2-sensitve fluorescence dye peroxyfluor-1, increased with decreasing microdroplet size. Cleavage of 4-carboxyphenylboronic acid and conversion of phenylboronic acid to phenols in microdroplets further confirmed the generation of H2O2 The generated H2O2 concentration was ∼30 µM (∼1 part per million) as determined by titration with potassium titanium oxalate. Changing the spray gas to O2 or bubbling O2 decreased the yield of H2O2 in microdroplets, indicating that pure water microdroplets directly generate H2O2 without help from O2 either in air surrounding the droplet or dissolved in water. We consider various possible mechanisms for H2O2 formation and report a number of different experiments exploring this issue. We suggest that hydroxyl radical (OH) recombination is the most likely source, in which OH is generated by loss of an electron from OH- at or near the surface of the water microdroplet. This catalyst-free and voltage-free H2O2 production method provides innovative opportunities for green production of hydrogen peroxide.

SELECCIÓN DE REFERENCIAS
DETALLE DE LA BÚSQUEDA
...