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1.
Nat Commun ; 14(1): 1789, 2023 Mar 30.
Artículo en Inglés | MEDLINE | ID: mdl-36997508

RESUMEN

Most future projections conducted with coupled general circulation models simulate a non-uniform Indian Ocean warming, with warming hotspots occurring in the Arabian Sea (AS) and the southeastern Indian Ocean (SEIO). But little is known about the underlying physical drivers. Here, we are using a suite of large ensemble simulations of the Community Earth System Model 2 to elucidate the causes of non-uniform Indian Ocean warming. Strong negative air-sea interactions in the Eastern Indian Ocean are responsible for a future weakening of the zonal sea surface temperature gradient, resulting in a slowdown of the Indian Ocean Walker circulation and the generation of southeasterly wind anomalies over the AS. These contribute to anomalous northward ocean heat transport, reduced evaporative cooling, a weakening in upper ocean vertical mixing and an enhanced AS future warming. In contrast, the projected warming in the SEIO is related to a reduction of low-cloud cover and an associated increase in shortwave radiation. Therefore, the regional character of air-sea interactions plays a key role in promoting future large-scale tropical atmospheric circulation anomalies with implications for society and ecosystems far outside the Indian Ocean realm.

2.
Diagnostics (Basel) ; 12(12)2022 Nov 25.
Artículo en Inglés | MEDLINE | ID: mdl-36552963

RESUMEN

The histopathological findings of the glomeruli from whole slide images (WSIs) of a renal biopsy play an important role in diagnosing and grading kidney disease. This study aimed to develop an automated computational pipeline to detect glomeruli and to segment the histopathological regions inside of the glomerulus in a WSI. In order to assess the significance of this pipeline, we conducted a multivariate regression analysis to determine whether the quantified regions were associated with the prognosis of kidney function in 46 cases of immunoglobulin A nephropathy (IgAN). The developed pipelines showed a mean intersection over union (IoU) of 0.670 and 0.693 for five classes (i.e., background, Bowman's space, glomerular tuft, crescentic, and sclerotic regions) against the WSI of its facility, and 0.678 and 0.609 against the WSI of the external facility. The multivariate analysis revealed that the predicted sclerotic regions, even those that were predicted by the external model, had a significant negative impact on the slope of the estimated glomerular filtration rate after biopsy. This is the first study to demonstrate that the quantified sclerotic regions that are predicted by an automated computational pipeline for the segmentation of the histopathological glomerular components on WSIs impact the prognosis of kidney function in patients with IgAN.

3.
Sci Adv ; 8(51): eadd2475, 2022 Dec 21.
Artículo en Inglés | MEDLINE | ID: mdl-36542698

RESUMEN

Annually, marine phytoplankton convert approximately 50 billion tons of dissolved inorganic carbon to particulate and dissolved organic carbon, a portion of which is exported to depth via the biological carbon pump. Despite its important roles in regulating atmospheric carbon dioxide via carbon sequestration and in sustaining marine ecosystems, model-projected future changes in marine net primary production are highly uncertain even in the sign of the change. Here, using an Earth system model, we show that frugal utilization of phosphorus by phytoplankton under phosphate-stressed conditions can overcompensate the previously projected 21st century declines due to ocean warming and enhanced stratification. Our results, which are supported by observations from the Hawaii Ocean Time-series program, suggest that nutrient uptake plasticity in the subtropical ocean plays a key role in sustaining phytoplankton productivity and carbon export production in a warmer world.

4.
Nat Commun ; 13(1): 5798, 2022 10 02.
Artículo en Inglés | MEDLINE | ID: mdl-36184681

RESUMEN

Seasonal ice in lakes plays an important role for local communities and lake ecosystems. Here we use Large Ensemble simulations conducted with the Community Earth System Model version 2, which includes a lake simulator, to quantify the response of lake ice to greenhouse warming and to determine emergence patterns of anthropogenic lake ice loss. Our model simulations show that the average duration of ice coverage and maximum ice thickness are projected to decrease over the next 80 years by 38 days and 0.23 m, respectively. In the Canadian Arctic, lake ice loss is accelerated by the cold-season polar amplification. Lake ice on the Tibetan Plateau decreases rapidly due to a combination of strong insolation forcing and ice-albedo feedbacks. Comparing the anthropogenic signal with natural variability represented by the Large Ensemble, we find that lake ecosystems in these regions may be exposed to no-analogue ice coverage within the next 4-5 decades.


Asunto(s)
Cambio Climático , Lagos , Canadá , Ecosistema , Cubierta de Hielo
5.
Proc Natl Acad Sci U S A ; 119(30): e2202393119, 2022 07 26.
Artículo en Inglés | MEDLINE | ID: mdl-35858427

RESUMEN

Climate change projections consistently demonstrate that warming temperatures and dwindling seasonal snowpack will elicit cascading effects on ecosystem function and water resource availability. Despite this consensus, little is known about potential changes in the variability of ecohydrological conditions, which is also required to inform climate change adaptation and mitigation strategies. Considering potential changes in ecohydrological variability is critical to evaluating the emergence of trends, assessing the likelihood of extreme events such as floods and droughts, and identifying when tipping points may be reached that fundamentally alter ecohydrological function. Using a single-model Large Ensemble with sophisticated terrestrial ecosystem representation, we characterize projected changes in the mean state and variability of ecohydrological processes in historically snow-dominated regions of the Northern Hemisphere. Widespread snowpack reductions, earlier snowmelt timing, longer growing seasons, drier soils, and increased fire risk are projected for this century under a high-emissions scenario. In addition to these changes in the mean state, increased variability in winter snowmelt will increase growing-season water deficits and increase the stochasticity of runoff. Thus, with warming, declining snowpack loses its dependable buffering capacity so that runoff quantity and timing more closely reflect the episodic characteristics of precipitation. This results in a declining predictability of annual runoff from maximum snow water equivalent, which has critical implications for ecosystem stress and water resource management. Our results suggest that there is a strong likelihood of pervasive alterations to ecohydrological function that may be expected with climate change.


Asunto(s)
Cambio Climático , Nieve , Ecosistema , Estaciones del Año , Agua
6.
Chem Commun (Camb) ; 57(49): 6019-6022, 2021 Jun 17.
Artículo en Inglés | MEDLINE | ID: mdl-34032240

RESUMEN

Pyridine-boryl (py-boryl) radicals serve as efficient electron-doping reagents for single-walled carbon nanotubes (SWCNTs). The doping mechanism comprises electron transfer from the py-boryl radical to the SWCNT. The formation of a stable py-boryl cation is essential for efficient doping; the captodative effect of the py-boryl cation is important to this process.

7.
Sci Technol Adv Mater ; 22(1): 272-279, 2021 Apr 13.
Artículo en Inglés | MEDLINE | ID: mdl-33907526

RESUMEN

The large anisotropic thermal conduction of a carbon nanotube (CNT) sheet that originates from the in-plane orientation of one-dimensional CNTs is disadvantageous for thermoelectric conversion using the Seebeck effect since the temperature gradient is difficult to maintain in the current flow direction. To control the orientation of the CNTs, polymer particles are introduced as orientation aligners upon sheet formation by vacuum filtration. The thermal conductivities in the in-plane direction decrease as the number of polymer particles in the sheet increases, while that in the through-plane direction increases. Consequently, a greater temperature gradient is observed for the anisotropy-controlled CNT sheet as compared to that detected for the CNT sheet without anisotropy control when a part of the sheet is heated, which results in a higher power density for the planar-type thermoelectric device. These findings are quite useful for the development of flexible and wearable thermoelectric batteries using CNT sheets.

8.
Kidney Int Rep ; 6(3): 716-726, 2021 Mar.
Artículo en Inglés | MEDLINE | ID: mdl-33732986

RESUMEN

INTRODUCTION: Diagnosing renal pathologies is important for performing treatments. However, classifying every glomerulus is difficult for clinicians; thus, a support system, such as a computer, is required. This paper describes the automatic classification of glomerular images using a convolutional neural network (CNN). METHOD: To generate appropriate labeled data, annotation criteria including 12 features (e.g., "fibrous crescent") were defined. The concordance among 5 clinicians was evaluated for 100 images using the kappa (κ) coefficient for each feature. Using the annotation criteria, 1 clinician annotated 10,102 images. We trained the CNNs to classify the features with an average κ ≥0.4 and evaluated their performance using the receiver operating characteristic-area under the curve (ROC-AUC). An error analysis was conducted and the gradient-weighted class activation mapping (Grad-CAM) was also applied; it expresses the CNN's focusing point with a heat map when the CNN classifies the glomerular image for a feature. RESULTS: The average κ coefficient of the features ranged from 0.28 to 0.50. The ROC-AUC of the CNNs for test data varied from 0.65 to 0.98. Among the features, "capillary collapse" and "fibrous crescent" had high ROC-AUC values of 0.98 and 0.91, respectively. The error analysis and the Grad-CAM visually showed that the CNN could not distinguish between 2 different features that had similar visual structures or that occurred simultaneously. CONCLUSION: The differences in the texture or frequency of the co-occurrence between the different features affected the CNN performance; thus, to improve the classification accuracy, methods such as segmentation are required.

9.
Sci Adv ; 6(51)2020 Dec.
Artículo en Inglés | MEDLINE | ID: mdl-33328238

RESUMEN

Tropical cyclones (TCs) are extreme storms that form over warm tropical oceans. Along their tracks, TCs mix up cold water, which can further affect their intensity. Because of the adoption of lower-resolution ocean models, previous modeling studies on the TC response to greenhouse warming underestimated such oceanic feedbacks. To address the robustness of TC projections in the presence of mesoscale air-sea interactions and complex coastal topography, we conduct greenhouse warming experiments using an ultrahigh-resolution Earth System Model. We find that a projected weakening of the rising branches of the summer Hadley cells suppresses future TC genesis and TC-generated ocean cooling. The forced response is similar to recent observational trends, indicating a possible emergence of the anthropogenic signal beyond natural variability levels. In the greenhouse warming simulations, landfalling TCs intensify, both in terms of wind speed and associated rainfall. Our modeling results provide relevant information for climate change adaptation efforts.

10.
Materials (Basel) ; 13(17)2020 Aug 28.
Artículo en Inglés | MEDLINE | ID: mdl-32872266

RESUMEN

Single-walled carbon nanotubes (SWCNTs) remain one of the most promising materials of our times. One of the goals is to implement semiconducting and metallic SWCNTs in photonics and microelectronics, respectively. In this work, we demonstrated how such materials could be obtained from the parent material by using the aqueous two-phase extraction method (ATPE) at a large scale. We also developed a dedicated process on how to harvest the SWCNTs from the polymer matrices used to form the biphasic system. The technique is beneficial as it isolates SWCNTs with high purity while simultaneously maintaining their surface intact. To validate the utility of the metallic and semiconducting SWCNTs obtained this way, we transformed them into thin free-standing films and characterized their thermoelectric properties.

11.
Angew Chem Int Ed Engl ; 54(31): 9057-60, 2015 Jul 27.
Artículo en Inglés | MEDLINE | ID: mdl-26083123

RESUMEN

An efficient catalytic system for the production of hydrogen from a methanol-water solution has been developed using a new anionic iridium complex bearing a functional bipyridonate ligand as a catalyst. This system can be operated under mild conditions [weakly basic solution (0.046 mol L(-1) NaOH) below 100 °C] without the use of an additional organic solvent. Long-term continuous hydrogen production from a methanol-water solution catalyzed by the anionic iridium complex was also achieved.


Asunto(s)
Hidrógeno/química , Iridio/química , Metanol/química , Catálisis , Ligandos , Estructura Molecular
12.
J Am Chem Soc ; 136(13): 4829-32, 2014 Apr 02.
Artículo en Inglés | MEDLINE | ID: mdl-24660903

RESUMEN

Homogeneous perdehydrogenation of saturated bicyclic 2,6-dimethyldecahydro-1,5-naphthyridine and perhydrogenation of aromatic 2,6-dimethyl-1,5-naphthyridine with release and uptake of five molecules of H2 are efficiently achieved by iridium complexes bearing a functional bipyridonate ligand. Successive perhydrogenation and perdehydrogenation of 2,6-dimethyl-1,5-naphthryridine using a single iridium complex also proceed with the reversible interconversion of the catalytic species, depending on the presence or absence of H2.

14.
J Org Chem ; 77(20): 9102-9, 2012 Oct 19.
Artículo en Inglés | MEDLINE | ID: mdl-23006061

RESUMEN

A simple and convenient CuI/2-pyridonate catalytic system for the oxidative amidation of aldehydes with secondary amines has been developed. With this system, a variety of useful arylamides have been synthesized in moderate to good yields in the presence of small amount of copper catalyst and the pyridonate ligand, generating only water as a coproduct. Synthesis of cinnamamides was also achieved by the reactions of cinnamaldehydes with secondary amines in moderate yields. Air was successfully employed as a green oxidant in this catalytic system, achieving a safe and atom-efficient system for the synthesis of amides.


Asunto(s)
Aldehídos/química , Amidas/síntesis química , Aminas/química , Cobre/química , Yoduros/química , Piridonas/química , Amidas/química , Catálisis , Estructura Molecular , Oxidación-Reducción
15.
J Am Chem Soc ; 134(8): 3643-6, 2012 Feb 29.
Artículo en Inglés | MEDLINE | ID: mdl-22339738

RESUMEN

A new catalytic system for the dehydrogenative oxidation of alcohols using a water-soluble Cp*Ir complex bearing a bipyridine-based functional ligand as catalyst has been developed. With this catalytic system, a variety of primary and secondary alcohols have been efficiently converted to aldehydes and ketones, respectively, in aqueous media without using any oxidant. Reuse of the catalyst by a very simple procedure has been also accomplished.


Asunto(s)
2,2'-Dipiridil/química , Alcoholes/química , Aldehídos/síntesis química , Iridio/química , Cetonas/síntesis química , Compuestos Organometálicos/química , Aldehídos/química , Catálisis , Cetonas/química , Ligandos , Estructura Molecular , Oxidación-Reducción , Solubilidad , Estereoisomerismo , Agua/química
16.
Chem Commun (Camb) ; 47(48): 12876-8, 2011 Dec 28.
Artículo en Inglés | MEDLINE | ID: mdl-22076830

RESUMEN

A highly efficient and convenient CuCl/2-pyridonate catalytic system for oxidative homocoupling of azoles affording a biazole product has been developed. With this system, a variety of biazoles have been effectively synthesized in good to excellent yields in the presence of a very small amount of copper catalyst (1.0 mol%). It was feasible to employ air as a green oxidant.


Asunto(s)
Azoles/química , Cobre/química , Piridonas/química , Aire , Azoles/síntesis química , Catálisis , Oxidación-Reducción
17.
Org Lett ; 13(9): 2278-81, 2011 May 06.
Artículo en Inglés | MEDLINE | ID: mdl-21473566

RESUMEN

A new catalytic system for the dehydrogenative oxidation of alcohols using a Cp*Ir complex having a functional C,N-chelate ligand has been developed. With this catalytic system, both primary and secondary alcohols were efficiently converted to aldehydes and ketones, respectively. Mechanistic investigations of this catalytic system have revealed that the catalytically active species is a hydrido iridium complex with a functional C,N-chelate ligand.

18.
J Am Chem Soc ; 132(43): 15108-11, 2010 Nov 03.
Artículo en Inglés | MEDLINE | ID: mdl-20931960

RESUMEN

Novel water-soluble Cp*Ir-ammine complexes have been synthesized, and a new and highly atom-economical system for the synthesis of organic amines using aqueous ammonia as a nitrogen source has been developed. With a water-soluble and air-stable Cp*Ir-ammine catalyst, [Cp*Ir(NH(3))(3)][I](2), a variety of tertiary and secondary amines were synthesized by the multialkylation of aqueous ammonia with theoretical equivalents of primary and secondary alcohols. The catalyst could be recycled by a facile procedure maintaining high activity. A one-flask synthesis of quinolizidine starting with 1,5,9-nonanetriol was also demonstrated. This new catalytic system would provide a practical and environmentally benign methodology for the synthesis of various organic amines.

19.
Org Lett ; 12(6): 1336-9, 2010 Mar 19.
Artículo en Inglés | MEDLINE | ID: mdl-20184342

RESUMEN

A simple and versatile catalytic system for N-alkylation of sulfonamides with various alcohols based on a catalytic hydrogen transfer reaction has been developed under a low catalyst loading of [Cp*IrCl(2)](2) (0.050-1.5 mol %) in the presence of t-BuOK. A variety of N-alkylated sulfonamides were prepared in good to excellent yields. Mechanistic investigations revealed that the key catalytic species in the present system is a sulfonylimido-bridged unsaturated diiridium complex [(Cp*Ir)(2)(mu-NTs)(2)].


Asunto(s)
Alcoholes/química , Iridio/química , Compuestos Organometálicos/química , Sulfonamidas/síntesis química , Alquilación , Catálisis , Ciclización , Estructura Molecular , Estereoisomerismo , Sulfonamidas/química
20.
J Am Chem Soc ; 131(24): 8410-2, 2009 Jun 24.
Artículo en Inglés | MEDLINE | ID: mdl-19480425

RESUMEN

The first homogeneous catalytic system for the efficient reversible dehydrogenation-hydrogenation reactions of nitrogen heterocycles in one flask has been developed using the pyridonate Cp*Ir complex as the single catalyst at relatively low temperature. The reversible catalytic reactions proceed with the reversible interconversion of catalytic species and can be nearly quantitatively repeated five times with almost no loss of efficiency. The remarkable feature of the present homogeneous catalytic system is that the reversible dehydrogenation-hydrogenation reactions proceed with the reversible interconversion of the catalytic species, depending on the absence or presence of hydrogen.

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