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1.
Proc Natl Acad Sci U S A ; 115(37): 9122-9127, 2018 09 11.
Artículo en Inglés | MEDLINE | ID: mdl-30154167

RESUMEN

Nucleation and growth of aerosol particles from atmospheric vapors constitutes a major source of global cloud condensation nuclei (CCN). The fraction of newly formed particles that reaches CCN sizes is highly sensitive to particle growth rates, especially for particle sizes <10 nm, where coagulation losses to larger aerosol particles are greatest. Recent results show that some oxidation products from biogenic volatile organic compounds are major contributors to particle formation and initial growth. However, whether oxidized organics contribute to particle growth over the broad span of tropospheric temperatures remains an open question, and quantitative mass balance for organic growth has yet to be demonstrated at any temperature. Here, in experiments performed under atmospheric conditions in the Cosmics Leaving Outdoor Droplets (CLOUD) chamber at the European Organization for Nuclear Research (CERN), we show that rapid growth of organic particles occurs over the range from [Formula: see text]C to [Formula: see text]C. The lower extent of autoxidation at reduced temperatures is compensated by the decreased volatility of all oxidized molecules. This is confirmed by particle-phase composition measurements, showing enhanced uptake of relatively less oxygenated products at cold temperatures. We can reproduce the measured growth rates using an aerosol growth model based entirely on the experimentally measured gas-phase spectra of oxidized organic molecules obtained from two complementary mass spectrometers. We show that the growth rates are sensitive to particle curvature, explaining widespread atmospheric observations that particle growth rates increase in the single-digit-nanometer size range. Our results demonstrate that organic vapors can contribute to particle growth over a wide range of tropospheric temperatures from molecular cluster sizes onward.

2.
Nat Commun ; 14(1): 3347, 2023 Jun 08.
Artículo en Inglés | MEDLINE | ID: mdl-37291087

RESUMEN

The interaction between nitrogen monoxide (NO) and organic peroxy radicals (RO2) greatly impacts the formation of highly oxygenated organic molecules (HOM), the key precursors of secondary organic aerosols. It has been thought that HOM production can be significantly suppressed by NO even at low concentrations. Here, we perform dedicated experiments focusing on HOM formation from monoterpenes at low NO concentrations (0 - 82 pptv). We demonstrate that such low NO can enhance HOM production by modulating the RO2 loss and favoring the formation of alkoxy radicals that can continue to autoxidize through isomerization. These insights suggest that HOM yields from typical boreal forest emissions can vary between 2.5%-6.5%, and HOM formation will not be completely inhibited even at high NO concentrations. Our findings challenge the notion that NO monotonically reduces HOM yields by extending the knowledge of RO2-NO interactions to the low-NO regime. This represents a major advance towards an accurate assessment of HOM budgets, especially in low-NO environments, which prevails in the pre-industrial atmosphere, pristine areas, and the upper boundary layer.


Asunto(s)
Atmósfera , Óxido Nítrico , Monoterpenos , Oxidación-Reducción , Aerosoles
3.
Materials (Basel) ; 14(21)2021 Oct 25.
Artículo en Inglés | MEDLINE | ID: mdl-34771925

RESUMEN

In this study, several biodegradable Mg alloys (Mg5Zn, Mg5Zn0.3Ca, Mg5Zn0.15Ca, and Mg5Zn0.15Ca0.15Zr, numbers in wt%) were investigated after thermomechanical processing via high-pressure torsion (HPT) at elevated temperature as well as after additional heat treatments. Indirect and direct analyses of microstructure revealed that the significant strength increases arise not only from dislocations and precipitates but also from vacancy agglomerates. By contrast with former low-temperature processing routes applied by the authors, a significant ductility was obtained because of temperature-induced dynamic recovery. The low initial values of Young's modulus were not significantly affected by warm HPT-processing. nor by heat treatments afterwards. Also, corrosion resistance did not change or even increase during those treatments. Altogether, the study reveals a viable processing route for the optimization of Mg alloys to provide enhanced mechanical properties while leaving the corrosion properties unaffected, suggesting it for the use as biodegradable implant material.

4.
Materials (Basel) ; 13(7)2020 Apr 08.
Artículo en Inglés | MEDLINE | ID: mdl-32276432

RESUMEN

Two binary biodegradable Mg-alloys and one ternary biodegradable Mg-alloy (Mg-0.3Ca, Mg-5Zn and Mg-5Zn-0.3Ca, all in wt%) were investigated. Surface-sensitive X-ray photoelectron spectroscopy analyses (XPS) of the alloy surfaces before and after immersion in simulated body fluid (SBF) were performed. The XPS analysis of the samples before the immersion in SBF revealed that the top layer of the alloy might have a non-homogeneous composition relative to the bulk. Degradation during the SBF immersion testing was monitored by measuring the evolution of H2. It was possible to evaluate the thickness of the sample degradation layers after the SBF immersion based on scanning electron microscopy (SEM) of the tilted sample. The thickness was in the order of 10-100 µm. The typical bio-corrosion products of all of the investigated alloys consisted of Mg, Ca, P and O, which suggests the formation of apatite (calcium phosphate hydroxide), magnesium hydrogen phosphate hydrate and magnesium hydroxide. The bioapplicability of the analyzed alloys with regard to surface composition and degradation kinetics is discussed.

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