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2.
Proc Natl Acad Sci U S A ; 120(47): e2217064120, 2023 Nov 21.
Artigo em Inglês | MEDLINE | ID: mdl-38033310

RESUMO

The intertropical convergence zone (ITCZ) plays a key role in regulating tropical hydroclimate and global water cycle through changes in its convection strength, latitudinal position, and width. The long-term variability of the ITCZ, along with the corresponding driving mechanisms, however, remains obscure, mainly because it is difficult to separate different ITCZ variables in paleoclimate proxy records. Here, we report a speleothem oxygen isotope (δ18O) record from southwestern Sulawesi, Indonesia, and compile it with other speleothem records from the Maritime Continent. Using the spatial gradient of speleothem δ18O along a transect across the ITCZ, we constrain ITCZ variabilities over the Maritime Continent during the past 30,000 y. We find that ITCZ convection strength overall intensified from the last glacial period to the Holocene, following changes in climate boundary conditions. The mean position of the regional ITCZ has moved latitudinally no more than 3° in the past 30,000 y, consistent with the deduction from the atmospheric energy framework. However, different from modern observations and model simulations for future warming, the ITCZ appeared narrower during both the late Holocene and most part of the last glacial period, and its expansion occurred during Heinrich stadials and the early-to-mid Holocene. We also find that during the last glacial and deglacial period, prominent millennial-scale ITCZ changes were closely tied to the variability of the Atlantic meridional overturning circulation (AMOC), whereas during the Holocene, they were predominantly modulated by the long-term variability of the Walker circulation.

3.
Chemosphere ; 241: 125024, 2020 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-31604191

RESUMO

Emission of reactive nitrogen species has a major impact on atmospheric chemistry, ecosystem and human health. The origin and formation mechanisms of wet-deposited nitrate are not well understood in Southeast Asia (SEA). In this study, we measured stable isotopes of nitrate (δ15N and δ18O) and chemical compositions of daily rainwater from May 2015 to July 2017 in Singapore. Our results showed that δ15N-NO3- and δ18O-NO3- varied seasonally with higher values during the Inter-monsoon period (April-May and October-November) than during Northeast (December-March) and Southwest monsoon (June-September). Bayesian mixing modeling, which took account of the isotope fractionation, indicated that traffic emission (47 ±â€¯32%) and lightning (19 ±â€¯20%) contributed the most to NO3- with increased traffic contribution (55 ±â€¯37%) in the Northeast monsoon and lightning (24 ±â€¯23%) during the Inter-monsoon period. Biomass burning and coal combustion, likely from transboundary transport, contributed ∼25% of nitrate in the rainwater. Monte Carlo simulation of δ18O-NO3- indicated that oxidation process by hydroxyl radical contributed 65 ±â€¯14% of NO3-, with the rest from hydrolysis of N2O5. Wind speed had large effect on δ18O-NO3- variations in the atmosphere with more involvement of hydroxyl radical reactions when wind speed increased. Our study highlights the key role of isotopic fractionation in nitrate source apportionment, and the influence of meteorological conditions on nitrate formation processes in SEA.


Assuntos
Monitoramento Ambiental/métodos , Nitratos/análise , Isótopos de Nitrogênio/análise , Isótopos de Oxigênio/análise , Chuva/química , Ecossistema , Conceitos Meteorológicos , Óxidos de Nitrogênio , Singapura , Poluentes Químicos da Água/análise , Poluentes Radioativos da Água/análise
4.
Rapid Commun Mass Spectrom ; 28(1): 96-108, 2014 Jan 15.
Artigo em Inglês | MEDLINE | ID: mdl-24285394

RESUMO

RATIONALE: Compound-specific stable isotope analysis of amino acids has proven informative to many ecological systems, but only a handful of analytical methods are routinely employed. We evaluated a simple, rapid procedure in which biological samples undergo short-duration acid hydrolysis and the resulting amino acids are derivatized with methyl chloroformate for gas chromatography/combustion/isotope-ratio mass spectrometry (GC/C/IRMS). METHODS: Amino acid derivatives were separated on a polar gas chromatography column, combusted, and δ(13)C and δ(15)N values were measured. Tests of reproducibility and accuracy were conducted for amino acid reference mixtures and biological samples. A brief case study of turtles was used to assess whether isotopic data were consistent with a priori ecological expectations. RESULTS: The methyl chloroformate based reaction successfully converted 15 amino acids from acid hydrolysates of biological materials into separable derivatives. The δ(13)C and δ(15)N values had high average measurement precision (σ <1‰). Reference materials were measured accurately, with good agreement between EA/IRMS and GC/C/IRMS determinations. Analysis of turtle blood samples yielded data consistent with their trophic ecology. CONCLUSIONS: This derivatization method is a rapid means of determining carbon and nitrogen isotopic ratios of amino acids present in the biological materials often sampled for ecological studies. While amino acids with charged or polar side chains do not have uniformly high recoveries, the average precision of measurements is comparable with that of other, more established methods. Batches of samples may be prepared from many raw materials in less than a day, representing a significant reduction in preparation time over prevailing methods.


Assuntos
Aminoácidos/análise , Aminoácidos/química , Formiatos/química , Cromatografia Gasosa-Espectrometria de Massas/métodos , Hidrobiologia/métodos , Animais , Isótopos de Carbono/análise , Galinhas , Isótopos de Nitrogênio/análise , Porphyra , Reprodutibilidade dos Testes , Tartarugas , Baleias
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