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Elemental carbon (EC), also known as black carbon, plays an important role in climate change. Accurately assessing EC concentration in aerosols remains challenging due to the overestimations caused by carbonates and organic carbon (OC) during thermal-optical measurement in the Tibetan Plateau (TP). This study evaluates the extent of EC overestimated by carbonates and OC at four remote sites (Nyalamu, Lulang, Everest and Ngari) in southern and western of the TP using different treatments. The average overestimation of EC concentration due to acid treatment was consistent across all sites (25.5 f 2.4 %). After correction, the proportion of EC overestimated by carbonates were approximately 8.5 f 7.3 %, 12.3 f 6.9 %, 18.1 f 11.8 % and 22.7 f 13.3 %, respectively, revealing an increasing trend from humid to arid regions. Methanol-soluble OC (MSOC) concentrations were significantly correlated with the reduction of EC concentrations, indicating that the methanol extraction effectively mitigates EC overestimation. Seasonal variation of carbonaceous aerosol concentrations was significantly affected by sources from South Asia. Despite the variations in climate and aerosol sources, the average overestimations of measured EC concentration by carbonates and OC were similar at Nyalamu (49.4 f 14.0 %), Lulang (47.8 f 8.4 %), Everest (48.7 f 15.9 %) and Ngari (49.3 f 13.7 %) sites. Therefore, the actual EC concentrations were only about 51.2 f 13.1 % of the original values. This estimation will significantly enhance the contribution of brown carbon (BrC) to radiative forcing relative to EC, highlighting a critical area for future research. Investigating the actual concentrations of EC in the TP provides critical data to support model simulation and validate model accuracy, further enhancing our understanding of EC's impacts on climate warming and glacier melting.

期刊论文 2024-12-15 DOI: 10.1016/j.envpol.2024.125277 ISSN: 0269-7491

The clumped and stable isotope (Delta(47), delta O-18, and delta C-13) composition of pedogenic (soil) carbonates from cold, arid environments may be a valuable paleoclimate archive for climate change-sensitive areas at high latitudes or elevations. However, previous work suggests that the isotopic composition of cold-climate soil carbonates is susceptible to kinetic isotope effects (KIE). To evaluate the conditions under which KIE occur in cold-climate soil carbonates, we examine the Delta(47), delta O-18, and delta C-13 composition of soil carbonate pendants from Antarctica (Dry Valleys, 77 degrees S), the High Arctic (Svalbard 79 degrees N), the Chilean and Argentinian Andes, and the Tibetan plateau (3800-4800 m), and compare the results to local climate and water delta O-18 records. At each site we calculate the expected equilibrium soil carbonate Delta(47) and delta O-18 values and estimate carbonate Delta(47) and delta O-18 anomalies (observed Delta(47) or delta O-18 minus the expected equilibrium Delta(47) or delta O-18). Additionally, we compare the measured carbonate delta C-13 to the expected range of equilibrium soil carbonate delta C-13 values. To provide context for interpreting the Delta(47) and delta O-18 anomalies, the soil carbonate results are compared to results for sub-glacial carbonates from two different sites, which exhibit large Delta(47) anomalies (up to -0.29 parts per thousand). The Antarctic and 4700 masl Chilean Andes samples have negative Delta(47) anomalies and positive delta O-18 anomalies consistent with KIE due to rapid bicarbonate dehydration during cryogenic carbonate formation. In contrast, the lower elevation Chilean Andes, Argentinian Andes, Tibetan Plateau and High Arctic results are consistent with equilibrium, summer carbonate formation. We attribute the differences in Delta(47) and delta O-18 anomalies to variations in inter-cobble matrix grain size and its effects on the effective soil pore space, permeability (hydraulic conductivity), moisture, and bicarbonate dehydration rate. The Antarctic and 4700 masl Chilean Andean soils have coarse-grained matrices that facilitate rapid bicarbonate dehydration. In contrast, the lower elevation Chilean Andes, Argentinian Andes, High Arctic and Tibetan Plateau soils have finer-grained matrices that decrease the soil pore space, soil permeability and CO2 gas flux, promoting equilibrium carbonate formation. The sub-glacial carbonate samples yield highly variable Delta(47) and delta O-18 anomalies, and we propose that the differences between the two glacier sites may be due to variations in local sub-glacial drainage conditions, pCO(2), and pH. Our findings suggest that carbonates from soils with coarse-grained matrices may exhibit KIE in cold climates, making them poor paleoclimate proxies. Soils with fine-grained matrices are more likely to yield equilibrium carbonates suitable for paleoclimate reconstructions regardless of climate. Paleosol matrix grain size should therefore be taken into account in the evaluation of carbonate stable and clumped isotope values in paleoclimate studies. (C) 2018 Elsevier Ltd. All rights reserved.

期刊论文 2018-08-15 DOI: 10.1016/j.gca.2018.06.006 ISSN: 0016-7037
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