Fossil and Nonfossil Sources of Organic and Elemental Carbon Aerosols in the Outflow from Northeast China

Source quantification of carbonaceous aerosols in the Chinese outflow regions still remains uncertain despite their high mass concentrations. Here, we unambiguously quantified fossil and nonfossil contributions to elemental carbon (EC) and organic carbon (OC) of total suspended particles (TSP) from a regional receptor site in the outflow of Northeast China using radiocarbon measurement. OC and EC concentrations were lower in summer, representing mainly marine air, than in other seasons, when air masses mostly traveled over continental regions in Mongolia and northeast China. The annual-mean contribution from fossil-fuel combustion to EC was 76 ± 11% (0.1−1.3 μg m−3). The remaining 24 ± 11% (0.03−0.42 μg m−3) was attributed to biomass burning, with slightly higher contribution in the cold period (∼31%) compared to the warm period (∼21%) because of enhanced emissions from regional biomass combustion sources in China. OC was generally dominated by nonfossil sources, with an annual average of 66 ± 11% (0.5−2.8 μg m−3), approximately half of which was apportioned to primary biomass burning sources (34 ± 6%). In winter, OC almost equally originated from primary OC (POC) emissions and secondary OC (SOC) formation from fossil fuel and biomass-burning sources. In contrast, summertime OC was dominated by primary biogenic emissions as well as secondary production from biogenic and biomass-burning sources, but fossil-derived SOC was the smallest contributor. Distinction of POC and SOC was performed using primary POC-to-EC emission ratios separated for fossil and nonfossil emissions.

Historic records of organic compounds from a high Alpine glacier: influences of biomass burning, anthropogenic emissions, and dust transport

Historic records of α-dicarbonyls (glyoxal, methylglyoxal), carboxylic acids (C6–C12 dicarboxylic acids, pinic acid, p-hydroxybenzoic acid, phthalic acid, 4-methylphthalic acid), and ions (oxalate, formate, calcium) were determined with annual resolution in an ice core from Grenzgletscher in the southern Swiss Alps, covering the time period from 1942 to 1993. Chemical analysis of the organic compounds was conducted using ultra-high-performance liquid chromatography (UHPLC) coupled to electrospray ionization high-resolution mass spectrometry (ESI-HRMS) for dicarbonyls and long-chain carboxylic acids and ion chromatography for short-chain carboxylates. Long-term records of the carboxylic acids and dicarbonyls, as well as their source apportionment, are reported for western Europe. This is the first study comprising long-term trends of dicarbonyls and long-chain dicarboxylic acids (C6–C12) in Alpine precipitation. Source assignment of the organic species present in the ice core was performed using principal component analysis. Our results suggest biomass burning, anthropogenic emissions, and transport of mineral dust to be the main parameters influencing the concentration of organic compounds. Ice core records of several highly correlated compounds (e.g., p-hydroxybenzoic acid, pinic acid, pimelic, and suberic acids) can be related to the forest fire history in southern Switzerland. P-hydroxybenzoic acid was found to be the best organic fire tracer in the study area, revealing the highest correlation with the burned area from fires. Historical records of methylglyoxal, phthalic acid, and dicarboxylic acids adipic acid, sebacic acid, and dodecanedioic acid are comparable with that of anthropogenic emissions of volatile organic compounds (VOCs). The small organic acids, oxalic acid and formic acid, are both highly correlated with calcium, suggesting their records to be affected by changing mineral dust transport to the drilling site.

(Table 1) Carbon and isotopic composition of organic carbon in sediments from DSDP Leg 56 Holes

We have analyzed inorganic and organic carbons and determined the isotopic composition of both sedimentary organic carbon and inorganic carbon in carbonates contained in sediments recovered from Holes 434, 434A, 434B, 435, and 435A in the landward slope of Japan and from Hole 436 in the oceanic slope of the Japan Trench. Both inorganic and organic carbons were assayed at the P. P. Shirshov Institute of Oceanology, in the same sample, using the Knopp technique and measuring evolved CO2 gravimetrically. Each sample was analyzed twice in parallel. Measurements were of a ±0.05 per cent accuracy and a probability level of 0.95. Carbon isotopic analysis was carried out on a MI-1305 mass spectrometer at the I. M. Gubkin Institute of Petrochemical and Gas Industry and the results presented as dC13 values related to the PDB standard. The procedure for preparing samples for organic carbon isotopic analysis involved (1) drying damp sediments at 60°C; (2) treating samples, while heating, with 10 N HCl to remove carbonate carbon; and (3) evaporating surplus HCl at 60°C. The organic substance was turned to CO2 by oxidizing it in an oxygen atmosphere. To prepare samples for inorganic carbon isotopic analysis we decomposed the carbonates with orthophosphoric acid and refined the gas evolved. The dC13 measurements, including a full cycle of sample preparation, were of a ±0.5 per cent accuracy and a probability level of 0.95.

(Tables 1, 3) Component composition of organic particles in samples from ODP Site 131-808

Analysis of the palynofacies and miospore thermal alteration indices (TAI) of sediments from ODP Site 808 in the Nankai Trough was undertaken to determine (1) the source, depositional environment, and diagenesis of organic matter in the accreted sediments, and (2) the thermal structure and history of the prism and its relationship to fluid flow. Using the Hartax classification system, two palynofacies were recognized in the sedimentary sequence. Facies 1 occurs within the upper 600 m of trench-wedge turbidites (sedimentation rate > 1 km/m.y.) and contains >50% inertite particles. The rest of the assemblage is dominated by well-preserved phytoclasts and contains small amounts of poorly preserved phytoclasts and well-preserved scleratoclasts. Facies 2 occurs within the Shikoku Basin hemipelagites (600-1300 m below seafloor; sedimentation rate <150 m/m.y.) and contains over two-thirds inertite particles. The rest of the assemblage is dominated by poorly preserved phytoclasts. Miospores and marine phytoplankton compose only a small percentage of both palynofacies. Degraded organic matter is most noticeable in Facies 2, whereas its presence in Facies 1 is overshadowed by the high influx of well-preserved primary organic matter. Most of the degraded organic matter and inertite is interpreted to be reworked. Some of the degraded organic matter may be primary, and may have experienced more biodegradation and thermal alteration in Facies 2 than in Facies 1. TAI values indicate an immature stage of organic maturation (< 2) down to about 900 mbsf. Below this, samples show an increase with depth to a mature stage, reaching peak levels of about 3 just above basement. Samples from within the thrust fault and decollement zones do not show levels of maturity significantly greater than those of surrounding samples, leaving uncertain whether hot fluids have migrated along these fault boundaries in the past.