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Aerosol black carbon (BC) is a short-lived climate pollutant. The poorly constrained provenance of tropical marine aerosol BC hinders the mechanistic understanding of extreme climate events and oceanic carbon cycling. Here, we collected PM 2.5 samples during research cruise NORC2016-10 through South China Sea (SCS) and Northeast Indian Ocean (NEIO) and measured the dual-carbon isotope compositions (δ 13 C- Δ 14 C) of BC using hydrogen pyrolysis technique. Aerosol BC exhibits six different δ 13 C- Δ 14 C isotopic spaces (i.e., isotope provinces). Liquid fossil fuel combustion, from shipping emissions and adjacent land, is the predominant source of BC over isotope provinces "SCS close to Chinese Mainland" (53.5%), "Malacca Strait" (53.4%), and "Open NEIO" (40.7%). C 3 biomass burning is the major contributor to BC over isotope provinces "NEIO close to Southeast Asia" (55.8%), "Open NEIO" (41.3%), and "Open SCS" (40.0%). Coal combustion and C 4 biomass burning show higher contributions to BC over "Sunda Strait" and "Open SCS" than the others. Overall, NEIO near the Bay of Bengal, Malacca Strait, and north SCS are three hot spots of fossil fuel-derived BC; the first two areas are also hot spots of biomass-derived BC. The comparable δ 13 C- Δ 14 C between BC in aerosol and dissolved BC in surface seawater may suggest atmospheric BC deposition as a potential source of oceanic dissolved BC.

Biomass burning (BB) is an important source of atmospheric persistent organic pollutants (POPs) across the world. However, there are few field-based regional studies regarding the POPs released from BB. Due to the current limitations of emission factors and satellites, the contribution of BB to airborne POPs is still not well understood. In this study, with the simultaneous monitoring of BB biomarkers and POPs based on polyurethane foam-based passive air sampling technique, we mapped the contribution of BB to polychlorinated biphenyls (PCBs) and organochlorine pesticides (OCPs) in the Indo-China Peninsula. Spearman correlations between levoglucosan and 16 PCBs ( r s = 0.264-0.767, p < 0.05) and 2 OCPs ( r s = 0.250-0.328, p < 0.05) confirmed that BB may facilitate POP emissions. Source apportionment indicated that BB contributed 9.3% to the total PCB and OCP mass. The high contribution of positive matrix factorization-resolved BB to PCBs and OCPs was almost consistent with their concentration distributions in the open BB season but not completely consistent with those in the pre-monsoon and/or monsoon seasons. Their contribution distributions may reflect the use history and geographic distribution in secondary sources of POPs. The field-based contribution dataset of BB to POPs is significant in improving regional BB emission inventories and model prediction.

An increasing number of alternative flame retardants (FRs) are being introduced, following the international bans on the use of polybrominated diphenyl ether (PBDE) commercial mixtures. FRs' production capacity has shifted from developed countries to developing countries, with China being the world's largest producer and consumer of FRs. These chemicals are also imported with e-waste to China. Therefore, it is important to understand the current status of regulated brominated FRs, their phase-out in China, and their replacement by alternatives. In this study, a broad suite of legacy and alternative FRs, including eight PBDEs, six novel brominated FRs (NBFRs), two dechlorane plus variants (DP S ), and 12 organophosphate FRs (OPFRs) were evaluated in the air of 10 large Chinese cities in 2018. OPFRs are the most prevalent FRs in China, exhibiting a wide range of 1-612 ng/m 3 , which is several orders of magnitude higher than PBDEs (1-1827 pg/m 3 ) and NBFRs (1-1428 pg/m 3 ). BDE 209 and DBDPE are the most abundant compounds in brominated FRs (>80%). The North China Plain (NCP, excluding Beijing), Guangzhou, and Lanzhou appear to be three hotspots, although with different FR patterns. From 2013/2014 to 2018, levels of PBDEs, NBFRs, and DPs have significantly decreased, while that of OPFRs has increased by 1 order of magnitude. Gas-particle partitioning analysis showed that FRs could have not reached equilibrium, and the steady-state model is better suited for FRs with a higher log K OA (>13). To facilitate a more accurate FR assessment in fine particles, we suggest that, in addition to the conventional volumetric concentration (pg/m 3 ), the mass-normalized concentration (pg/g PM 2.5 ) could also be used.

Although organochlorine pesticides (OCPs) have been banned for more than three decades, their concentrations have only decreased gradually. This may be largely attributable to their environmental persistence, illegal application, and exemption usage. This study assessed the historic and current regional context for dichlorodiphenyltrichloroethane (DDT), chlordane, and hexachlorobenzene (HCB), which were added to the Stockholm Convention in 2001. An air sampling campaign was carried out in 2018 in nine cities of the Pearl River Delta (PRD), where the historical OCP application was the most intensive in China. Different seasonalities were observed: DDT exhibited higher concentrations in summer than in winter; chlordane showed less seasonal variation, whereas HCB was higher in winter. The unique coupling of summer monsoon with DDT-infused paint usage, winter monsoon with HCB-combustion emission, and local chlordane emission jointly presents a dynamic picture of these OCPs in the PRD air. We used the BETR Global model to back-calculate annual local emissions, which accounted for insignificant contributions to the nationally documented production (<1‰). Local emissions were the main sources of p,p' -DDT and chlordane, while ocean sources were limited (<4%). This study shows that geographic-anthropogenic factors, including source, history, and air circulation pattern, combine to affect the regional fate of OCP compounds.

Polychlorinated biphenyls (PCBs) were not widely manufactured or used in China before they became the subject of international bans on production. Recent work has shown that they have reached China associated with imported wastes and that there are considerable unintentional sources of PCBs that have only recently been identified. As such, it was hypothesized that the source inventory and profile of PCBs may be different or unique in China, compared to countries where they were widely used and which have been widely studied. For the first time in this study, we undertook a complete analysis of 209 PCB congeners and assessed the contribution of unintentionally produced PCBs (UP-PCBs) in the atmosphere of China, using polyurethane foam passive air samplers (PUF-PAS) deployed across a wide range of Chinese locations. ∑ 209 PCBs ranged from 9 to 6856 pg/m 3 (median: 95 pg/m 3 ) during three deployments in 2016-2017. PCB 11 was one of the most detected congeners, contributing 33 ± 19% to ∑ 209 PCBs. The main sources to airborne PCBs in China were estimated and ranked as pigment/painting (34%), metallurgical industry/combustion (31%), e-waste (23%), and petrochemical/plastic industry (6%). For typical Aroclor-PCBs, e-waste sources were dominated (>50%). Results from our study indicate that UP-PCBs have become the controlling source in the atmosphere of China, and an effective control strategy is urgently needed to mitigate emissions from multiple industrial sources.

Although polychlorinated biphenyls (PCBs) have been banned for several decades, they are still detected with elevated levels due to their unintentional production from combustion and industrial thermal processes (UP-PCBs). To investigate the composition and current levels of UP-PCBs and understand which sources are controlling PCB burdens in ambient atmosphere, air samples were collected from August 2012 to August 2015 at a background site in east China. An unexpected high abundance of PCB47+48+75 was observed to be the predominant congener with an average concentration of 786 ± 637 pg/m 3 . It accounted for 48 ± 16% of ΣPCBs, followed by PCB51 (10 ± 4%), PCB11 (8 ± 6%), and PCB68 (7 ± 3%). Seasonal variations with high levels in summer and lowest levels in winter were observed for PCB47+48+75, 51, and 68. These tetrachlorobiphenyl congeners were strongly correlated with temperature ( r 2 > 0.7), suggesting the control of temperature-dependent volatilization processes from contaminated surfaces. The decreased occurrence of PCB47+48+75, 51, and 68 in commercial products and their negative correlations (| r| < 0.35) with polycyclic aromatic hydrocarbon (PAHs) and weak correlation with other PCB congeners suggested unique unintentional sources that differ from combustion and industrial thermal processes or pigment, such as the use of polymer sealant, for PCB47+48+75, 51, and 68 in the ambient air.

Monosaccharides are important tracers of pollution aerosol from biomass burning. Air sampling of monosaccharides is often conducted using active samplers. However, applicability of sampling monosaccharides using polyurethane foam passive air samplers (PUF-PASs) has not been investigated, since passive air samplers are often applied to monitor semivolatile organic contaminants in large scale and remote area. Our study successfully collected atmospheric monosaccharides using PUF-PASs, providing a valuable tool for monosaccharides sampling. PUF-PAS sampling rates for individual monosaccharides were calibrated using an active sampler for 92 days, and were 1.1, 1.5, and 1.1 m 3 /d for levoglucosan, mannosan, and galactosan, respectively. Degradation of monosaccharides in PUF-PAS was demonstrated to be negligible by spike test of 13 C-labeled levoglucosan. Furthermore, passive sampling was carried out at 11 sites in the Pearl River Delta of Southern China from January to April and July to September of 2015. Monosaccharide concentrations derived from PUF-PASs were comparable with the reported data obtained by active sampling, demonstrating that the PUF-PAS approach is valid for monosaccharides monitoring. On the basis of our approach, we found that there is a clear correlation between the monosaccharide concentrations and the MODIS fire activities during January-April.

This study aimed for the first time to reconstruct historical exposure profiles for PCBs to the Chinese population, by examining the combined effect of changing temporal emissions and dietary transition. A long-term (1930-2100) dynamic simulation of human exposure using realistic emission scenarios, including primary emissions, unintentional emissions, and emissions from e-waste, combined with dietary transition trends was conducted by a multimedia fate model (BETR-Global) linked to a bioaccumulation model (ACC-HUMAN). The model predicted an approximate 30-year delay of peak body burden for PCB-153 in a 30-year-old Chinese female, compared to their European counterpart. This was mainly attributed to a combination of change in diet and divergent emission patterns in China. A fish-based diet was predicted to result in up to 8 times higher body burden than a vegetable-based diet (2010-2100). During the production period, a worst-case scenario assuming only consumption of imported food from a region with more extensive production and usage of PCBs would result in up to 4 times higher body burden compared to consumption of only locally produced food. However, such differences gradually diminished after cessation of production. Therefore, emission reductions in China alone may not be sufficient to protect human health from PCB-like chemicals, particularly during the period of mass production. The results from this study illustrate that human exposure is also likely to be dictated by inflows of PCBs via the environment, waste, and food.

Polychlorinated biphenyls (PCBs) are industrial organic contaminants identified as persistent, bioaccumulative, toxic (PBT), and subject to long-range transport (LRT) with global scale significance. This study focuses on a reconstruction and prediction for China of long-term emission trends of intentionally and unintentionally produced (UP) ∑ 7 PCBs (UP-PCBs, from the manufacture of steel, cement and sinter iron) and their re-emissions from secondary sources (e.g., soils and vegetation) using a dynamic fate model (BETR-Global). Contemporary emission estimates combined with predictions from the multimedia fate model suggest that primary sources still dominate, although unintentional sources are predicted to become a main contributor from 2035 for PCB-28. Imported e-waste is predicted to play an increasing role until 2020-2030 on a national scale due to the decline of intentionally produced (IP) emissions. Hypothetical emission scenarios suggest that China could become a potential source to neighboring regions with a net output of ∼0.4 t year -1 by around 2050. However, future emission scenarios and hence model results will be dictated by the efficiency of control measures.

DGT (diffusive gradients in thin-films) has been proposed as a tool for predicting Cd concentrations in rice grain, but there is a lack of authenticating data. To further explore the relationship between DGT measured Cd and concentrations in rice cultivated in challenging, metal degraded, field locations with different heavy metal pollutant sources, 77 paired soil and grain samples were collected in Southern China from industrial zones, a "cancer village" impacted by mining waste and an organic farm. In situ deployments of DGT in flooded paddy rice rhizospheres were compared with a laboratory DGT assay on dried and rewetted soil. Total soil concentrations were a very poor predictor of plant uptake. Laboratory and field deployed DGT assays and porewater measurements were linearly related to grain concentrations in all but the most contaminated samples where plant toxicity occurred. The laboratory DGT assay was the best predictor of grain Cd concentrations, accommodating differences in soil Cd, pollutant source, and Cd:Zn ratios. Field DGT measurements showed that Zn availability in the flooded rice rhizospheres was greatly diminished compared to that of Cd, resulting in very high Cd:Zn ratios (0.1) compared to commonly observed values (0.005). These results demonstrate the potential of the DGT technique to predict Cd concentrations in field cultivated rice and demonstrate its robustness in a range of environments. Although, field deployments provided important details about in situ element stoichiometry, due to the inherent heterogeneity of the rice rhizosphere soils, deployment of DGT in dried and homogenized soils offers the best possibility of a soil screening tool.