Holocene changes in biomass burning in the boreal Northern Hemisphere, reconstructed from anhydrosugar fluxes in an Arctic sediment profile.

The rapid warming of Arctic is causing increased fire activities in the boreal Northern Hemisphere (NH), leading to unprecedent changes in the global carbon cycling, human health and ecosystems. Understanding the interaction between fire and climate in this far north region is crucial for predicting future changes of wildfires. However, fire records over geological time scales are still scarce in the high latitudes of NH to provide comprehensive pictures of the fire history in this region. Here, we used the flux of levoglucosan (Lev) and its isomers in a sediment profile YN from Svalbard, high Arctic, as proxies for the changes in biomass burning from ∼9-2 kyr BP (thousand years before present). Backward trajectories and comparison with charcoal syntheses from various regions confirmed that the Lev transport to the profile site is sourced from the fire activities in the boreal NH, especially in northern Europe and northern Siberia. The Lev flux exhibited a slight overall decreasing trend at ∼3 %/kyr (p = 0.09) over the study period, as well as centennial maxima at ∼9, 8-7, 6, 5, and 4-3 kyr BP (p = 0.06). On sub-orbital scales, the long-term decrease in fire activities corresponded to trends of summer temperature in the extratropics of the NH (p = 0.01, r = 0.42), reflecting their regulation of fuel availability and flammability. On centennial to sub-millennial time scales, high levels of biomass burning were associated with periods of increased North Atlantic ice-rafted debris (p = 0.02, r = 0.38), which were indicative of cold and dry conditions over most of the source regions, reflecting the impacts of dryness on fuel flammability. The results suggested that enhanced Arctic amplification on centennial time scales may reduce biomass burning in most of the boreal NH, although fires in some mid-latitude regions may be facilitated.

Spatiotemporal distribution and influencing factors of secondary organic aerosols in the summer atmosphere from the Bering Sea to the western North Pacific.

To better understand the formation process of biogenic and anthropogenic secondary organic aerosols (BSOA and ASOA) in the marine atmosphere under the background of global warming, aerosol samples were collected over three summers (i.e., 2014, 2016 and 2018) from the Bering Sea (BS) to the western North Pacific (WNP). The results showed that temporally, atmospheric concentrations of isoprene-derived SOA (SOAI) tracers were the lowest in 2014 regardless of the marine region, while atmospheric concentrations of monoterpenes-derived SOA (SOAM) tracers in this year were the highest and the aerosols were more aged than those in the other two years. In comparison, the concentrations of ß-caryophyllene-derived and toluene-derived SOA (SOAC and SOAA) tracers were relatively low overall. Spatially, the concentrations of SOA tracers were significantly higher over the WNP than over the BS, with SOA tracers over the BS mainly coming from marine sources, while the WNP was strongly influenced by terrestrial inputs. In particular, for land-influenced samples from the WNP, NOx-channel products of SOAI were more dependent on O3 and SO2 relative to HO2-channel product, and the high atmospheric oxidation capacity and SO2 could promote the formation of later-generation SOAM products. The extent of terrestrial influence was further quantified using a principal component analysis (PCA)-generalized additive model (GAM), which showed that terrestrial emissions explained more than half of the BSOA tracers' concentrations and contributed almost all of the ASOA tracer. In addition, the assessment of secondary organic carbon (SOC) highlighted the key role of anthropogenic activities in organic carbon levels in offshore areas. Our study revealed significant contributions of terrestrial natural and anthropogenic sources to different SOA over the WNP, and these relevant findings help improve knowledge about SOA in the marine atmosphere.

Molecular characteristics, sources and influencing factors of isoprene and monoterpenes secondary organic aerosol tracers in the marine atmosphere over the Arctic Ocean.

Biogenic secondary organic aerosols (BSOA) are important components of the remote marine atmosphere. However, the response of BSOA changes to sea ice reduction over the Arctic Ocean remains unclear. Here we investigated isoprene and monoterpenes secondary organic aerosol (SOAI and SOAM) tracers in three years of summer aerosol samples collected from the Arctic Ocean atmosphere. The results indicated that methyltetrols were the most abundant SOAI tracers, while the main oxidation products of monoterpenes varied over the years owing to different aerosol aging. The results of the principal component analysis (PCA)-generalized additive model (GAM) combined with correlation analysis suggested that SOAI tracers were mainly generated by the oxidation of isoprene from marine emissions, while SOAM tracers were probably more influenced by terrestrial transport. Estimation of secondary organic carbon (SOC) indicated that monoterpenes oxidation contributed more than isoprene and that sea ice changes had a relatively small effect on biogenic SOC concentration levels. Our study quantified the contribution of influencing factors to the atmospheric concentration of BSOA tracers in the Arctic Ocean, and showed that there were differences in the sources of precursors for different BSOA. Hence, our findings have contributed to a better understanding of the characteristics, sources and formation of SOA in the atmosphere of the Arctic Ocean.

Polycyclic aromatic hydrocarbons (PAHs) in urban stream sediments of Suzhou Industrial Park, an emerging eco-industrial park in China: Occurrence, sources and potential risk.

In this study, urban stream sediment samples were collected in the Suzhou Industrial Park (SIP), one of the earliest national demonstration eco-industrial parks of China. PAHs were analyzed in these sediments, and concentrations of total PAHs were 180-81,000 ng g-1 (5700 ± 14,000 ng g-1). Medium molecular weight (4- ring) PAHs were predominant (42 ± 12%), followed by high molecular weight (5- and 6- ring) PAHs (31 ± 10%). No correlation was found between concentrations of PAHs and land uses of SIP in this study. Diagnostic ratios and a positive matrix factorization (PMF) model indicated that coal/biomass combustion might be the primary PAH source (61%), followed by non-combustion sources (21%) and vehicular emission (18%). According to the spatial analysis, PAHs in the sediments of SIP might be mainly associated with the coal/biomass combustion in the northeast industrial zone. Residential & commercial activities seem not to be the major causes of PAH contamination. Total PAH toxic equivalent concentrations, effect range low/effect range median values, and mean effects range-median quotient all showed that PAHs were present at a low toxicity risk level in most regions of the SIP. However, vigilance is required at some sampling sites with extremely high PAH concentrations or high mean effects range-median quotient.

Volatilization of polycyclic aromatic hydrocarbons (PAHs) over the North Pacific and adjacent Arctic Ocean: The impact of offshore oil drilling.

Air and seawater samples were collected in 2016 over the North Pacific Ocean (NPO) and adjacent Arctic Ocean (AO), and Polycyclic Aromatic Hydrocarbons (PAHs) were quantified in them. Atmospheric concentrations of ∑15 PAHs (gas + particle phase) were 0.44-7.0 ng m-3 (mean = 2.3 ng m-3), and concentrations of aqueous ∑15 PAHs (dissolved phase) were 0.82-3.7 ng L-1 (mean = 1.9 ng L-1). Decreasing latitudinal trends were observed for atmospheric and aqueous PAHs. Results of diagnostic ratios suggested that gaseous and aqueous PAHs were most likely to be related to the pyrogenic and petrogenic sources, respectively. Three sources, volatilization, coal and fuel oil combustion, and biomass burning, were determined by the PMF model for gaseous PAHs, with percent contributions of 10%, 44%, and 46%, respectively. The 4- ring PAHs underwent net deposition during the cruise, while some 3- ring PAHs were strongly dominated by net volatilization, even in the high latitude Arctic region. Offshore oil/gas production activities might result in the sustained input of low molecular weight 3- ring PAHs to the survey region, and further lead to the volatilization of them. Compared to the gaseous exchange fluxes, fluxes of atmospheric dry deposition and gaseous degradation were negligible. According to the extrapolated results, the gaseous exchange of semivolatile aromatic-like compounds (SALCs) may have a significant influence on the carbon cycling in the low latitude oceans, but not for the high latitude oceans.

Atmospheric organochlorine pesticides (OCPs) and polychlorinated biphenyls (PCBs) in the Antarctic marginal seas: Distribution, sources and transportation.

From November 2013 to March 2014, air samples were collected in the Antarctic marginal seas during the 30th Chinese Antarctic research expedition. Organochlorine pesticides (OCPs) and polychlorinated biphenyls (PCBs) were analyzed in these samples. The mean concentrations were observed for hexachlorobenzene (HCB) >ΣPCBs >Σhexachlorocyclohexanes(HCHs) >Σdichlorodiphenyltrichloroethane(DDTs)>Σchlordanes. High levels of HCB were found near east Antarctica and in the Ross Sea, reflecting the re-emission of HCB from environmental reservoirs of these regions. Parent DDTs (p,p'- and o,p'-DDT) were rarely detected, suggesting that atmospheric DDT was predominantly influencedby weathered DDT from some secondarysources. However, fresh inputs of DDTs could not be excluded because there were still some samples with high proportions of parent DDTs. HCHs only were detected in the South Indian Ocean (near Australia), andthis result might be related to the intense emissions of HCHs from southern Australia. Ratios of trans-chlordane/cis-chlordanein most samples were lower than that in technical chlordane, reflecting the main influence of weathered chlordane. High levels of ΣPCBs were found in the Ross Sea, suggesting an intense re-emission of PCBs. Furthermore, atmospheric PCBs near the Antarctic Peninsula were also relatively high, this finding might be attributed to the emissions of PCBs from nearby Antarctic research stations. Comparing with the Arctic, transport of OCPs and PCBs towards Antarctica is more difficult. The Antarctic marginal seas would act as both barriers and "buffer zones"during the transportation processes.