The abrupt warming events punctuating the Termination 1 (about 11.7-18 ka Before Present, BP) were marked by sharp rises in the concentration of atmospheric methane (CH4). The role of permafrost organic carbon (OC) in these rises is still debated, with studies based on top-down measurements of radiocarbon (14C) content of CH(4 )trapped in ice cores suggesting minimum contributions from old and strongly C-14-depleted permafrost OC. However, organic matter from permafrost can exhibit a continuum of C-14 ages (contemporaneous to >50 ky). Here, we investigate the large-scale permafrost remobilization at the Younger Dryas-Preboreal transition (ca. 11.6 ka BP) using the sedimentary record deposited at the Lena River paleo-outlet (Arctic Ocean) to reflect permafrost destabilization in this vast drainage basin. Terrestrial OC was isolated from sediments and characterized geochemically measuring delta C-13, Delta C-14, and lignin phenol molecular fossils. Results indicate massive remobilization of relatively young (about 2,600 years) permafrost OC from inland Siberia after abrupt warming triggered severe active layer deepening. Methane emissions from this young fraction of permafrost OC contributed to the deglacial CH4 rise. This study stresses that underestimating permafrost complexities may affect our comprehension of the deglacial permafrost OC-climate feedback and helps understand how modern permafrost systems may react to rapid warming events, including enhanced CH4 emissions that would amplify anthropogenic climate change.
Sources and implications of black carbon (BC) and mineral dust (MD) on two glaciers on the central Tibetan Plateau were estimated based on in situ measurements and modeling. The results indicated that BC and MD accounted for 11 +/- 1% and 4 +/- 0% of the albedo reduction relative to clean snow, while the radiative forcing varied between 11 and 196 and 1-89 W m(-2), respectively. Assessment of BC and MD contributions to the glacier melt can reach up 88 to 434 and 35 to 187 mm w.e., respectively, contributing 9-23 and 4-10% of the total glacier melt. A footprint analysis indicated that BC and MD deposited on the glaciers originated mainly from the Middle East, Central Asia, North China and South Asia during the study period. Moreover, a potentially large fraction of BC may have originated from local and regional fossil fuel combustion. This study suggests that BC and MD will enhance glacier melt and provides a scientific basis for regional mitigation efforts.
Vehicle -emitted fine particulate matter (PM 2.5 ) has been associated with significant health outcomes and environmental risks. This study estimates the contribution of traffic -related exhaust emissions (TREE) to observed PM 2.5 using a novel factorization framework. Specifically, co -measured nitrogen oxides (NO x ) concentrations served as a marker of vehicle -tailpipe emissions and were integrated into the optimization of a Non -negative Matrix Factorization (NMF) analysis to guide the factor extraction. The novel TREE-NMF approach was applied to long-term (2012 - 2019) PM 2.5 observations from air quality monitoring (AQM) stations in two urban areas. The extracted TREE factor was evaluated against co -measured black carbon (BC) and PM 2.5 species to which the TREE-NMF optimization was blind. The contribution of the TREE factor to the observed PM 2.5 concentrations at an AQM station from the first location showed close agreement ( R 2 = 0 .79) with monitored BC data. In the second location, a comparison of the extracted TREE factor with measurements at a nearby Surface PARTiculate mAtter Network (SPARTAN) station revealed moderate correlations with PM 2.5 species commonly associated with fuel combustion, and a good linear regression fit with measured equivalent BC concentrations. The estimated concentrations of the TREE factor at the second location accounted for 7 - 11 % of the observed PM 2.5 in the AQM stations. Moreover, analysis of specific days known to be characterized by little traffic emissions suggested that approximately 60 - 78 % of the traffic -related PM 2.5 concentrations could be attributed to particulate traffic -exhaust emissions. The methodology applied in this study holds great potential in areas with limited monitoring of PM 2.5 speciation, in particular BC, and its results could be valuable for both future environmental health research, regional radiative forcing estimates, and promulgation of tailored regulations for traffic -related air pollution abatement.
Carbonaceous particles are an important radiative forcing agent in the atmosphere, with large temporal and spatial variations in their concentrations and compositions, especially in remote regions. This study reported the delta C-14 and delta C-13 of total carbon (TC) and water-insoluble particulate carbon (IPC) of the total suspended particles (TSP) and PM2.5 at a remote site of the eastern Tibetan Plateau (TP), a region that is influenced by heavy air pollution from Southwest China. The average organic carbon and elemental carbon concentrations of TSP samples in this study were 3.20 +/- 2.38 mu g m(-3) and 0.68 +/- 0.67 mu g m(-3), respectively, with low and high values in summer and winter, respectively. The fossil fuel contributions of TC in TSP and PM2.5 samples were 18.91 +/- 7.22% and 23.13 +/- 12.52%, respectively, both of which were far lower than that in Southwest China, indicating the importance of non-fossil contributions from local sources. The delta C-13 of TC in TSP samples of the study site was -27.06 +/- 0.96 parts per thousand, which is between the values of long-range transported sources (e.g., Southwest China) and local biomass combustion emissions. Therefore, despite the contribution from the long-range transport of particles, aerosols emitted from local biomass combustion also have an important influence on carbonaceous particles at the study site. The findings of this work can be applied to other remote sites on the eastern TP and should be considered in related research in the future.
PM2.5 impacts the atmospheric temperature structure through scattering or absorbing solar radiation, whose concentration and composition can affect the impact. This study calculated the effect of PM2.5 on the temperature structures in the urban centre and the suburbs of Nanjing, as well as their differences. The results show that the optical parameters, atmospheric heating rate, radiative forcing, and temperature are all impacted by the concentration and composition of PM2.5. The uneven distribution of PM2.5 influences the differences in those factors between the urban centre and suburbs. In spring, summer, autumn, and winter, surface temperatures in the urban centre were approximately 283 K, 285 K, 305 K, and 277 K, while those in the suburbs were approximately 282 K, 283 K, 304 K, and 274 K. The urban heat island intensity has been reduced by 0.1-0.4 K due to the presence of PM2.5 in Nanjing. Due to the black carbon component's warming effect on the top of the boundary layer, the impact of PM2.5 on the urban heat island intensity profile drops quickly at the 0.75-1.25 km. PM2.5 may mask the warm city problem and have a more complex impact on the urban climate.
Arctic rivers provide an integrated signature of the changing landscape and transmit signals of change to the ocean. Here, we use a decade of particulate organic matter (POM) compositional data to deconvolute multiple allochthonous and autochthonous pan-Arctic and watershed-specific sources. Constraints from carbon-to-nitrogen ratios (C:N), delta C-13, and Delta C-14 signatures reveal a large, hitherto overlooked contribution from aquatic biomass. Separation in Delta C-14 age is enhanced by splitting soil sources into shallow and deep pools (mean +/- SD: -228 +/- 211 vs. - 492 +/- 173%) rather than traditional active layer and permafrost pools (-300 +/- 236 vs. -441 +/- 215%) that do not represent permafrost-free Arctic regions. We estimate that 39 to 60% (5 to 95% credible interval) of the annual pan-Arctic POM flux (averaging 4,391 Gg/y particulate organic carbon from 2012 to 2019) comes from aquatic biomass. The remainder is sourced from yedoma, deep soils, shallow soils, petrogenic inputs, and fresh terrestrial production. Climate change-induced warming and increasing CO2 concentrations may enhance both soil destabilization and Arctic river aquatic biomass production, increasing fluxes of POM to the ocean. Younger, autochthonous, and older soil-derived POM likely have different destinies (preferential microbial uptake and processing vs. significant sediment burial, respectively). A small (similar to 7%) increase in aquatic biomass POM flux with warming would be equivalent to a similar to 30% increase in deep soil POM flux. There is a clear need to better quantify how the balance of endmember fluxes may shift with different ramifications for different endmembers and how this will impact the Arctic system.
Since China implemented the Air Pollution Prevention and Control Action Plan in 2013, the aerosol emis-sions in East Asia have been greatly reduced, while emissions in South Asia have continued to increase. This has led to a dipole pattern of aerosol emissions between South Asia and East Asia. Here, the East Asian summer monsoon (EASM) responses to the dipole changes in aerosol emissions during 2013-17 are investigated using the atmosphere model of Com-munity Earth System Model version 2 (CESM2). We show that decreases in East Asian emissions alone lead to a positive aerosol effective radiative forcing (ERF) of 1.59 (+/- 0.97) W m-2 over central-eastern China (25 degrees-40 degrees N, 105 degrees-122.5 degrees E), along with a 0.09 (+/- 0.07)degrees C warming in summer during 2013-17. The warming intensified the land-sea thermal contrast and increased the rainfall by 0.32 (+/- 0.16) mm day-1. When considering both the emission reductions in East Asia and in-creases in South Asia, the ERF is increased to 3.39 (+/- 0.89) W m-2, along with an enhanced warming of 0.20 (+/- 0.08)degrees C over central-eastern China, while the rainfall insignificant decreased by 0.07 (+/- 0.16) mm day-1. It is due to the westward shift of the strengthened western Pacific subtropical high, linked to the increase in black carbon in South Asia. Based on multiple EASM indices, the reductions in aerosol emissions from East Asia alone increased the EASM strength by almost 5%. Considering the effect of the westward shift of WPSH, the dipole changes in emissions together increased the EASM by 5%-15% during 2013-17, revealing an important role of South Asian aerosols in changing the East Asian climate.
Aviation emissions are the only direct source of anthropogenic particulate pollution at high altitudes, which can form con-trails and contrail-induced clouds, with consequent effects upon global radiative forcing. In this study, we develop a pre-dictive model, called APMEP-CNN, for aviation non-volatile particulate matter (nvPM) emissions using a convolutional neural network (CNN) technique. The model is established with data sets from the newly published aviation emission databank and measurement results from several field studies on the ground and during cruise operation. The model also takes the influence of sustainable aviation fuels (SAFs) on nvPM emissions into account by considering fuel properties. This study demonstrates that the APMEP-CNN can predict nvPM emission index in mass (EIm) and number (EIn) for a number of high-bypass turbofan engines. The accuracy of predicting EIm and EIn at ground level is significantly improved (R2 = 0.96 and 0.96) compared to the published models. We verify the suitability and the applicability of the APMEP-CNN model for estimating nvPM emissions at cruise and burning SAFs and blend fuels, and find that our predictions for EIm are within & PLUSMN;36.4 % of the measurements at cruise and within & PLUSMN;33.0 % of the measurements burning SAFs in av-erage. In the worst case, the APMEP-CNN prediction is different by -69.2 % from the measurements at cruise for the JT3D-3B engine. Thus, the APMEP-CNN model can provide new data for establishing accurate emission inventories of global aviation and help assess the impact of aviation emissions on human health, environment and climate.Synopsis: The results of this paper provide accurate predictions of nvPM emissions from in-use aircraft engines, which im-pact airport local air quality and global radiative forcing.
Carbonaceous particles are an important radiative forcing agent in the atmosphere, with large temporal and spatial variations in their concentrations and compositions, especially in remote regions. This study reported the delta C-14 and delta C-13 of total carbon (TC) and water-insoluble particulate carbon (IPC) of the total suspended particles (TSP) and PM2.5 at a remote site of the eastern Tibetan Plateau (TP), a region that is influenced by heavy air pollution from Southwest China. The average organic carbon and elemental carbon concentrations of TSP samples in this study were 3.20 +/- 2.38 mu g m(-3) and 0.68 +/- 0.67 mu g m(-3), respectively, with low and high values in summer and winter, respectively. The fossil fuel contributions of TC in TSP and PM2.5 samples were 18.91 +/- 7.22% and 23.13 +/- 12.52%, respectively, both of which were far lower than that in Southwest China, indicating the importance of non-fossil contributions from local sources. The delta C-13 of TC in TSP samples of the study site was -27.06 +/- 0.96 parts per thousand, which is between the values of long-range transported sources (e.g., Southwest China) and local biomass combustion emissions. Therefore, despite the contribution from the long-range transport of particles, aerosols emitted from local biomass combustion also have an important influence on carbonaceous particles at the study site. The findings of this work can be applied to other remote sites on the eastern TP and should be considered in related research in the future.
The atmospheric circulation plays a critical role in the global transport and deposition of atmospheric pollutants such as mercury (Hg). Desert dust emissions contribute to nearly 60-95% of the global dust budget and thus, desert dust may facilitate atmospheric Hg transport and deposition to the downwind regions worldwide. The role of desert dust in biogeochemical cycling of Hg, however, has not been well recognized by the Hg research community. In this study, we measured the concentration of particulate bound Hg (HgP) in total suspended particulate (TSP) collected from China's largest desert, Taklimakan Desert, between 2013 and 2017. The results show that HgP concentrations over the Taklimakan Desert atmosphere are remarkably higher than those observed from background sites in China and are even comparable to those measured in most of the Chinese metropolitan cities. Moreover, HgP concentrations in the Taklimakan Desert exhibit a distinct seasonal pattern peaking during dust storm outbreak periods in spring and summer (March to August). A preliminary estimation demonstrates that export of total Hg associated with atmospheric dust from the Taklimakan Desert could be 59.7 +/- 60.3 (1SD) Mg yr(-1). The unexpectedly high HgP concentrations during duststorms, together with consistent seasonal pattern of Hg revealed from the snow/ice, clearly demonstrate that Asian desert dust could act as a significant carrier of atmospheric Hg to the cryosphere of Western China and even can have further global reach. (C) 2020 Elsevier Ltd. All rights reserved.