Search

Mountainous rivers are critical in transporting dissolved organic carbon (DOC) from terrestrial environments to downstream ecosystems. However, how geomorphologic factors and anthropogenic impacts control the composition and export of DOC in mountainous rivers remains largely unclear. Here, we explore DOC dynamics in three subtropical mountainous catchments (i.e., the Yinjiang, Shiqian, and Yuqing catchments) in southwest China, which are heavily influenced by anthropogenic activities. Water chemistry, stable and radioactive carbon isotopes of DOC (δ13CDOC and Δ14CDOC), and optical properties (UV absorbance and fluorescence spectra) were employed to assess the biogeochemical processes and controlling factors on riverine DOC. The radiocarbon ages of DOC in the Yinjiang River varied widely from 928 years BP to the present. Stepwise multiple regression analyses and partial least square path models revealed that geomorphology and anthropogenic activities were the major drivers controlling DOC concentrations and DOM characteristics. Catchments with higher catchment slope gradients were characterized by lower DOC concentrations, enriched δ13CDOC and Δ14CDOC, and more aromatic dissolved organic matter (DOM), which were opposite to catchments with gentle catchment slopes. Variabilities in DOC concentrations were also regulated by land use, with higher DOC concentrations in urban and agricultural areas. Furthermore, DOM in catchments with a higher proportion of urban and agricultural land uses was less aromatic, less recently produced, and exhibited a higher degree of humification and more autochthonous humic-like DOM. This research highlights the significance of incorporating geomorphologic controls on DOC sources and anthropogenic impacts on DOM composition into the understanding of DOC dynamics and the quality of DOM in mountainous rivers, which are globally abundant.

A primary sink of air pollutants and their precursors is dry deposition. Dry deposition estimates differ across chemical transport models, yet an understanding of the model spread is incomplete. Here, we introduce Activity 2 of the Air Quality Model Evaluation International Initiative Phase 4 (AQMEII4). We examine 18 dry deposition schemes from regional and global chemical transport models as well as standalone models used for impact assessments or process understanding. We configure the schemes as single-point models at eight Northern Hemisphere locations with observed ozone fluxes. Single-point models are driven by a common set of site-specific meteorological and environmental conditions. Five of eight sites have at least 3 years and up to 12 years of ozone fluxes. The interquartile range across models in multiyear mean ozone deposition velocities ranges from a factor of 1.2 to 1.9 annually across sites and tends to be highest during winter compared with summer. No model is within 50 % of observed multiyear averages across all sites and seasons, but some models perform well for some sites and seasons. For the first time, we demonstrate how contributions from depositional pathways vary across models. Models can disagree with respect to relative contributions from the pathways, even when they predict similar deposition velocities, or agree with respect to the relative contributions but predict different deposition velocities. Both stomatal and nonstomatal uptake contribute to the large model spread across sites. Our findings are the beginning of results from AQMEII4 Activity 2, which brings scientists who model air quality and dry deposition together with scientists who measure ozone fluxes to evaluate and improve dry deposition schemes in the chemical transport models used for research, planning, and regulatory purposes.

Strict air pollution control strategies have been implemented in recent decades in the North China Plain (NCP), previously one of the most polluted regions in the world, and have resulted in considerable changes in emissions of air pollutants. However, little is so far known about the long-term trends of the regional background level of NOx and SO2, along with the increase and decrease processes of regional emissions. In this study, the seasonal and diurnal variations of NOx and SO2 as well as their long-term trends at a regional background station in the NCP were characterized from 2004 to 2016. On average, SO2 and NOx mixing ratios were 5.7 ± 8.4 and 14.2 ± 12.4 ppb, respectively. The seasonal variations in SO2 and NOx mixing ratios showed a similar pattern, with a peak in winter and a valley in summer. However, the diurnal variations in SO2 and NOx mixing ratios greatly differed for all seasons, indicating different sources for SO2 and NOx and meteorological effects on their concentrations. Overall, the annual mean SO2 exhibited a significant decreasing trend of −6.1 % yr−1 (R = −0.84, P < 0.01) from 2004 to 2016, which is very close to −6.3 % yr−1 of the annual SO2 emission in Beijing, and a greater decreasing trend of −7.4 % yr−1 (R = −0.95, P < 0.01) from 2008 to 2016. The annual mean of NOx showed a fluctuating rise of +3.4 % yr−1 (R = 0.38, P = 0.40) from 2005 to 2010, reaching the peak value (16.9 ppb) in 2010, and then exhibited an extremely significant fluctuating downward trend of −4.5 % yr−1 (R = 0.95, P < 0.01) from 2010 to 2016. After 2010, the annual mean NOx mixing ratios correlated significantly (R = 0.94, P < 0.01) with the annual NOx emission in North China. The decreasing rate (−4.8 % yr−1, R = −0.92, P < 0.01) of the annual mean NOx mixing ratios from 2011 to 2016 at the Shangdianzi (SDZ) regional atmospheric background station is lower than the one (−8.8 % yr−1, R = −0.94, P < 0.01) for the annual NOx emission in the NCP and in Beijing (−9.0 % yr−1, R = −0.96, P < 0.01). This indicated that surface NOx mixing ratios at SDZ had a weaker influence than SO2 on the emission reduction in Beijing and its surrounding areas in the NCP. The increase in the number of motor vehicles led to an increase in traffic emissions for NOx. This study supported conclusions from previous studies that the measures taken for controlling NOx and SO2 in the NCP in the past decades were generally successful. However, NOx emission control should be strengthened in the future.

In situ measurements of vertically resolved particle size distributions based on a tethered balloon system were carried out for the first time in the highland city of Lhasa over the Tibetan Plateau in summer 2020, using portable optical counters for the size range of ​​​​​​​0.124–32 µm. The vertical structure of 112 aerosol profiles was found to be largely shaped by the evolution of the planetary boundary layer (PBL), with a nearly uniform distribution of aerosols within the daytime mixing layer and a sharp decline with the height in the shallow nocturnal boundary layer. During the campaign, mass concentrations of particulate matter smaller than 2.5 µm in aerodynamic diameter (PM2.5) within the PBL ranged from 0.5 to 12.0 µg m−3, with an average and standard deviation of 3.4 ± 2.3 µg m−3, almost 4 times the amount in the free troposphere (FT), which was rarely affected by surface anthropogenic emissions. Though there was a lower level of particle mass in the residual layer (RL) than in the PBL, a similarity in particle mass size distributions (PMSDs) suggested that particles in the RL might be of the same origin as the particles in the PBL. This was also consistent with the source apportionment analysis based on the PMSDs. In total, three distinct modes were observed in the PMSDs for the PBL and the RL. One mode was exclusively coarse particles up to roughly 15 µm, peaking around 5 µm. More than 50 % of total particle mass was often contributed by coarse-mode particles in this area, which was thought to be associated with local dust resuspension. The mode peaking over 0.5–0.7 µm was representative of biomass burning on religious holidays and was found to be most pronounced on holiday mornings. The contribution from the religious burning factor rose from about 25 % on non-holidays to nearly 50 % on holiday mornings. The mode dominated by particles smaller than 0.3 µm was thought to be associated with combustion-related emissions and/or secondary aerosol formation. In the FT coarse mode, particles only accounted for less than 10 % of the total mass, and particles larger than 5 µm were negligible. The predominant submicron particles in the FT might be related to secondary aerosol formation and the aging of existing particles. To give a full picture of aerosol physical and chemical properties and better understand the origin and impacts of aerosols in this area, intensive field campaigns involving measurements of vertically resolved aerosol chemical compositions in different seasons would be highly encouraged in the future.

CO2 efflux at the water–air interface is an essential component of the riverine carbon cycle. However, the lack of spatially resolved CO2 emission measurements prohibits reliable estimation of the global riverine CO2 emissions. By deploying floating chambers, seasonal changes in river water CO2 partial pressure (pCO2) and CO2 emissions from the Dong River in south China were investigated. Spatial and temporal patterns of pCO2 were mainly affected by terrestrial carbon inputs (i.e., organic and inorganic carbon) and in-stream metabolism, both of which varied due to different land cover, catchment topography, and seasonality of precipitation and temperature. Temperature-normalized gas transfer velocity (k600) in small rivers was 8.29 ± 11.29 and 4.90 ± 3.82 m d−1 for the wet season and dry season, respectively, which was nearly 70 % higher than that of large rivers (3.90 ± 5.55 m d−1 during the wet season and 2.25 ± 1.61 m d−1 during the dry season). A significant correlation was observed between k600 and flow velocity but not wind speed regardless of river size. Most of the surveyed rivers were a net CO2 source while exhibiting substantial seasonal variations. The mean CO2 flux was 300.1 and 264.2 mmol m−2 d−1 during the wet season for large and small rivers, respectively, 2-fold larger than that during the dry season. However, no significant difference in CO2 flux was observed between small and large rivers. The absence of commonly observed higher CO2 fluxes in small rivers could be associated with the depletion effect caused by abundant and consistent precipitation in this subtropical monsoon catchment.

The Community Multiscale Air Quality (CMAQ) model version 5.3 (CMAQ53), released to the public in August 2019 and followed by version 5.3.1 (CMAQ531) in December 2019, contains numerous science updates, enhanced functionality, and improved computation efficiency relative to the previous version of the model, 5.2.1 (CMAQ521). Major science advances in the new model include a new aerosol module (AERO7) with significant updates to secondary organic aerosol (SOA) chemistry, updated chlorine chemistry, updated detailed bromine and iodine chemistry, updated simple halogen chemistry, the addition of dimethyl sulfide (DMS) chemistry in the CB6r3 chemical mechanism, updated M3Dry bidirectional deposition model, and the new Surface Tiled Aerosol and Gaseous Exchange (STAGE) bidirectional deposition model. In addition, support for the Weather Research and Forecasting (WRF) model's hybrid vertical coordinate (HVC) was added to CMAQ53 and the Meteorology-Chemistry Interface Processor (MCIP) version 5.0 (MCIP50). Enhanced functionality in CMAQ53 includes the new Detailed Emissions Scaling, Isolation and Diagnostic (DESID) system for scaling incoming emissions to CMAQ and reading multiple gridded input emission files. Evaluation of CMAQ531 was performed by comparing monthly and seasonal mean daily 8 h average (MDA8) O3 and daily PM2.5 values from several CMAQ531 simulations to a similarly configured CMAQ521 simulation encompassing 2016. For MDA8 O3, CMAQ531 has higher O3 in the winter versus CMAQ521, due primarily to reduced dry deposition to snow, which strongly reduces wintertime O3 bias (2–4 ppbv monthly average). MDA8 O3 is lower with CMAQ531 throughout the rest of the year, particularly in spring, due in part to reduced O3 from the lateral boundary conditions (BCs), which generally increases MDA8 O3 bias in spring and fall (∼0.5 µg m−3). For daily 24 h average PM2.5, CMAQ531 has lower concentrations on average in spring and fall, higher concentrations in summer, and similar concentrations in winter to CMAQ521, which slightly increases bias in spring and fall and reduces bias in summer. Comparisons were also performed to isolate updates to several specific aspects of the modeling system, namely the lateral BCs, meteorology model version, and the deposition model used. Transitioning from a hemispheric CMAQ (HCMAQ) version 5.2.1 simulation to a HCMAQ version 5.3 simulation to provide lateral BCs contributes to higher O3 mixing ratios in the regional CMAQ simulation in higher latitudes during winter (due to the decreased O3 dry deposition to snow in CMAQ53) and lower O3 mixing ratios in middle and lower latitudes year-round (due to reduced O3 over the ocean with CMAQ53). Transitioning from WRF version 3.8 to WRF version 4.1.1 with the HVC resulted in consistently higher (1.0–1.5 ppbv) MDA8 O3 mixing ratios and higher PM2.5 concentrations (0.1–0.25 µg m−3) throughout the year. Finally, comparisons of the M3Dry and STAGE deposition models showed that MDA8 O3 is generally higher with M3Dry outside of summer, while PM2.5 is consistently higher with STAGE due to differences in the assumptions of particle deposition velocities to non-vegetated surfaces and land use with short vegetation (e.g., grasslands) between the two models. For ambient NH3, STAGE has slightly higher concentrations and smaller bias in the winter, spring, and fall, while M3Dry has higher concentrations and smaller bias but larger error and lower correlation in the summer.

The element silicon (Si) is required for the growth of silicified organisms in marine environments, such as diatoms. These organisms consume vast amounts of Si together with N, P, and C, connecting the biogeochemical cycles of these elements. Thus, understanding the Si cycle in the ocean is critical for understanding wider issues such as carbon sequestration by the ocean's biological pump. In this review, we show that recent advances in process studies indicate that total Si inputs and outputs, to and from the world ocean, are 57 % and 37 % higher, respectively, than previous estimates. We also update the total ocean silicic acid inventory value, which is about 24 % higher than previously estimated. These changes are significant, modifying factors such as the geochemical residence time of Si, which is now about 8000 years, 2 times faster than previously assumed. In addition, we present an updated value of the global annual pelagic biogenic silica production (255 Tmol Si yr−1) based on new data from 49 field studies and 18 model outputs, and we provide a first estimate of the global annual benthic biogenic silica production due to sponges (6 Tmol Si yr−1). Given these important modifications, we hypothesize that the modern ocean Si cycle is at approximately steady state with inputs =14.8(±2.6) Tmol Si yr−1 and outputs =15.6(±2.4) Tmol Si yr−1. Potential impacts of global change on the marine Si cycle are discussed.

In this study, we present O3 retrievals from ground-based Fourier transform infrared (FTIR) solar absorption measurements between June 2018 and December 2019 at Xianghe, China (39.75∘ N, 116.96∘ E). The FTIR spectrometer at Xianghe is operated with indium gallium arsenide (InGaAs) and indium antimonide (InSb) detectors, recording the spectra between 1800 and 11 000 cm−1. As the harmonized FTIR O3 retrieval strategy (Vigouroux et al., 2015) within the Network for the Detection of Atmospheric Composition Change (NDACC) uses the 1000 cm−1 spectral range, we apply the O3 retrieval in the 3040 cm−1 spectral range at Xianghe. The retrieved O3 profile is mainly sensitive to the vertical range between 10 and 40 km, and the degrees of freedom for signal is 2.4±0.3 (1σ), indicating that there are two individual pieces of information in partial columns between the surface and 20 km and between 20 and 40 km. According to the optimal estimation method, the systematic and random uncertainties of the FTIR O3 total columns are about 13.6 % and 1.4 %, respectively. The random uncertainty is consistent with the observed daily standard deviation of the FTIR retrievals. To validate the FTIR O3 total and partial columns, we apply the same O3 retrieval strategy at Maïdo, Réunion (a.k.a. Reunion Island; 21.08∘ N, 55.38∘ E). The FTIR O3 (3040 cm−1) measurements at Xianghe and Maïdo are then compared with the nearby ozonesondes at Beijing (39.81∘ N, 116.47∘ E) and at Gillot (20.89∘ S, 55.53∘ E), respectively, as well as with co-located TROPOspheric Monitoring Instrument (TROPOMI) satellite measurements at both sites. In addition at Maïdo, we compare the FTIR O3 (3040 cm−1) retrievals with the standard NDACC FTIR O3 measurements using the 1000 cm−1 spectral range. It was found that the total columns retrieved from the FTIR O3 3040 cm−1 measurements are underestimated by 5.5 %–9.0 %, which is mainly due to the systematic uncertainty in the partial column between 20 and 40 km (about −10.4 %). The systematic uncertainty in the partial column between surface and 20 km is relatively small (within 2.4 %). By comparison with other measurements, it was found that the FTIR O3 (3040 cm−1) retrievals capture the seasonal and synoptic variations of the O3 total and two partial columns very well. Therefore, the ongoing FTIR measurements at Xianghe can provide useful information on the O3 variations and (in the future) long-term trends.

Characterizing vertical profiles of aerosol optical properties is important because relying on only the surface or column-integrated measurements cannot unambiguously constrain the radiative impacts of aerosol. This study presents series of vertical profiles of in situ measured multi-wavelength optical properties of aerosols during three pollution events from November to December 2016 over the Beijing region. For all pollution events, the clean periods (CPs) before pollution initialization showed a higher scattering Ångström exponent (SAE) and a smaller asymmetry parameter (g) with relatively uniform vertical structures. The heavy pollution periods (HPs) showed an increased particle size, causing these parameters to vary in the opposite way. During the transition periods (TPs), regional transport of aged aerosols at higher altitudes was found. The Aerosol Robotic Network (AERONET) aerosol optical depth (AOD) matched the in situ measurements within 10 %; however the AERONET absorption optical depth (AAOD) was 10 %–20 % higher than the in situ measurements, and this positive discrepancy increased to 30 % at shorter wavelengths. The absorption of brown carbon (BrC) was identified by the increased-absorption Ångström exponent (AAE), and the heating rate of black carbon (BC) and BrC was estimated by computing the spectral absorption coefficient and actinic flux calculated by a radiative transfer model. BC and BrC had a heating rate of up to 0.18 and 0.05 K h−1 in the planetary boundary layer (PBL), respectively, during the pollution period. The fraction of BrC absorption increased from 12 % to 40 % in the PBL from the CP to the HP. Notably, a higher contribution of BrC heating was found above the PBL under polluted conditions. This study paints a full picture of shortwave heating impacts of carbonaceous aerosols during different stages of pollution events and highlights the increased contribution of BrC absorption especially at higher altitudes during pollution.

Natural sea-salt aerosols, when interacting with anthropogenic emissions, can enhance the formation of particulate nitrate. This enhancement has been suggested to increase the direct radiative forcing of nitrate, called the “mass-enhancement effect”. Through a size-resolved dynamic mass transfer modeling approach, we show that interactions with sea salt shift the nitrate from sub- to super-micron-sized particles (“redistribution effect”), and hence this lowers its efficiency for light extinction and reduces its lifetime. The redistribution effect overwhelms the mass-enhancement effect and significantly moderates nitrate cooling; e.g., the nitrate-associated aerosol optical depth can be reduced by 10 %–20 % over European polluted regions during a typical sea-salt event, in contrast to an increase by ∼10 % when only accounting for the mass-enhancement effect. Global model simulations indicate significant redistribution over coastal and offshore regions worldwide. Our study suggests a strong buffering by natural sea-salt aerosols that reduces the climate forcing of anthropogenic nitrate, which had been expected to dominate the aerosol cooling by the end of the century. Comprehensive considerations of this redistribution effect foster better understandings of climate change and nitrogen deposition.

Abstract We present a regional‐scale integrated modeling system (IMS) that includes Environmental Policy Integrated Climate (EPIC), Weather Research and Forecast (WRF), Community Multiscale Air Quality (CMAQ), and Soil and Water Assessment Tool (SWAT) models. The centerpiece of the IMS is the Fertilizer Emission Scenario Tool for CMAQ (FEST‐C), which includes a Java‐based interface and EPIC adapted to regional applications along with built‐in database and tools. The SWAT integration capability is a key enhanced feature in the current release of FEST‐C v1.4. For integrated modeling demonstration and evaluation, FEST‐C EPIC is simulated over three individual years with WRF/CMAQ weather and N deposition. Simulated yearly changes in water and N budgets along with yields for two major crops (corn grain and soybean) match those inferred from intuitive physical reasoning and survey data given different‐year weather conditions. Yearlong air quality simulations with an improved bidirectional ammonia flux modeling approach directly using EPIC‐simulated soil properties including NH3 content helps reduce biases of simulated gas‐phase NH3 and NH4+ wet deposition over the growing season. Integrated hydrology and water quality simulations applied to the Mississippi River Basin show that estimated monthly streamflow and dissolved N near the outlet to the Gulf of Mexico display similar seasonal patterns as observed. Limitations and issues in different parts of the integrated multimedia simulations are identified and discussed to target areas for future improvements.

This study describes and implements an integrated, multimedia, process-based system-level approach to estimating nitrogen (N) fate and transport in large river basins. The modeling system includes the following components: (1) Community Multiscale Air Quality (CMAQ), (2) Weather Research and Forecasting Model (WRF), (3) Environmental Policy Integrated Climate (EPIC), and (4) Soil and Water Assessment Tool (SWAT). The previously developed Fertilizer Emission Scenario Tool for CMAQ (FEST-C), an advanced user interface, integrated EPIC with the WRF model and CMAQ. The FEST-C system, driven by process-based WRF weather simulations, includes atmospheric N additions to agricultural cropland and agricultural cropland contributions to ammonia emissions. This study focuses on integrating the watershed hydrology and water quality model with FEST-C system so that a full multimedia assessment on water quality in large river basins to address impacts of fertilization, meteorology, and atmospheric N deposition on water quality can be achieved. Objectives of this paper are to describe how to expand the previous effort by integrating the SWAT model with the FEST-C (CMAQ/WRF/EPIC) modeling system, as well as to demonstrate application of the Integrated Modeling System (IMS) to the Mississippi River basin (MRB) to simulate streamflow and dissolved N loadings to the Gulf of Mexico (GOM). IMS simulation results generally agree with US Geological Survey (USGS) observations/estimations; the annual simulated streamflow is 218.9 mm and USGS observation is 211.1 mm and the annual simulated dissolved N is 2.1 kg ha−1 and the USGS estimation is 2.8 kg ha−1. Integrating SWAT with the CMAQ/WRF/EPIC modeling system allows for its use within large river basins without losing EPIC's more detailed biogeochemistry processes, which will strengthen the assessment of impacts of future climate scenarios, regulatory and voluntary programs for N oxide air emissions, and land use and land management on N transport and transformation in large river basins.

Riverine export of terrestrially derived carbon represents a key component of the global carbon cycle. In this study we quantify the fate of riverine carbon within the Wuding River catchment on the Chinese Loess Plateau. Export of dissolved organic and inorganic carbon (DOC and DIC) exhibited pronounced spatial and temporal variability. While DOC concentration first presented a downward trend along the river course and then increased in the main-stem river, it showed no significant seasonal differences and was not sensitive to flow dynamics. This likely reflects the predominance of groundwater input over the entire year and its highly stable DOC. DIC concentration in the loess subcatchment is significantly higher than that in the sandy subcatchment, due largely to dissolution of carbonates that are abundant in loess. In addition, bulk particulate organic carbon content (POC%) showed strong seasonal variability with low values in the wet season owing to input of deeper soils by gully erosion. The downstream carbon flux was (7.0 ± 1.9) × 1010 g C yr−1 and dominated by DIC and POC. Total CO2 emissions from water surface were (3.7 ± 0.6) × 1010 g C yr−1. Radiocarbon analysis revealed that the degassed CO2 was 810–1890 years old, indicating the release of old carbon previously stored in soil horizons. Riverine carbon export in the Wuding River catchment has been greatly modified by check dams. Our estimate shows that carbon burial through sediment storage was (7.8 ± 4.1) × 1010 g C yr−1, representing 42 % of the total riverine carbon export from terrestrial ecosystems on an annual basis ((18.5 ± 4.5) × 1010 g C yr−1). Moreover, the riverine carbon export accounted for 16 % of the catchment's net ecosystem production (NEP). It appears that a significant fraction of terrestrial NEP in this arid to semiarid catchment is laterally transported from the terrestrial biosphere to the drainage network.

Human activities are drastically altering water and material flows in river systems across Asia. These anthropogenic perturbations have rarely been linked to the carbon (C) fluxes of Asian rivers that may account for up to 40–50 % of the global fluxes. This review aims to provide a conceptual framework for assessing the human impacts on Asian river C fluxes, along with an update on anthropogenic alterations of riverine C fluxes. Drawing on case studies conducted in three selected rivers (the Ganges, Mekong, and Yellow River) and other major Asian rivers, the review focuses on the impacts of river impoundment and pollution on CO2 outgassing from the rivers draining South, Southeast, and East Asian regions that account for the largest fraction of river discharge and C exports from Asia and Oceania. A critical examination of major conceptual models of riverine processes against observed trends suggests that to better understand altered metabolisms and C fluxes in anthropogenic land-water-scapes, or riverine landscapes modified by human activities, the traditional view of the river continuum should be complemented with concepts addressing spatial and temporal discontinuities created by human activities, such as river impoundment and pollution. Recent booms in dam construction on many large Asian rivers pose a host of environmental problems, including increased retention of sediment and associated C. A small number of studies that measured greenhouse gas (GHG) emissions in dammed Asian rivers have reported contrasting impoundment effects: decreased GHG emissions from eutrophic reservoirs with enhanced primary production vs. increased emissions from the flooded vegetation and soils in the early years following dam construction or from the impounded reaches and downstream estuaries during the monsoon period. These contrasting results suggest that the rates of metabolic processes in the impounded and downstream reaches can vary greatly longitudinally over time as a combined result of diel shifts in the balance between autotrophy and heterotrophy, seasonal fluctuations between dry and monsoon periods, and a long-term change from a leaky post-construction phase to a gradual C sink. The rapid pace of urbanization across southern and eastern Asian regions has dramatically increased municipal water withdrawal, generating annually 120 km3 of wastewater in 24 countries, which comprises 39 % of the global municipal wastewater production. Although municipal wastewater constitutes only 1 % of the renewable surface water, it can disproportionately affect the receiving river water, particularly downstream of rapidly expanding metropolitan areas, resulting in eutrophication, increases in the amount and lability of organic C, and pulse emissions of CO2 and other GHGs. In rivers draining highly populated metropolitan areas, lower reaches and tributaries, which are often plagued by frequent algal blooms and pulsatile CO2 emissions from urban tributaries delivering high loads of wastewater, tended to exhibit higher levels of organic C and the partial pressure of CO2 (pCO2) than less impacted upstream reaches and eutrophic impounded reaches. More field measurements of pCO2, together with accurate flux calculations based on river-specific model parameters, are required to provide more accurate estimates of GHG emissions from the Asian rivers that are now underrepresented in the global C budgets. The new conceptual framework incorporating discontinuities created by impoundment and pollution into the river continuum needs to be tested with more field measurements of riverine metabolisms and CO2 dynamics across variously affected reaches to better constrain altered fluxes of organic C and CO2 resulting from changes in the balance between autotrophy and heterotrophy in increasingly human-modified river systems across Asia and other continents.

The heterogeneous hydrolysis of N2O5 on the surface of deliquescent aerosol leads to HNO3 formation and acts as a major sink of NOx in the atmosphere during night-time. The reaction constant of this heterogeneous hydrolysis is determined by temperature (T), relative humidity (RH), aerosol particle composition, and the surface area concentration (S). However, these parameters were not comprehensively considered in the parameterization of the heterogeneous hydrolysis of N2O5 in previous mass-based 3-D aerosol modelling studies. In this investigation, we propose a sophisticated parameterization (NewN2O5) of N2O5 heterogeneous hydrolysis with respect to T, RH, aerosol particle compositions, and S based on laboratory experiments. We evaluated closure between NewN2O5 and a state-of-the-art parameterization based on a sectional aerosol treatment. The comparison showed a good linear relationship (R = 0.91) between these two parameterizations. NewN2O5 was incorporated into a 3-D fully online coupled model, COSMO–MUSCAT, with the mass-based aerosol treatment. As a case study, we used the data from the HOPE Melpitz campaign (10–25 September 2013) to validate model performance. Here, we investigated the improvement of nitrate prediction over western and central Europe. The modelled particulate nitrate mass concentrations ([NO3−]) were validated by filter measurements over Germany (Neuglobsow, Schmücke, Zingst, and Melpitz). The modelled [NO3−] was significantly overestimated for this period by a factor of 5–19, with the corrected NH3 emissions (reduced by 50 %) and the original parameterization of N2O5 heterogeneous hydrolysis. The NewN2O5 significantly reduces the overestimation of [NO3−] by ∼ 35 %. Particularly, the overestimation factor was reduced to approximately 1.4 in our case study (12, 17–18 and 25 September 2013) when [NO3−] was dominated by local chemical formations. In our case, the suppression of organic coating was negligible over western and central Europe, with an influence on [NO3−] of less than 2 % on average and 20 % at the most significant moment. To obtain a significant impact of the organic coating effect, N2O5, SOA, and NH3 need to be present when RH is high and T is low. However, those conditions were rarely fulfilled simultaneously over western and central Europe. Hence, the organic coating effect on the reaction probability of N2O5 may not be as significant as expected over western and central Europe.

Understanding riverine carbon dynamics is critical for not only better estimates of various carbon fluxes but also evaluating their significance in the global carbon budget. As an important pathway of global land–ocean carbon exchange, the Yangtze River has received less attention regarding its vertical carbon evasion compared with lateral transport. Using long-term water chemistry data, we calculated CO2 partial pressure (pCO2) from pH and alkalinity and examined its spatial and temporal dynamics and the impacts of environmental settings. With alkalinity ranging from 415 to > 3400 µeq L−1, the river waters were supersaturated with dissolved CO2, generally 2–20-fold the atmospheric equilibrium (i.e., 390 µatm). Changes in pCO2 were collectively controlled by carbon inputs from terrestrial ecosystems, hydrological regime, and rock weathering. High pCO2 values were observed spatially in catchments with abundant carbonate presence and seasonally in the wet season when recently fixed organic matter was exported into the river network. In-stream processing of organic matter facilitated CO2 production and sustained the high pCO2, although the alkalinity presented an apparent dilution effect with water discharge. The decreasing pCO2 from the smallest headwater streams through tributaries to the mainstem channel illustrates the significance of direct terrestrial carbon inputs in controlling riverine CO2. With a basin-wide mean pCO2 of 2662 ± 1240 µatm, substantial CO2 evasion from the Yangtze River fluvial network is expected. Future research efforts are needed to quantify the amount of CO2 evasion and assess its biogeochemical implications for watershed-scale carbon cycle. In view of the Yangtze River's relative importance in global carbon export, its CO2 evasion would be significant for global carbon budget.

Abstract A new windblown dust emission treatment was incorporated in the Community Multiscale Air Quality (CMAQ) modeling system. This new model treatment has been built upon previously developed physics‐based parameterization schemes from the literature. A distinct and novel feature of this scheme, however, is the incorporation of a newly developed dynamic relation for the surface roughness length relevant to small‐scale dust generation processes. Through this implementation, the effect of nonerodible elements on the local flow acceleration, drag partitioning, and surface coverage protection is modeled in a physically based and consistent manner. Careful attention is paid in integrating the new windblown dust treatment in the CMAQ model to ensure that the required input parameters are correctly configured. To test the performance of the new dust module in CMAQ, the entire year 2011 is simulated for the continental United States, with particular emphasis on the southwestern United States (SWUS) where windblown dust concentrations are relatively large. Overall, the model shows good performance with the daily mean bias of soil concentrations fluctuating in the range of ±1 µg m−3 for the entire year. Springtime soil concentrations are in quite good agreement (normalized mean bias of 8.3%) with observations, while moderate to high underestimation of soil concentration is seen in the summertime. The latter is attributed to the issue of representing the convective dust storms in summertime. Evaluations against observations for seven elevated dust events in the SWUS indicate that the new windblown dust treatment is capable of capturing spatial and temporal characteristics of dust outbreaks.

The North China Plain (NCP) has become one of the most polluted regions in China, with the rapidly increasing economic growth in the past decades. High concentrations of ambient O3 and aerosol have been observed at urban as well as rural sites in the NCP. Most of the in situ observations of air pollutants have been conducted near the ground so that current knowledge about the vertical distributions of tropospheric O3 and aerosol over the NCP region is still limited. In this study, vertical profiles of O3 and size-resolved aerosol concentrations below 2.5 km were measured in summer 2014 over a rural site in the NCP, using an unmanned aerial vehicle (UAV) equipped with miniature analyzers. In addition, vertical profiles of aerosol scattering property in the lower troposphere and vertical profiles of O3 below 1 km were also observed at the site using a lidar and tethered balloon, respectively. The depths of the mixed layer and residual layer were determined according to the vertical gradients of lidar particle extinction and aerosol number concentration. Average O3 and size-resolved aerosol number concentration in both the mixed and residual layer were obtained from the data observed in seven UAV flights. The results show that during most of the flights the O3 levels above the top of mixed layer were higher than those below. Such a positive gradient in the vertical distribution of O3 makes the residual layer an important source of O3 in the mixed layer, particularly during the morning when the top of mixed layer is rapidly elevated. In contrast to O3, aerosol number concentration was normally higher in the mixed layer than in the residual layer, particularly in the early morning. Aerosol particles were overwhelmingly distributed in the size range 3 vertical profiles over Beijing from the Measurement of Ozone and Water Vapor by Airbus In-Service Aircraft (MOZAIC), a strong increase in O3 can be found at all heights below 2.5 km in the decade from 2004 to 2014, with the largest enhancement of about 41.6 ppb. This indicates that the lower troposphere over the northern part of the NCP has experienced rapidly worsening photochemical pollution. This worsening trend in photochemical pollution deserves more attention in the future.

Sea salt aerosol (SSA) is one of the major components of primary aerosols and has significant impact on the formation of secondary inorganic particles mass on a global scale. In this study, the fully online coupled WRF-Chem model was utilized to evaluate the SSA emission scheme and its influence on the nitrate simulation in a case study in Europe during 10–20 September 2013. Meteorological conditions near the surface, wind pattern and thermal stratification structure were well reproduced by the model. Nonetheless, the coarse-mode (PM1 − 10) particle mass concentration was substantially overestimated due to the overestimation of SSA and nitrate. Compared to filter measurements at four EMEP stations (coastal stations: Bilthoven, Kollumerwaard and Vredepeel; inland station: Melpitz), the model overestimated SSA concentrations by a factor of 8–20. We found that this overestimation was mainly caused by overestimated SSA emissions over the North Sea during 16–20 September. Over the coastal regions, SSA was injected into the continental free troposphere through an “aloft bridge” (about 500 to 1000 m above the ground), a result of the different thermodynamic properties and planetary boundary layer (PBL) structure between continental and marine regions. The injected SSA was further transported inland and mixed downward to the surface through downdraft and PBL turbulence. This process extended the influence of SSA to a larger downwind region, leading, for example, to an overestimation of SSA at Melpitz, Germany, by a factor of ∼ 20. As a result, the nitrate partitioning fraction (ratio between particulate nitrate and the summation of particulate nitrate and gas-phase nitric acid) increased by about 20 % for the coarse-mode nitrate due to the overestimation of SSA at Melpitz. However, no significant difference in the partitioning fraction for the fine-mode nitrate was found. About 140 % overestimation of the coarse-mode nitrate resulted from the influence of SSA at Melpitz. In contrast, the overestimation of SSA inhibited the nitrate particle formation in the fine mode by about 20 % because of the increased consumption of precursor by coarse-mode nitrate formation.

Black carbon (BC) is a dominant absorber in the visible spectrum and a potent factor in climatic effects. Vertical profiles of BC were measured using a micro-aethalometer attached to a tethered balloon during the Vertical Observations of trace Gases and Aerosols (VOGA) field campaign, in summer 2014 at a semirural site in the North China Plain (NCP). The diurnal cycle of BC vertical distributions following the evolution of the mixing layer (ML) was investigated for the first time in the NCP region. Statistical parameters including identified mixing height (Hm) and average BC mass concentrations within the ML (Cm) and in the free troposphere (Cf) were obtained for a selected dataset of 67 vertical profiles. Hm was usually lower than 0.2 km in the early morning and rapidly rose thereafter due to strengthened turbulence. The maximum height of the ML was reached in the late afternoon. The top of a full developed ML exceeded 1 km on sunny days in summer, while it stayed much lower on cloudy days. The sunset triggered the collapse of the ML, and a stable nocturnal boundary layer (NBL) gradually formed. Accordingly, the highest level Cm was found in the early morning and the lowest was found in the afternoon. In the daytime, BC was almost uniformly distributed within the ML and significantly decreased above the ML. During the field campaign, Cm averaged about 5.16 ± 2.49 µg m−3, with a range of 1.12 to 14.49 µg m−3, comparable with observational results in many polluted urban areas such as Milan in Italy and Shanghai in China. As evening approached, BC gradually built up near the surface and exponentially declined with height. In contrast to the large variability found both in Hm and Cm, Cf stayed relatively unaffected through the day. Cf was less than 10 % of the ground level under clean conditions, while it amounted to half of the ground level in some polluted cases. In situ measurements of BC vertical profiles would hopefully have an important implication for accurately estimating direct radiative forcing by BC and improving the retrieval of aerosol optical properties by remote sensing in this region.

The Emission Scenario Projection (ESP) method produces future-year air pollutant emissions for mesoscale air quality modeling applications. We present ESP v2.0, which expands upon ESP v1.0 by spatially allocating future-year non-power sector emissions to account for projected population and land use changes. In ESP v2.0, US Census division-level emission growth factors are developed using an energy system model. Regional factors for population-related emissions are spatially disaggregated to the county level using population growth and migration projections. The county-level growth factors are then applied to grow a base-year emission inventory to the future. Spatial surrogates are updated to account for future population and land use changes, and these surrogates are used to map projected county-level emissions to a modeling grid for use within an air quality model. We evaluate ESP v2.0 by comparing US 12 km emissions for 2005 with projections for 2050. We also evaluate the individual and combined effects of county-level disaggregation and of updating spatial surrogates. Results suggest that the common practice of modeling future emissions without considering spatial redistribution over-predicts emissions in the urban core and under-predicts emissions in suburban and exurban areas. In addition to improving multi-decadal emission projections, a strength of ESP v2.0 is that it can be applied to assess the emissions and air quality implications of alternative energy, population and land use scenarios.

Carbon transport in river systems is an important component of the global carbon cycle. Most rivers of the world act as atmospheric CO2 sources due to high riverine CO2 partial pressure (pCO2). By determining the pCO2 from alkalinity and pH, we investigated its spatial and temporal variation in the Yellow River watershed using historical water chemistry records (1950s–1984) and recent sampling along the mainstem (2011–2012). Except the headwater region where the pCO2 was lower than the atmospheric equilibrium (i.e. 380 μatm), river waters in the remaining watershed were supersaturated with CO2. The average pCO2 for the watershed was estimated at 2810 ± 1985 μatm, which is 7-fold the atmospheric equilibrium. As a result of severe soil erosion and dry climate, waters from the Loess Plateau in the middle reaches had higher pCO2 than that from the upper and lower reaches. From a seasonal perspective, the pCO2 varied from about 200 μatm to > 30 000 μatm with higher pCO2 usually occurring in the dry season and lower pCO2 in the wet season (at 73% of the sampling sites), suggesting the dilution effect of water. While the pCO2 responded exponentially to total suspended solids (TSS) export when the TSS concentration was less than 100 kg m−3, it decreased slightly and remained stable if the TSS concentration exceeded 100 kg m−3. This stable pCO2 is largely due to gully erosion that mobilizes subsoils characterized by low organic carbon for decomposition. In addition, human activities have changed the pCO2 dynamics. Particularly, flow regulation by dams can diversely affect the temporal changes of pCO2, depending on the physiochemical properties of the regulated waters and adopted operation scheme. Given the high pCO2 in the Yellow River waters, large potential for CO2 evasion is expected and warrants further investigation.

Through several years of development, the city of Lhasa has become one of the most populated and urbanized areas on the highest plateau in the world. In the process of urbanization, current and potential air quality issues have been gradually concerned. To investigate the current status of air pollution in Lhasa, various gas pollutants including NOx, CO, SO2, and O3, were continuously measured from June 2012 to May 2013 at an urban site (29.40° N, 91.08° E, 3650 m a.s.l.). The seasonal variations of primary gas pollutants exhibited a peak from November to January with a large variability. High mixing ratios of primary trace gases almost exclusively occurred under low wind speed and showed no distinct dependence on wind direction, implying local urban emissions to be predominant. A comparison of NO2, CO, and SO2 mixing ratios in summer between 1998 and 2012 indicated a significant increase in emissions of these gas pollutants and a change in their intercorrelations, as a result of a substantial growth in the demand of energy consumption using fossil fuels instead of previously widely used biomass. The pronounced diurnal double peaks of primary trace gases in all seasons suggested automobile exhaust to be a major emission source in Lhasa. The secondary gas pollutant O3 displayed an average diurnal cycle of a shallow flat peak for about 4–5 h in the afternoon and a minimum in the early morning. Nighttime O3 was sometimes completely consumed by the high level of NOx. Seasonally, the variations of O3 mixing ratios displayed a low valley in winter and a peak in spring. In autumn and winter, transport largely contributed to the observed O3 mixing ratios, given its dependence on wind speed and wind direction, while in spring and summer photochemistry played an important role. A more efficient buildup of O3 mixing ratios in the morning and a higher peak in the afternoon was found in summer 2012 than in 1998. An enhancement in O3 mixing ratios would be expected in the future and more attention should be given to O3 photochemistry in response to increasing precursor emissions in this area.

Abstract The current study focuses on examining the characteristics of biofuel obtained from the pyrolysis of Madhuca longifolia residues, since the selected forest residue was primarily motivated by its greater volatile matter content. The study used several analytical techniques to describe pyrolysis oil, char, and gas obtained from slow pyrolysis process conducted between 350 and 600 °C in a fixed-bed reactor. Initially, the effect of process temperature on product distribution was assessed to motivate maximum pyrolysis oil yield and found to be 44.2 wt% at pyrolysis temperature of 475 °C, while the yields of char and gas were 22.1 wt% and 33.7 wt%, respectively. In order to determine the suitability of the feedstock, the Madhuca longifolia residues were analyzed by TGA and FT-IR, which revealed that the feedstock could be a feasible option as an energy source. The characterization of pyrolysis oil, char, and gas has been done through various analytical methods like FT-IR, GC-MS, and gas chromatography. The physicochemical characteristics of the pyrolysis oil sample were examined, and the results showed that the oil is a viscous liquid with a lower heating value than conventional diesel. The FT-IR and GC-MS analysis of pyrolysis oil revealed the presence of increased levels of oxygenated chemicals, acids, and phenol derivatives. The findings of the FT-IR analysis of char indicated the existence of aromatic and aliphatic hydrocarbons. The increased carbon content in the char indicated the possibility of using solid fuel. Gas chromatography was used to examine the chemical structure of the pyrolysis gas, and the results showed the existence of combustible elements.

The fungal kingdom is among the most diversified kingdoms on Earth, with estimations of up to 12 million species. However, it remains poorly understood, with only 150 000 fungal species currently described. Given the major ecological role of fungi in ecosystem functioning, these numbers stress the importance of investigating fungal diversity description across different ecosystem types. Here, we explored the spatial distribution of the soil fungal diversity on a broad geographical scale, using the French Soil Quality Monitoring Network that covers the whole French territory (2171 soils sampled along a systematic grid). Fungal alpha diversity was assessed directly from soil DNA using a meta-barcoding approach by targeting the 18S rDNA gene. The total accumulated fungal diversity across France included 136 219 operational taxonomic units (OTUs), i.e., about 1 % of worldwide soil fungal diversity (based on a maximum diversity estimate of 12 million) for a territory representing only 0.3 % of the terrestrial surface on Earth. Based on this dataset, the first extensive map of fungal alpha diversity was drawn and showed a heterogeneous and spatially structured distribution in large biogeographical patterns of 231 km radius for richness (Hill diversity of order 0) and smaller patterns of 36 km radius for dominant fungi (Hill diversity of order 2). As related to other environmental parameters, the spatial distribution of fungal diversity (Hill numbers based on different orders of diversity) was mainly influenced by local filters such as soil characteristics and land management and also by global filters such as climate conditions with various relative influences. Interestingly, cropped soils exhibited the highest pool of fungal diversity relative to forest and vineyard soils. To complement this, soil fungal OTU network interactions were calculated for the different land uses across France. They varied hugely and showed a loss of 75 % of the complexity in crop systems and grasslands compared to forests and up to 83 % in vineyard systems. Overall, our study revealed that a nationwide survey with a high spatial-resolution approach is relevant for deeply investigating the spatial distribution and determinism of soil fungal diversity. Our findings provide novel insights for a better understanding of soil fungal ecology across the 18S rDNA gene and upgrade biodiversity conservation policies by supplying representative repositories dedicated to soil fungi.

Acceptance of insect-containing foods remains low among European consumers. This study aims to explore the factors affecting willingness to consume insects among students in two European countries with different culinary traditions, namely France and Ireland. An online survey was developed and distributed in both countries, with 183 participants (France: n = 103; Ireland: n = 80) included in total. While more participants in France (43.7%) had a positive opinion of entomophagy compared to the ones in Ireland (21.3%), no significant difference was found in their willingness to consume insects for the first time. When given information on the approval of insects as a novel food in Europe, students in France were significantly more willing to consume insects than students in Ireland. For both groups, food neophobia and disgust were impediments to entomophagy. Moreover, males older than 30 yr enrolled in engineering courses, not following a specific diet, more concerned about the environment and health and less about familiarity, culture and religion were the most willing to consume insects. Participants in France and Ireland were more willing to consume insects if they were tasty or disguised (invisible) in another product and not if they were presented in their usual form (‘whole’). This case study shows that entomophagy acceptance is affected by the characteristics of the products, food neophobia, disgust and food choice motives of the consumers, while the impact of information on regulation is country dependent. These findings could be the starting point to guide the development of insect-containing foods acceptable to consumers in Europe.

Introduction In recent decades, there has been extensive research on the association between Autism Spectrum Disorders (ASD) and Eating Disorders (ED), as well as the existence of sensory sensitivity alterations in both diagnostic groups. Objectives The present study aimed to examine the presence of autistic traits in a sample of adult women diagnosed with different ED, and the concurrent role of autistic traits and sensory sensitivity in both their eating disorder symptomatology and their autism-related eating behaviours. Methods Seventy-five women with different ED completed the Eating Attitude Test (EAT-26), the Autism Quotient (AQ), the Ritvo Autism Asperger Diagnostic Scale-Revised (RAADS-R), the Sensory Perception Quotient - Short Form 35 item (SPQ-SF35) and the Swedish Eating Assessment for Autism Spectrum Disorders (SWEAA), which investigates specific eating behaviour related to autism. Results 12% of the sample scored above the cut-off at both the AQ and the RAADS-R, while 68% scored above the cut-off at the RAADS-R only. We found an association between: i) hypersensitivity in the taste domain and ED severity and autistic-like eating behaviours; ii) hypersensitivity in the vision domain and autistic-like eating behaviours; iii) higher autistic traits and ED severity and autistic-like eating behaviours. Conclusions This study confirms the presence of autistic traits in patients with ED and underscores the significance of conducting additional systematical investigations on this topic across all diagnostic categories of ED. It is becoming progressively evident that identifying and measuring the levels of autistic traits in patients with ASD is crucial not only for a better understanding of the causes of these disorders, but also because it would help to tailor specific therapeutic interventions, especially considering the cognitive flexibility issues presented by these patients and the socio-emotional challenges they face. Additionally, this study has laid the foundation for further insights into the relationship between sensory sensitivity and dysfunctional eating behaviours typical of ED and ASD. Disclosure of Interest None Declared

BackgroundNeurocognitive changes occurring after a surgical aortic valve replacement (SAVR) or transcatheter aortic valve implantation (TAVI) procedure for the correction of severe aortic stenosis (AS) have not been widely addressed and, if addressed, have produced conflicting results. The purpose of this study is to identify the pre-procedural neurocognitive pattern and its determinants in a setting of elderly (>65 years) patients with severe AS undergoing SAVR or TAVI and the changes occurring at a 2–3 month follow-up.MethodsThis was a prospective cohort study included in the Italian Registry on Outcomes in Aortic Stenosis Treatment in Elderly Patients. Patients were assessed both before and after (2–3 months) the procedure using the Montreal Cognitive Assessment (MoCA) test. Data on periprocedural demographics, clinical factors, and outcome measures were collected.ResultsBefore the procedure, 70% of the patients demonstrated a MoCA score