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Regional land carbon budgets provide insights into the spatial distribution of the land uptake of atmospheric carbon dioxide and can be used to evaluate carbon cycle models and to define baselines for land-based additional mitigation efforts. The scientific community has been involved in providing observation-based estimates of regional carbon budgets either by downscaling atmospheric CO2 observations into surface fluxes with atmospheric inversions, by using inventories of carbon stock changes in terrestrial ecosystems, by upscaling local field observations such as flux towers with gridded climate and remote sensing fields, or by integrating data-driven or process-oriented terrestrial carbon cycle models. The first coordinated attempt to collect regional carbon budgets for nine regions covering the entire globe in the RECCAP-1 project has delivered estimates for the decade 2000–2009, but these budgets were not comparable between regions due to different definitions and component fluxes being reported or omitted. The recent recognition of lateral fluxes of carbon by human activities and rivers that connect CO2 uptake in one area with its release in another also requires better definitions and protocols to reach harmonized regional budgets that can be summed up to a globe scale and compared with the atmospheric CO2 growth rate and inversion results. In this study, using the international initiative RECCAP-2 coordinated by the Global Carbon Project, which aims to be an update to regional carbon budgets over the last 2 decades based on observations for 10 regions covering the globe with a better harmonization than the precursor project, we provide recommendations for using atmospheric inversion results to match bottom-up carbon accounting and models, and we define the different component fluxes of the net land atmosphere carbon exchange that should be reported by each research group in charge of each region. Special attention is given to lateral fluxes, inland water fluxes, and land use fluxes.

In this study, we present the first combined open and coastal ocean pCO2 mapped monthly climatology (Landschützer et al. (2020), doi:10.25921/qb25-f418, https://www.nodc.noaa.gov/ocads/oceans/MPI-ULB-SOM_FFN_clim.html) constructed from observations collected between 1998 and 2015 extracted from the Surface Ocean CO2 Atlas (SOCAT) database. We combine two neural network-based pCO2 products, one from the open ocean and the other from the coastal ocean, and investigate their consistency along their common overlap areas. While the difference between open and coastal ocean estimates along the overlap area increases with latitude, it remains close to 0 μatm globally. Stronger discrepancies, however, exist on the regional level resulting in differences that exceed 10 % of the climatological mean pCO2, or an order of magnitude larger than the uncertainty from state of the art measurements. This also illustrates the potential of such analysis to inform the measurement community about the locations where additional measurements are essential to better represent the aquatic continuum and improve our understanding of the carbon exchange at the air water interface. A regional analysis further shows that the seasonal carbon dynamics at the coast-open interface are well represented in our climatology. While our combined product is only a first step towards a true representation of both the open ocean and the coastal ocean air-sea CO2 flux in marine carbon budgets, we show it is a feasible task and the present data product already constitutes a valuable tool to investigate and quantify the dynamics of the air-sea CO2 exchange consistently for oceanic regions regardless of its distance to the coast.

Leaching of dissolved organic carbon (DOC) from soils to the river network is an important component of the land carbon (C) budget. At regional to global scales, its significance has been estimated through simple mass budgets, often using multi-year averages of observed fluvial DOC fluxes as proxy of DOC leaching due to the limited availability of observations of the leaching flux itself. This procedure leads to a systematic underestimation of the leaching flux because of the reactivity of DOC during fluvial transport. Moreover, this procedure does not allow to reveal spatio-temporal variability in DOC leaching from soils, which is needed to better understand the drivers of DOC leaching and its impact on the local soil C budget. In this study, we use the land surface model ORCHILEAK to simulate the terrestrial C budget including leaching of DOC from the soil and its subsequent reactive transport through the river network of Europe. The model performance is not only evaluated against the sparse observations of DOC leaching, but also against the more abundant observations of fluxes and reactivity of DOC in rivers, providing further evidence that our simulated DOC leaching fluxes are realistic. The model is then used to simulate the spatio-temporal patterns of DOC leaching across Europe over the period 1972 to 2012, quantifying both the environmental drivers of these patterns as well as the impact of DOC leaching on the land C budget. Over the simulation period, we find that on average 14.3 TgC yr−1 of DOC is leached from land to European rivers, which is only about 0.6 % of the terrestrial net primary production, a fraction about one order of magnitude lower than reported for tropical river networks. Of the DOC leaching, on average 12.3 TgC yr−1 is exported to the coast via the river network, the rest being respired in transit. DOC leaching presents a large seasonal variability, with a maximum occurring in winter and a minimum in summer, except for the Northern most part of Europe where the maximum occurs in spring due to the snow melt. DOC leaching rate is generally lower in warm and dry regions, and higher in cold and wet regions of Europe. Furthermore, runoff, and the ratio between runoff from shallower flow paths vs. deep drainage and groundwater flow, is the main driver of the spatial variation of DOC leaching. Temperature, as a major control of DOC production and decomposition rates in the soils, plays only a secondary role.

Changes in winter and spring temperatures have been widely used to explain the diverse responses of spring phenology to climate change. However, our understanding of their respective roles remain incomplete. Using >300,000 in situ observations of leaf unfolding date (LUD) in Europe, we show that the advancement of LUD since 1950 is due both to accelerated spring thermal accumulation and changes in winter chilling which explain 61% and 39% of the LUD shifts, respectively. Winter warming did not substantially retard the releasing of bud dormancy, but increased the thermal requirement to reach leaf unfolding. The increase of thermal requirement and decreased efficiency of spring warming on accelerating thermal accumulation partly explained the temporally (1950s-2010s) decreasing response of LUD to warming. Our study stresses the need to better assess the antagonistic and heterogeneous effects of winter and spring warming on leaf phenology, which is key to projection of future vegetation-climate feedbacks.

Accurate monitoring of vegetation stress is required for better modelling and forecasting of primary production, in a world where heatwaves and droughts are expected to become increasingly prevalent. Variability in formaldehyde (HCHO) concentrations in the troposphere is dominated by local emissions of short-lived biogenic (BVOC) and pyrogenic volatile organic compounds. BVOCs are emitted by plants in a rapid protective response to abiotic stress, mediated by the energetic status of leaves (the excess of reducing power when photosynthetic light and dark reactions are decoupled, as occurs when stomata close in response to water stress). Emissions also increase exponentially with leaf temperature. New analytical methods for the detection of spatiotemporally contiguous extremes in remote-sensing data are applied here to satellite-derived atmospheric HCHO columns. BVOC emissions are shown to play a central role in the formation of the largest positive HCHO anomalies. Although vegetation stress can be captured by various remotely sensed quantities, spaceborne HCHO emerges as the most consistent recorder of vegetation responses to the largest climate extremes, especially in forested regions.

Past century increases in terrigenous N and P inputs to the ocean due to industrialization, agricultural practices and wastewater have been reported to have dramatic consequences for ecosystems in various coastal regions. Yet, the impacts of increased nutrient inputs through river transports and atmospheric deposition on the coastal and open ocean carbon cycle have yet to be quantitatively investigated at the global scale. To address this gap of knowledge, we enhanced the ocean biogeochemical model HAMOCC at a horizontal resolution of around 0.4° in order to improve the representation of temporal changes of riverine fluxes and of coastal ocean dynamics in the model. Through a series of simulations with differing model forcings, we isolated individual effects arising from (1) increasing atmospheric CO2 levels, (2) a changing physical climate and (3) alterations in oceanic inputs of terrigenous P and N inputs, all over the 1905 to 2010 period. Our results indicate a strong response of the coastal ocean ecosystem to increased terrestrial nutrient inputs, which induce the global coastal Net Primary Production (NPP) to increase by 14% over the simulation time span. This eutrophication signal is, furthermore, partly exported to the open ocean, which undergoes an increase in NPP of 1.75 Pg C yr-1, or 4 % in relative terms, in the simulations, owing to the cross-shelf export of 33-46% of the anthropogenic P and N inputs to the coastal ocean. As a whole, increased P and N inputs lead to an overall global ocean NPP rise of around 2.15 Pg C yr-1, or 5% (combined coastal and open ocean). This net increase attributed to land-ocean couplings exceeds the simulated global oceanic NPP decrease of 4 % associated with stronger upper ocean thermal stratification over the time span, a feedback that been under stronger scrutiny in published literature. Our results suggest that increased riverine nutrient concentrations due to anthropogenic activities may also have substantial impacts for ecosystems in the open ocean, in contrary to what was assumed until now, although this is dependent on the rate of transfer of the nutrients from the coastal to the open ocean.

The spatio-temporal variability and the underlying drivers of the carbon dioxide (CO2) exchange at the air-water interface (FCO2) of the global coastal ocean are still poorly understood and their quantification remains highly uncertain. Here, we present an analysis of the spatial and seasonal variability of FCO2 using a high-resolution (0.25 degree) monthly climatology (1998-2015 period) for coastal sea surface partial pressure in CO2 (pCO2), globally.Overall, a clear latitudinal pattern emerges from our analysis regarding sources/sinks distribution of atmospheric CO2 and we find that in most regions, annual mean CO2 flux densities are comparable in sign and magnitude to those of the adjacent open ocean except for river dominated systems. Globally, coastal regions act as a CO2 sink with a more intense uptake occurring in summer because of the disproportionate influence of high latitude coastal seas in the Northern Hemisphere. The majority of the coastal seasonal FCO2 variations stems from the air-sea pCO2 gradient, although changes in wind speed and sea-ice cover can also be significant regionally. To investigate further the drivers of the spatio-seasonal variability, our observation-based pCO2 climatology is used in conjunction with global ocean biogeochemistry model MOM6-COBALT. The model outputs allow us to quantify the respective contributions of thermal effects, biology, and non-thermal physical processes (circulation and freshwater inputs) to seasonal variations in coastal pCO2. Generally, biological activity is the dominant driver of the pCO2 seasonal variability in temperate and high latitudes while thermal and non-thermal physical processes dominate in low latitudes.

Resolving regional carbon budgets is critical for informing land-based mitigation policy. For nine regions covering nearly the whole globe, we collected inventory estimates of carbon-stock changes complemented by satellite estimates of biomass changes where inventory data are missing. The net land–atmospheric carbon exchange (NEE) was calculated by taking the sum of the carbon-stock change and lateral carbon fluxes from crop and wood trade, and riverine-carbon export to the ocean. Summing up NEE from all regions, we obtained a global ‘bottom-up’ NEE for net land anthropogenic CO2 uptake of –2.2 ± 0.6 PgC yr−1 consistent with the independent top-down NEE from the global atmospheric carbon budget during 2000–09. This estimate is so far the most comprehensive global bottom-up carbon budget accounting, which set up an important milestone for global carbon-cycle studies. By decomposing NEE into component fluxes, we found that global soil heterotrophic respiration amounts to a source of CO2 of 39 PgC yr−1 with an interquartile of 33–46 PgC yr−1—a much smaller portion of net primary productivity than previously reported., info:eu-repo/semantics/published

International audience; We synthesized N2O emissions over North America using 17 bottom-up (BU) estimates from 1980–2016 and five top-down (TD) estimates from 1998 to 2016. The BU-based total emission shows a slight increase owing to U.S. agriculture, while no consistent trend is shown in TD estimates. During 2007–2016, North American N2O emissions are estimated at 1.7 (1.0–3.0) Tg N yr−1 (BU) and 1.3 (0.9–1.5) Tg N yr−1 (TD). Anthropogenic emissions were twice as large as natural fluxes from soil and water. Direct agricultural and industrial activities accounted for 68% of total anthropogenic emissions, 71% of which was contributed by the U.S. Our estimates of U.S. agricultural emissions are comparable to the EPA greenhouse gas (GHG) inventory, which includes estimates from IPCC tier 1 (emission factor) and tier 3 (process-based modeling) approaches. Conversely, our estimated agricultural emissions for Canada and Mexico are twice as large as the respective national GHG inventories.Nitrous oxide (N2O) is the third most important greenhouse gase (GHG) after CO2 and CH4 causing global warming. Among world regions, North America (defined herein as U.S., Canada, and Mexico) is the second largest source of N2O emissions globally, and previous source estimates for this region vary widely. This study aims to provide a comprehensive N2O assessment over North America including all available estimates based on a number of approaches. We report total emissions, and emissions from four anthropogenic source sectors, over the past four decades. Agriculture and industry are two major N2O sources in North America. Our results show a minor increase in the total N2O emission due to agricultural trends in the U.S. Our bottom-up estimate of U.S. agricultural N2O emissions are close to those in the EPA national GHG inventory that includes both empirical and model results. The high consistency suggests the need to take process-based modeling results into account for future national GHG inventories.

The contribution of continental shelves to the marine carbon cycle is still poorly understood. Their preindustrial state is, for one, essentially unknown, which strongly limits the quantitative assessment of their anthropogenic perturbation. To date, approaches developed to investigate and quantify carbon fluxes on continental shelves have strongly simplified their physical and biogeochemical features. In this study, we enhance the global ocean biogeochemistry model HAMburg Ocean Carbon Cycle by explicitly representing riverine loads of carbon and nutrients, as well as improving the representation of organic matter dynamics in the coastal ocean. Our simulations, at a resolution of similar to 0.4 degrees, reveal a globally averaged shelf water residence time (RT) of 12-17 months, which is much shorter than the global RTs previously assumed in benchmark studies (>4 years). This shorter global RT, induced primarily through outer shelf regions with large oceanic inflows, promotes an efficient offshore transport of terrestrial and marine organic carbon (0.44 PgCyr(-1)) and a dissolved inorganic carbon sink from the organic cycling of carbon on the global shelf (net ecosystem productivity [NEP] equal to +0.20 PgCyr(-1)). In turn, this autotrophic state of continental shelves contributes to a weak global preindustrial sink of atmospheric CO2 (0.04 PgCyr(-1)), dominated by extensive regions with large oceanic inflows and positive NEPs, such as the Patagonian shelf, the East China Sea and the outer North Sea. The contemporary global shelf CO2 uptake of 0.15 PgCyr(-1) furthermoresuggests that the anthropogenic CO2 uptake (0.11 PgCyr(-1)) on the global continental shelf is less efficient with respect to the open ocean.

The implications of climate change and other human perturbations on the oceanic carbon cycle are still associated with large uncertainties. Global-scale modelling studies are essential to investigate anthropogenic perturbations of oceanic carbon fluxes but, until now, they have not considered the impacts of temporal changes in riverine and atmospheric inputs of P and N on the marine net biological productivity (NPP) and air–sea CO2 exchange (FCO2). To address this, we perform a series of simulations using an enhanced version of the global ocean biogeochemistry model HAMOCC to isolate effects arising from (1) increasing atmospheric CO2 levels, (2) a changing physical climate and (3) alterations in inputs of terrigenous P and N on marine carbon cycling over the 1905–2010 period. Our simulations reveal that our first-order approximation of increased terrigenous nutrient inputs causes an enhancement of 2.15 Pg C year−1 of the global marine NPP, a relative increase of +5% over the simulation period. This increase completely compensates the simulated NPP decrease as a result of increased upper ocean stratification of −3% in relative terms. The coastal ocean undergoes a global relative increase of 14% in NPP arising largely from increased riverine inputs, with regional increases exceeding 100%, for instance on the shelves of the Bay of Bengal. The imprint of enhanced terrigenous nutrient inputs is also simulated further offshore, inducing a 1.75 Pg C year−1 (+4%) enhancement of the NPP in the open ocean. This finding implies that the perturbation of carbon fluxes through coastal eutrophication may extend further offshore than that was previously assumed. While increased nutrient inputs are the largest driver of change for the CO2 uptake at the regional scale and enhance the global coastal ocean CO2 uptake by 0.02 Pg C year−1, they only marginally affect the FCO2 of the open ocean over our study's timeline., SCOPUS: ar.j, info:eu-repo/semantics/published

Reliable quantification of the sources and sinks of atmospheric carbon dioxide (CO 2 ), including that of their trends and uncertainties, is essential to monitoring the progress in mitigating anthropogenic emissions under the Kyoto Protocol and the Paris Agreement. This study provides a consolidated synthesis of estimates for all anthropogenic and natural sources and sinks of CO 2 for the European Union and UK (EU27 + UK), derived from a combination of state-of-the-art bottom-up (BU) and top-down (TD) data sources and models. Given the wide scope of the work and the variety of datasets involved, this study focuses on identifying essential questions which need to be answered to properly understand the differences between various datasets, in particular with regards to the less-well-characterized fluxes from managed ecosystems. The work integrates recent emission inventory data, process-based ecosystem model results, data-driven sector model results and inverse modeling estimates over the period 1990–2018. BU and TD products are compared with European national greenhouse gas inventories (NGHGIs) reported under the UNFCCC in 2019, aiming to assess and understand the differences between approaches. For the uncertainties in NGHGIs, we used the standard deviation obtained by varying parameters of inventory calculations, reported by the member states following the IPCC Guidelines. Variation in estimates produced with other methods, like atmospheric inversion models (TD) or spatially disaggregated inventory datasets (BU), arises from diverse sources including within-model uncertainty related to parameterization as well as structural differences between models. In comparing NGHGIs with other approaches, a key source of uncertainty is that related to different system boundaries and emission categories (CO 2 fossil) and the use of different land use definitions for reporting emissions from land use, land use change and forestry (LULUCF) activities (CO 2 land). At the EU27 + UK level, the NGHGI (2019) fossil CO 2 emissions (including cement production) account for 2624 Tg CO 2 in 2014 while all the other seven bottom-up sources are consistent with the NGHGIs and report a mean of 2588 ( ± 463 Tg CO 2 ). The inversion reports 2700 Tg CO 2 ( ± 480 Tg CO 2 ), which is well in line with the national inventories. Over 2011–2015, the CO 2 land sources and sinks from NGHGI estimates report −90 Tg C yr −1 ± 30 Tg C yr −1 while all other BU approaches report a mean sink of −98 Tg C yr −1 ( ± 362 Tg of C from dynamic global vegetation models only). For the TD model ensemble results, we observe a much larger spread for regional inversions (i.e., mean of 253 Tg C yr −1 ± 400 Tg C yr −1 ). This concludes that (a) current independent approaches are consistent with NGHGIs and (b) their uncertainty is too large to allow a verification because of model differences and probably also because of the definition of “CO 2 flux” obtained from different approaches. The referenced datasets related to figures are visualized at https://doi.org/10.5281/zenodo.4626578 (Petrescu et al., 2020a).

Reliable quantification of the sources and sinks of greenhouse gases, together with trends and uncertainties, is essential to monitoring the progress in mitigating anthropogenic emissions under the Paris Agreement. This study provides a consolidated synthesis of CH4 and N2O emissions with consistently derived state-of-the-art bottom-up (BU) and top-down (TD) data sources for the European Union and UK (EU27 + UK). We integrate recent emission inventory data, ecosystem process-based model results and inverse modeling estimates over the period 1990-2017. BU and TD products are compared with European national greenhouse gas inventories (NGHGIs) reported to the UN climate convention UNFCCC secretariat in 2019. For uncertainties, we used for NGHGIs the standard deviation obtained by varying parameters of inventory calculations, reported by the member states (MSs) following the recommendations of the IPCC Guidelines. For atmospheric inversion models (TD) or other inventory datasets (BU), we defined uncertainties from the spread between different model estimates or model-specific uncertainties when reported. In comparing NGHGIs with other approaches, a key source of bias is the activities included, e.g. anthropogenic versus anthropogenic plus natural fluxes. In inversions, the separation between anthropogenic and natural emissions is sensitive to the geospatial prior distribution of emissions. Over the 2011-2015 period, which is the common denominator of data availability between all sources, the anthropogenic BU approaches are directly comparable, reporting mean emissions of 20.8 Tg CH4 yr-1 (EDGAR v5.0) and 19.0 Tg CH4 yr-1 (GAINS), consistent with the NGHGI estimates of 18.9 ± 1.7 Tg CH4 yr-1. The estimates of TD total inversions give higher emission estimates, as they also include natural emissions. Over the same period regional TD inversions with higher-resolution atmospheric transport models give a mean emission of 28.8 Tg CH4 yr-1. Coarser-resolution global TD inversions are consistent with regional TD inversions, for global inversions with GOSAT satellite data (23.3 Tg CH4 yr-1) and surface network (24.4 Tg CH4 yr-1). The magnitude of natural peatland emissions from the JSBACH-HIMMELI model, natural rivers and lakes emissions, and geological sources together account for the gap between NGHGIs and inversions and account for 5.2 Tg CH4 yr-1. For N2O emissions, over the 2011-2015 period, both BU approaches (EDGAR v5.0 and GAINS) give a mean value of anthropogenic emissions of 0.8 and 0.9 Tg N2O yr-1, respectively, agreeing with the NGHGI data (0.9 ± 0.6 Tg N2O yr-1). Over the same period, the average of the three total TD global and regional inversions was 1.3 ± 0.4 and 1.3 ± 0.1 Tg N2O yr-1, respectively. The TD and BU comparison method defined in this study can be operationalized for future yearly updates for the calculation of CH4 and N2O budgets both at the EU+UK scale and at the national scale. The referenced datasets related to figures are visualized at. (Petrescu et al. 2020b)., SCOPUS: re.j, info:eu-repo/semantics/published

Global water erosion strongly affects the terrestrial carbon balance. However, this process is currently ignored by most global land surface models (LSMs) that are used to project the responses of terrestrial carbon storage to climate and land use changes. One of the main obstacles to implement erosion processes in LSMs is the high spatial resolution needed to accurately represent the effect of topography on soil erosion and sediment delivery to rivers. In this study, we present an upscaling scheme for including erosion‐induced lateral soil organic carbon (SOC) movements into the ORCHIDEE LSM. This upscaling scheme integrates information from high‐resolution (3″) topographic and soil erodibility data into a LSM forcing file at 0.5° spatial resolution. Evaluation of our model for the Rhine catchment indicates that it reproduces well the observed spatial and temporal (both seasonal and interannual) variations in river runoff and the sediment delivery from uplands to the river network. Although the average annual lateral SOC flux from uplands to the Rhine River network only amounts to 0.5% of the annual net primary production and 0.01% of the total SOC stock in the whole catchment, SOC loss caused by soil erosion over a long period (e.g., thousands of years) has the potential to cause a 12% reduction in the simulated equilibrium SOC stocks. Overall, this study presents a promising approach for including the erosion‐induced lateral carbon flux from the land to aquatic systems into LSMs and highlights the important role of erosion processes in the terrestrial carbon balance., Key Points We presented an upscaling scheme for including erosion‐induced lateral soil and carbon transfers into a global land surface modelOur model is a useful tool to estimate the impacts of climate and land cover changes on erosion‐induced soil carbon loss at large scaleModel application for the Rhine basin demonstrates that erosion‐induced soil carbon losses substantially reduce soil carbon stocks

Terrestrial ecosystems absorb, at present, about one-fourth of anthropogenic CO2 emissions, which is accumulating in the carbon (C) stocks of vegetation and soils. Land-surface models are used to project the 21st century evolution of this CO2 sink, which mitigates the expected increase in atmospheric CO2 concentration and, thus, climate change. However, classical land-surface models neglect that a fraction of the anthropogenic C absorbed by terrestrial ecosystems is not accumulating on land but is instead exported through the river network. Using the Amazon basin as a case study and a novel land-surface model that represents C exports through rivers, we prove that classical land-surface models such as those used for the Assessment Reports of the IPCC underestimate the CO2 uptake by terrestrial ecosystems and overestimate the amount of anthropogenic C sequestered within vegetation and soils. We provide reasons justifying that similar biases are to be expected at global scale., SCOPUS: ar.j, info:eu-repo/semantics/published

In this second part of a two-part study, we performed a simulation of the carbon and water budget of the Lena catchment with the land surface model ORCHIDEE MICT-LEAK, enabled to simulate dissolved organic carbon (DOC) production in soils and its transport and fate in high-latitude inland waters. The model results are evaluated for their ability to reproduce the fluxes of DOC and carbon dioxide (CO2) along the soil-inland-water continuum and the exchange of CO2 with the atmosphere, including the evasion outgassing of CO2 from inland waters. We present simulation results over the years 1901-2007 and show that the model is able to broadly reproduce observed state variables and their emergent properties across a range of interacting physical and biogeochemical processes. These include (1) net primary production (NPP), respiration and riverine hydrologic amplitude, seasonality, and inter-annual variation; (2) DOC concentrations, bulk annual flow, and their volumetric attribution at the sub-catchment level; (3) high headwater versus downstream CO2 evasion, an emergent phenomenon consistent with observations over a spectrum of high-latitude observational studies. These quantities obey emergent relationships with environmental variables like air temperature and topographic slope that have been described in the literature. This gives us confidence in reporting the following additional findings: of the ĝ'1/434TgCyr-1 left over as input to soil matter after NPP is diminished by heterotrophic respiration, 7TgCyr-1 is leached and transported into the aquatic system. Of this, over half (3.6TgCyr-1) is evaded from the inland water surface back into the atmosphere and the remainder (3.4TgCyr-1) flushed out into the Arctic Ocean, mirroring empirically derived studies. These riverine DOC exports represent ĝ'1/41.5% of NPP. DOC exported from the floodplains is dominantly sourced from recent more "labile" terrestrial production in contrast to DOC leached from the rest of the watershed with runoff and drainage, which is mostly sourced from recalcitrant soil and litter. All else equal, both historical climate change (a spring-summer warming of 1.8ĝ' C over the catchment) and rising atmospheric CO2 (+85.6ppm) are diagnosed from factorial simulations to contribute similar significant increases in DOC transport via primary production, although this similarity may not hold in the future., SCOPUS: ar.j, info:eu-repo/semantics/published

In contrast to the open ocean, the sources and sinks for atmospheric carbon dioxide (CO2) in the coastal seas are poorly constrained and understood. Here we address this knowledge gap by analyzing the spatial and temporal variability of the coastal air-sea flux of CO2 (FCO2) using a recent high-resolution (0.25°) monthly climatology for coastal sea surface partial pressure in CO2 (pCO2). Coastal regions are characterized by CO2 sinks at temperate and high latitudes and by CO2 sources at low latitude and in the tropics, with annual mean CO2 flux densities comparable in magnitude and pattern to those of the adjacent open ocean with the exception of river-dominated systems. The seasonal variations in FCO2 are large, often exceeding 2 mol C m−2 year−1, a magnitude similar to the variations exhibited across latitudes. The majority of these seasonal variations stems from the air-sea pCO2 difference, although changes in wind speed and sea ice cover can also be significant regionally. Globally integrated, the coastal seas act currently as a CO2 sink of −0.20 ± 0.02 Pg C year−1, with a more intense uptake occurring in summer because of the disproportionate influence of high-latitude shelves in the Northern Hemisphere. Combined with estimates of the carbon sinks in the open ocean and the Arctic, this gives for the global ocean, averaged over the 1998 to 2015 period an annual net CO2 uptake of −1.7 ± 0.3 Pg C year−1., SCOPUS: ar.j, info:eu-repo/semantics/published

We present the first version of OMEN-SED (Organic Matter ENabled SEDiment model), a new, onedimensional analytical early diagenetic model resolving organic matter cycling and the associated biogeochemical dynamics in marine sediments designed to be coupled to Earth system models. OMEN-SED explicitly describes organic matter (OM) cycling and the associated dynamics of the most important terminal electron acceptors (i.e. O2, NO3, SO4) and methane (CH4), related reduced substances (NH4, H2S), macronutrients (PO4) and associated pore water quantities (ALK, DIC). Its reaction network accounts for the most important primary and secondary redox reactions, equilibrium reactions, mineral dissolution and precipitation, as well as adsorption and desorption processes associated with OM dynamics that affect the dissolved and solid species explicitly resolved in the model. To represent a redox-dependent sedimentary P cycle we also include a representation of the formation and burial of Fe-bound P and authigenic Ca-P minerals. Thus, OMEN-SED is able to capture the main features of diagenetic dynamics in marine sediments and therefore offers similar predictive abilities as a complex, numerical diagenetic model. Yet, its computational efficiency allows for its coupling to global Earth system models and therefore the investigation of coupled global biogeochemical dynamics over a wide range of climate-relevant timescales. This paper provides a detailed description of the new sediment model, an extensive sensitivity analysis and an evaluation of OMEN-SED's performance through comprehensive comparisons with observations and results from a more complex numerical model. We find that solid-phase and dissolved pore water profiles for different ocean depths are reproduced with good accuracy and simulated terminal electron acceptor fluxes fall well within the range of globally observed fluxes. Finally, we illustrate its application in an Earth system model framework by coupling OMEN-SED to the Earth system model cGENIE and tune the OM degradation rate constants to optimise the fit of simulated benthic OM contents to global observations. We find that the simulated sediment characteristics of the coupled model framework, such as OM degradation rates, oxygen penetration depths and sediment-water interface fluxes, are generally in good agreement with observations and in line with what one would expect on a global scale. Coupled to an Earth system model, OMENSED is thus a powerful tool that will not only help elucidate the role of benthic-pelagic exchange processes in the evolution and the termination of a wide range of climate events, but will also allow for a direct comparison of model output with the sedimentary record - the most important climate archive on Earth., SCOPUS: ar.j, info:eu-repo/semantics/published

Sediments were sampled at nine stations on a transect across a 7–10 m thick Holocene mud layer in Aarhus Bay, Denmark, to investigate the linkages between CH 4 dynamics and the rate and depth distribution of organic matter degradation. High-resolution sulfate reduction rates determined by tracer experiments ( 35 S-SRR) decreased by several orders of magnitude down through the mud layer. The rates showed a power law dependency on sediment age: SRR (nmol cm −3 d −1 ) = 10 6.18 × Age −2.17 . The rate data were used to independently quantify enhanced SO 4 2− transport by bioirrigation. Field data (SO 4 2– , TCO 2 , T 13 CO 2 , NH 4 + and CH 4 concentrations) could be simulated with a reaction-transport model using the derived bioirrigation rates and assuming that the power law was continuous into the methanogenic sediments below the sulfate-methane transition zone (SMTZ). The model predicted an increase in anaerobic organic carbon mineralization rates across the transect from 2410 to 3540 nmol C cm −2 d −1 caused by an increase in the sediment accumulation rate. Although methanogenesis accounted for only ∼1% of carbon mineralization, a large relative increase in methanogenesis along the transect led to a considerable shallowing of the SMTZ from 428 to 257 cm. Methane gas bubbles appeared once a threshold in the sedimentation accumulation rate was surpassed. The 35 S-measured SRR data indicated active sulfate reduction throughout the SO 4 2− zone whereas quasi-linear SO 4 2− gradients over the same zone indicated insignificant sulfate reduction. This apparent inconsistency, observed at all stations, was reconciled by considering the transport of SO 4 2− into the sediment by bioirrigation, which accounted for 94 ± 2% of the total SO 4 2− flux across the sediment-water interface. The SRR determined from the quasi-linear SO 4 2− gradients were two orders of magnitude lower than measured rates. We conclude that models solely based on SO 4 2− concentration gradients will not capture high SRRs at the top of the sulfate reduction zone if they do not properly account for (i) SO 4 2− influx by bioirrigation, and/or (ii) the continuity of organic matter reactivity with sediment depth or age.

The river‐floodplain network plays an important role in the carbon (C) cycle of the Amazon basin, as it transports and processes a significant fraction of the C fixed by terrestrial vegetation, most of which evades as CO2 from rivers and floodplains back to the atmosphere. There is empirical evidence that exceptionally dry or wet years have an impact on the net C balance in the Amazon. While seasonal and interannual variations in hydrology have a direct impact on the amounts of C transferred through the river‐floodplain system, it is not known how far the variation of these fluxes affects the overall Amazon C balance. Here, we introduce a new wetland forcing file for the ORCHILEAK model, which improves the representation of floodplain dynamics and allows us to closely reproduce data‐driven estimates of net C exports through the river–floodplain network. Based on this new wetland forcing and two climate forcing datasets, we show that across the Amazon, the percentage of net primary productivity (NPP) lost to the river–floodplain system is highly variable at the interannual timescale, and wet years fuel aquatic CO2 evasion. However, at the same time overall net ecosystem productivity (NEP) and C sequestration are highest during wet years, partly due to reduced decomposition rates in water‐logged floodplain soils. It is years with the lowest discharge and floodplain inundation, often associated with El Nino events, that have the lowest NEP and the highest total (terrestrial plus aquatic) CO2 emissions back to atmosphere. Furthermore, we find that aquatic C fluxes display greater variation than terrestrial C fluxes, and that this variation significantly dampens the interannual variability in NEP of the Amazon basin. These results call for a more integrative view of the C fluxes through the vegetation‐soil‐river‐floodplain continuum, which directly places aquatic C fluxes into the overall C budget of the Amazon basin.

Natural lakes and reservoirs are important, yet not well constrained sources of greenhouse gasses to the atmosphere. In particular for N2O emissions, a huge variability is observed in the few, observation‐driven flux estimates that have been published so far. Recently, a process‐based, spatially explicit model has been used to estimate global N2O emissions from more than 6,000 reservoirs based on nitrogen (N) and phosphorous inflows and water residence time. Here, we extend the model to a dataset of 1.4 million standing water bodies comprising natural lakes and reservoirs. For validation, we normalized the simulated N2O emissions by the surface area of each water body and compared them against regional averages of N2O emission rates taken from the literature or estimated based on observed N2O concentrations. We estimate that natural lakes and reservoirs together emit 4.5±2.9 Gmol N2O‐N yr‐1 globally. Our global scale estimate falls in the far lower end of existing, observation‐driven estimates. Natural lakes contribute only about half of this flux, although they contribute 91% of the total surface area of standing water bodies. Hence, the mean N2O emission rates per surface area are substantially lower for natural lakes than for reservoirs with 0.8±0.5 mmol N m‐2yr‐1 vs. 9.6±6.0 mmol N m‐2yr‐1, respectively. This finding can be explained by on average lower external N inputs to natural lakes. We conclude that upscaling based estimates, which do not distinguish natural lakes from reservoirs, are prone to important biases. Funding agencies: European UnionEuropean Union (EU) [776810]; Swedish Research Council VRSwedish Research Council; Swedish Research Council FORMASSwedish Research CouncilSwedish Research Council Formas; European Research Council (ERC Grant)European Research Council (ERC) Accepted version on author's personal web page https://liu.se/dfsmedia/dd35e243dfb7406993c1815aaf88a675/35054-source/options/download/natural-lakes

This study presents the first regional application of the generic estuarine reactive-transport model C-GEM (Carbon-Generic Estuary Model) that is here combined with high-resolution databases to produce a carbon and CO2 budget for all tidal estuaries discharging into the North Sea. Steady-state simulations are performed for yearly-averaged conditions to quantify the carbon processing in the six main tidal estuaries Elbe, Ems, Humber, Scheldt, Thames, and Weser, which show contrasted physical and biogeochemical dynamics and contribute the most to the regional filter. The processing rates derived from these simulations are then extrapolated to the riverine carbon loads of all the other North Sea catchments intercepted by smaller tidal estuarine systems. The Rhine-Meuse estuarine system is also included in the carbon budget and overall, we calculate that the export of organic and inorganic carbon from tidal estuaries to the North sea amounts to 44 and 409 Gmol C yr−1, respectively, while 41 Gmol C are lost annually through CO2 outgassing. The carbon is mostly exported from the estuaries in its inorganic form (>90%), a result that reflects the low organic/inorganic carbon ratio of the riverine waters, as well as the very intense decomposition of organic carbon within the estuarine systems. Our calculations also reveal that with a filtering capacity of 15% for total carbon, the contribution of estuaries to the CO2 outgassing is relatively small. Organic carbon dynamics is dominated by heterotrophic degradation, which also represents the most important contribution to the estuarine CO2 evasion. Nitrification only plays a marginal role in the CO2 dynamics, while the contribution of riverine oversaturated waters to the CO2 outgassing is generally significant and strongly varies across systems.

Nitrous oxide (N2 O) emissions from inland waters remain a major source of uncertainty in global greenhouse gas budgets. N2 O emissions are typically estimated using emission factors (EFs), defined as the proportion of the terrestrial nitrogen (N) load to a water body that is emitted as N2 O to the atmosphere. The Intergovernmental Panel on Climate Change (IPCC) has proposed EFs of 0.25% and 0.75%, though studies have suggested that both these values are either too high or too low. In this work, we develop a mechanistic modeling approach to explicitly predict N2 O production and emissions via nitrification and denitrification in rivers, reservoirs and estuaries. In particular, we introduce a water residence time dependence, which kinetically limits the extent of denitrification and nitrification in water bodies. We revise existing spatially explicit estimates of N loads to inland waters to predict both lumped watershed and half-degree grid cell emissions and EFs worldwide, as well as the proportions of these emissions that originate from denitrification and nitrification. We estimate global inland water N2 O emissions of 10.6-19.8GmolNyear-1 (148-277GgNyear-1 ), with reservoirs producing most N2 O per unit area. Our results indicate that IPCC EFs are likely overestimated by up to an order of magnitude, and that achieving the magnitude of the IPCC's EFs is kinetically improbable in most river systems. Denitrification represents the major pathway of N2 O production in river systems, whereas nitrification dominates production in reservoirs and estuaries.

It has been speculated that the partial pressure of carbon dioxide (pCO2) in shelf waters may lag the rise in atmospheric CO2. Here, we show that this is the case across many shelf regions, implying a tendency for enhanced shelf uptake of atmospheric CO2. This result is based on analysis of long-term trends in the air–sea pCO2 gradient (ΔpCO2) using a global surface ocean pCO2 database spanning a period of up to 35 years. Using wintertime data only, we find that ΔpCO2 increased in 653 of the 825 0.5° cells for which a trend could be calculated, with 325 of these cells showing a significant increase in excess of +0.5 μatm yr−1 (p, 0, SCOPUS: ar.j, info:eu-repo/semantics/published

CO2 evasion from rivers (FCO2) is an important component of the global carbon budget. Here we present the first global maps of CO2 partial pressures (pCO2) in rivers of stream orders 3 and higher and the resulting FCO2 at 0.5° resolution constructed with a statistical model. A geographic information system based approach is used to derive a pCO2 prediction function trained on data from 1182 sampling locations. While data from Asia and Africa are scarce and the training data set is dominated by sampling locations from the Americas, Europe, and Australia, the sampling locations cover the full spectrum from high to low latitudes. The predictors of pCO2 are net primary production, population density, and slope gradient within the river catchment as well as mean air temperature at the sampling location (r2 = 0.47). The predicted pCO2 map was then combined with spatially explicit estimates of stream surface area Ariver and gas exchange velocity k calculated from published empirical equations and data sets to derive the FCO2 map. Using Monte Carlo simulations, we assessed the uncertainties of our estimates. At the global scale, we estimate an average river pCO2 of 2400 (2019-2826) μatm and a FCO2 of 650 (483-846) Tg C yr-1 (5th and 95th percentiles of confidence interval). Our global CO2 evasion is substantially lower than the recent estimate of 1800 Tg C yr-1 although the training set of pCO2 is very similar in both studies, mainly due to lower tropical pCO2 estimates in the present study. Our maps reveal strong latitudinal gradients in pCO2, Ariver, and FCO2. The zone between 10°N and 10°S contributes about half of the global CO2 evasion. Collection of pCO2 data in this zone, in particular, for African and Southeast Asian rivers is a high priority to reduce uncertainty on FCO2.

This regional study quantifies the CO2 exchange at the air–water interface along the land–ocean aquatic continuum (LOAC) of the northeast North American coast, from streams to the shelf break. Our analysis explicitly accounts for spatial and seasonal variability in the CO2 fluxes. The yearly integrated budget reveals the gradual change in the intensity of the CO2 exchange at the air–water interface, from a strong source towards the atmosphere in streams and rivers (3.0 ± 0.5 TgC yr−1) and estuaries (0.8 ± 0.5 TgC yr−1) to a net sink in continental shelf waters (−1.7 ± 0.3 TgC yr−1). Significant differences in flux intensity and their seasonal response to climate variations is observed between the North and South sections of the study area, both in rivers and coastal waters. Ice cover, snowmelt, and intensity of the carbon removal efficiency through the estuarine filter are identified as important control factors of the observed spatiotemporal variability in CO2 exchange along the LOAC.

Over the past decade, estimates of the atmospheric CO2 uptake by continental shelf seas were constrained within the 0.18–0.45 Pg C yr−1 range. However, most of those estimates are based on extrapolations from limited data sets of local flux measurements (n

The damming of rivers represents one of the most far-reaching human modifications of the flows of water and associated matter from land to sea. Dam reservoirs are hotspots of sediment accumulation, primary productivity (P) and carbon mineralization (R) along the river continuum. Here we show that for the period 1970–2030, global carbon mineralization in reservoirs exceeds carbon fixation (P, https://www.nature.com/articles/ncomms15347, SCOPUS: ar.j, info:eu-repo/semantics/published

Lateral transfer of carbon (C) from terrestrial ecosystems into the inland water network is an important component of the global C cycle, which sustains a large aquatic CO2 evasion flux fueled by the decomposition of allochthonous C inputs. Globally, estimates of the total C exports through the terrestrial-aquatic interface range from 1.5 to 2.7 Pg C yr−1 (Cole et al., 2007; Battin et al., 2009; Tranvik et al., 2009), i.e. in the order of 2–5% of the terrestrial NPP. Earth System Models (ESM) of the climate system ignore these lateral transfers of C, and thus likely overestimate the terrestrial C sink. In this study, we present the implementation of fluvial transport of dissolved organic carbon (DOC) and CO2 into ORCHIDEE, the land surface scheme of the Institut Pierre-Simon Laplace ESM. This new model branch, called ORCHILEAK, represents DOC production from canopy and soils, DOC and CO2 leaching from soils to streams, DOC decomposition and CO2 evasion to the atmosphere during its lateral transport in rivers, as well as exchange with the soil carbon and litter stocks on floodplains and in swamps. We parameterized and validated ORCHILEAK for the Amazon basin, the world's largest river system with regard to discharge and one of the most productive ecosystems of the world. With ORCHILEAK, we are able to reproduce observed terrestrial and aquatic fluxes of DOC and CO2 in the Amazon basin, both in terms of mean values and seasonality. In addition, we are able to resolve the spatio-temporal variability in C fluxes along the canopy-soil-aquatic continuum at high resolution (1°, daily) and to quantify the different terrestrial contributions to the aquatic C fluxes. We simulate that more than 2/3 of the Amazon's fluvial DOC export is contributed by the decomposition of submerged litter. Throughfall DOC fluxes from canopy to ground are about as high as the total DOC inputs to inland waters. The latter, however, are mainly sustained by litter decomposition. Decomposition of DOC and submerged plant litter contributes slightly more than half of the CO2 evasion from the water surface, while the remainder is contributed by soil respiration. Total CO2 evasion from the water surface equals about 5 % of the terrestrial NPP. Our results highlight that ORCHILEAK is well suited to simulate carbon transfers along the terrestrial-aquatic continuum of tropical forests. It also opens the perspective that provided parameterization, calibration and validation is performed for other biomes, the new model branch could improve the quantification of the global terrestrial C sink and help better constrain carbon cycle-climate feedbacks in future projections.

Accurate assessment of anthropogenic carbon dioxide (CO2) emissions and their redistribution among the atmosphere, ocean, and terrestrial biosphere is important to better understand the global carbon cycle, support the development of climate policies, and project future climate change. Here we describe data sets and a methodology to quantify all major components of the global carbon budget, including their uncertainties, based on the combination of a range of data, algorithms, statistics and model estimates and their interpretation by a broad scientific community. We discuss changes compared to previous estimates, consistency within and among components, alongside methodology and data limitations. CO2 emissions from fossil-fuel combustion and cement production (EFF) are based on energy statistics, while emissions from land-use change (ELUC), mainly deforestation, are based on combined evidence from land-cover change data, fire activity associated with deforestation, and models. The global atmospheric CO2 concentration is measured directly and its rate of growth (G ATM) is computed from the annual changes in concentration. The mean ocean CO2 sink (SOCEAN) is based on observations from the 1990s, while the annual anomalies and trends are estimated with ocean models. The variability in SOCEAN is evaluated for the first time in this budget with data products based on surveys of ocean CO2 measurements. The global residual terrestrial CO2 sink (SLAND) is estimated by the difference of the other terms of the global carbon budget and compared to results of independent dynamic global vegetation models forced by observed climate, CO2 and land cover change (some including nitrogen-carbon interactions). All uncertainties are reported as ±1σ ,reflecting the current capacity to characterise the annual estimates of each component of the global carbon budget. For the last decade available (2003-2012), EFF was 8.6±0.4 GtC yr-1, ELUC 0.9±0.5 GtC yr-1, GATM 4.3±0.1 GtC yr-1, SOCEAN 2.5±0.5 GtC yr -1, and SLAND 2.8±0.8 GtC yr-1. For year 2012 alone, EFF grew to 9.7±0.5 GtC yr-1, 2.2% above 2011, reflecting a continued growing trend in these emissions, G ATM was 5.1±0.2 GtC yr-1, SOCEAN was 2.9±0.5 GtC yr-1, and assuming an ELUC of 1.0±0.5 GtC yr-1 (based on the 2001-2010 average), S LAND was 2.7±0.9 GtC yr-1. GATM was high in 2012 compared to the 2003-2012 average, almost entirely reflecting the high EFF. The global atmospheric CO2 concentration reached 392.52±0.10 ppm averaged over 2012. We estimate that EFF will increase by 2.1% (1.1- 3.1 %) to 9.9±0.5 GtC in 2013, 61% above emissions in 1990, based on projections of world gross domestic product and recent changes in the carbon intensity of the economy.With this projection, cumulative emissions ofCO2 will reach about 535±55 GtC for 1870-2013, about 70% from EFF (390±20 GtC) and 30% from ELUC (145±50 GtC). This paper also documents any changes in the methods and data sets used in this new carbon budget from previous budgets (Le Quéré et al. 2013). All observations presented here can be downloaded from the Carbon Dioxide Information Analysis Center (doi:10.3334/CDIAC/GCP-2013-V2.3). © 2014 Author(s) CC Attribution 3.0 License., 0, SCOPUS: ar.j, info:eu-repo/semantics/published

Estuaries act as strong carbon and nutrient filters and are relevant contributors to the atmospheric CO2 budget. They thus play an important, yet poorly constrained, role for global biogeochemical cycles and climate. This manuscript reviews recent developments in the modelling of estuarine biogeochemical dynamics. The first part provides an overview of the dominant physical and biogeochemical processes that control the transformations and fluxes of carbon and nutrients along the estuarine gradient. It highlights the tight links between estuarine geometry, hydrodynamics and scalar transport, as well as the role of transient and nonlinear dynamics. The most important biogeochemical processes are then discussed in the context of key biogeochemical indicators such as the net ecosystem metabolism (NEM), air–water CO2 fluxes, nutrient-filtering capacities and element budgets. In the second part of the paper, we illustrate, on the basis of local estuarine modelling studies, the power of reaction-transport models (RTMs) in understanding and quantifying estuarine biogeochemical dynamics. We show how a combination of RTM and high-resolution data can help disentangle the complex process interplay, which underlies the estuarine NEM, carbon and nutrient fluxes, and how such approaches can provide integrated assessments of the air–water CO2 fluxes along river–estuary–coastal zone continua. In addition, trends in estuarine biogeochemical dynamics across estuarine geometries and environmental scenario are explored, and the results are discussed in the context of improving the modelling of estuarine carbon and CO2 dynamics at regional and global scales.

We present a one-dimensional reactive transport model to estimate benthic fluxes of dissolved inorganic carbon (DIC) and alkalinity (AT) from coastal marine sediments. The model incorporates the transport processes of sediment accumulation, molecular diffusion, bioturbation and bioirrigation, while the reactions included are the redox pathways of organic carbon oxidation, re-oxidation of reduced nitrogen, iron and sulfur compounds, pore water acid-base equilibria, and dissolution of particulate inorganic carbon (calcite, aragonite, and Mg-calcite). The coastal zone is divided into four environmental units with different particulate inorganic carbon (PIC) and particulate organic carbon (POC) fluxes: reefs, banks and bays, carbonate shelves and non-carbonate shelves. Model results are analyzed separately for each environment and then scaled up to the whole coastal ocean. The model-derived estimate for the present-day global coastal benthic DIC efflux is 126 Tmol yr-1, based on a global coastal reactive POC depositional flux of 117 Tmol yr-1. The POC decomposition leads to a carbonate dissolution from shallow marine sediments of 7 Tmol yr-1 (on the order of 0.1 Pg C yr-1. Assuming complete re-oxidation of aqueous sulfide released from sediments, the effective net flux of alkalinity to the water column is 29 Teq. yr-1, primarily from PIC dissolution (46%) and ammonification (33%). Because our POC depositional flux falls in the high range of global values given in the literature, the reported DIC and alkalinity fluxes should be viewed as upper-bound estimates. Increasing coastal seawater DIC to what might be expected in year 2100 due to the uptake of anthropogenic CO2 increases PIC dissolution by 2.3 Tmol yr-1and alkalinity efflux by 4.8 Teq. yr-1. Our reactive transport modeling approach not only yields global estimates of benthic DIC, alkalinity and nutrient fluxes under variable scenarios of ocean productivity and chemistry, but also provides insights into the underlying processes. © Author(s) 2013., SCOPUS: ar.j, info:eu-repo/semantics/published

The carbon cycle of the coastal ocean is a dynamic component of the global carbon budget. But the diverse sources and sinks of carbon and their complex interactions in these waters remain poorly understood. Here we discuss the sources, exchanges and fates of carbon in the coastal ocean and how anthropogenic activities have altered the carbon cycle. Recent evidence suggests that the coastal ocean may have become a net sink for atmospheric carbon dioxide during post-industrial times. Continued human pressures in coastal zones will probably have an important impact on the future evolution of the coastal ocean's carbon budget.

Understanding the global carbon (C) cycle is of crucial importance to map current and future climate dynamics relative to global environmental change. A full characterization of C cycling requires detailed information on spatiotemporal patterns of surface-atmosphere fluxes. However, relevant C cycle observations are highly variable in their coverage and reporting standards. Especially problematic is the lack of integration of vertical oceanic, inland freshwaters and terrestrial carbon dioxide (CO2) exchange. Here we adopt a data-driven approach to synthesize a wide range of observation-based spatially explicit surface-atmosphere CO2 fluxes from 2001 and 2010, to identify the state of today’s observational opportunities and data limitation. The considered fluxes include vertical net exchange of open oceans, continental shelves, estuaries, rivers, and lakes, as well as CO2 fluxes related to gross primary productivity, terrestrial ecosystem respiration, fire emissions, loss of tropical aboveground C, harvested wood and crops, as well as fossil fuel and cement emissions. Spatially explicit CO2 fluxes are obtained through geostatistical and/or remote sensing-based upscaling; minimizing biophysical or biogeochemical assumptions encoded in process-based models. We estimate a global bottom-up net C exchange (NCE) between the surface (land, ocean, and coastal areas) and the atmosphere. Uncertainties for NCE and its components are derived using resampling. In most continental regions our NCE estimates agree well with independent estimates from other sources. This holds for Europe (mean ±1 SD: 0.80 ± 0.16 PgC/yr, positive numbers are sources to the atmosphere), Russia (−0.02 ± 0.49 PgC/yr), East Asia (1.76 ± 0.38 PgC/yr), South Asia (0.25 ± 0.16 PgC/yr), and Australia (0.22 ± 0.47 PgC/yr). Our NCE estimates also suggest large C sink in tropical areas. The global NCE estimate is −6.07 ± 3.38 PgC/yr. This global bottom-up value is the opposite direction of what is expected from the atmospheric growth rate of CO2, and would require an offsetting surface C source of 4.27±0.10 PgC/yr. This mismatch highlights large knowledge and observational gaps in tropical areas, particularly in South America, Africa, and Southeast Asia, but also in North America. Our uncertainty assessment provides the basis for designing new observation campaigns. In particular, we lack seasonal monitoring of shelf, estuary and inland water-atmosphere C exchange. Also, extensive pCO2 measurements are missing in the Southern Ocean. Most importantly, tropical land C fluxes suffer from a lack of in-situ observations. The consistent derivation of data uncertainties could serve as prior knowledge in multi-criteria optimization such as the Carbon Cycle Data Assimilation System (CCDAS) without overstating data credibility. Furthermore, the spatially explicit flux estimates may be used as a starting point to assess the validity of countries’ claims of reducing net C emissions in climate change negotiations.

We present a new version of the coupled Earth system model GEOCLIM. The new release, GEOCLIM reloaded (v 1.0), links the existing atmosphere and weathering modules to a novel, temporally and spatially resolved model of the global ocean circulation, which provides a physical framework for a mechanistic description of the marine biogeochemical dynamics of carbon, nitrogen, phosphorus and oxygen. The ocean model is also coupled to a fully formulated, vertically resolved diagenetic model. GEOCLIM reloaded is thus a unique tool to investigate the short- and long-term feedbacks between climatic conditions, continental inputs, ocean biogeochemical dynamics and diagenesis. A complete and detailed description of the resulting Earth system model and its new features is first provided. The performance of GEOCLIM reloaded is then evaluated by comparing steady-state simulation under present-day conditions with a comprehensive set of oceanic data and existing global estimates of bio-element cycling in the pelagic and benthic compartments.

We present a novel approach for the simulation of the impacts of finfish aquaculture on sedimentary redox dynamics, based on the coupling of a fish farm waste deposition model (DEPOMOD) and a knowledge-based reactive transport model (RTM) of early diagenesis. The integrated model was applied to a salmon fish farm located in a Scottish fjordic sealoch. The major diagenetic processes of the reaction network were first identified on the basis of literature information and historic data. Next, the organic carbon (OC) flux at a pristine site near the farm was estimated by fitting the vertical profiles of pore water and solid-state chemical species measured in the field. DEPOMOD was then used to predict the fluxes of OC due to the release of uneaten feed and faeces at various distances away from the farm. These fluxes were added to the background 'natural' fluxes and used as forcing functions for the RTM. Comparison of the simulated transient profiles with data collected at an impacted site revealed that the RTM model satisfactorily predicted the transient dynamics of the system. We discuss the use of the model for cost-effective environmental impact assessments, site selection and the optimization of husbandry practices. © Inter-Research 2009.

A fully transient, two-dimensional nested grid reactive-transport model of the Scheldt tidal river-estuary continuum is used to quantify seasonally-resolved silica and nitrogen filtering capacities and export fluxes to the coastal zone over a period of one year. Simulation results indicate that a pronounced seasonal variability in nutrient cycling results from the combined effect of biogeochemical transformations and nutrient flux imbalances, which arise from the time-lagged response of the scalar fields to hydrological perturbations. Dissolved silica reveals a larger mass storage capacity and a slower flux response to upstream perturbations than nitrogen. As a consequence, the nutrient export flux ratio to the coastal zone, which is instrumental for the marine phytoplankton dynamics, depends strongly on the transient propagation of the scalar fluxes. The estuarine nutrient retention shows a strong temporal variability, which is driven by the complex interplay between reaction and transport. Results reveal that seasonal filtering capacities, with values comprised between 0.01 and 0.81 for silica and 0.13 and 0.78 for nitrogen, cannot be estimated by existing empirical relationships between this parameter and freshwater residence time. At the seasonal scale, nutrient export fluxes to the coastal zone cannot be quantified from the river loads and the estuarine filtering capacities.

A fully coupled, two-dimensional hydrodynamic and reactive-transport model of C, N, O2 and Si along a river–estuarine–coastal zone system is presented. It is applied to the Scheldt continuum, a macrotidal environment strongly affected by anthropogenic perturbations. The model extends from the upper tidal river and its tributaries to the southern Bight of the North Sea. Five dynamically linked nested grids are used, with a spatial resolution progressively increasing from 33 m to 2.7 km. The biogeochemical reaction network consists of aerobic degradation, nitrification, denitrification, phytoplankton growth and mortality, as well as reaeration. Diagnostic simulations of a typical summer situation in the early 1990s are compared to field data taken from the OMES database (> 300 samples per variable). Results demonstrate that the process rates in the tidal river are very high and far larger than in the saline estuary, with maximum nitrification rates in the water column up to 70 mM N day− 1, and maximum aerobic respiration and denitrification up to 70 and 40 mM C day− 1, respectively. Phytoplankton production is about one order of magnitude lower, a result which confirms the dominance of heterotrophic processes in this system. The influence of secondary and tertiary wastewater treatment in the catchment is then assessed. Results show a significant decrease of organic matter and ammonium concentrations above Antwerp, which in turn leads to a partial restoration of oxygen levels. The model also predicts a reduction of denitrification rates, which locally results in a 4-fold increase of the nitrate concentration. Mass budgets for carbon, nitrogen and oxygen are established for the saline estuary (km 0 to 100) and for the tidal river network (km 100 to 160). Three scenarios, corresponding to the situation in the early 1990s, the years 2000 and the situation expected in 2010 are considered. They show that the tidal river and the estuary contribute almost equally to the overall biogeochemical cycling of these elements, despite the very different water volumes involved. For the simulated periods, the large decrease in nitrogen input (> 55%) expected between 1990 and 2010 will not lead to a significant decrease of N export to the coastal zone during the summer period.

This study applies the Carbon-Generic Estuary Model (C-GEM) modeling platform to simulate the estuarine biogeochemical dynamics - in particular the air-water CO2 exchange - in three idealized tidal estuaries characterized by increasing riverine influence, from a so-called "marine estuary" to a "riverine estuary". An intermediate case called "mixed estuary" is also considered. C-GEM uses a generic biogeochemical reaction network and a unique set of model parameters extracted from a comprehensive literature survey to perform steady-state simulations representing average conditions for temperate estuaries worldwide. Climate and boundary conditions are extracted from published global databases (e.g. World Ocean Atlas, GLORICH) and catchment model outputs (GlobalNEWS2). The whole-system biogeochemical indicators net ecosystem metabolism (NEM), C and N filtering capacities (FCTC and FCTN, respectively) and CO2 gas exchanges (FCO2) are calculated across the three idealized systems and are related to their main hydrodynamic and transport characteristics. A sensitivity analysis, which propagates the parameter uncertainties, is also carried out, followed by projections of changes in the biogeochemical indicators for the year 2050. Results show that the average C filtering capacities for baseline conditions are 40, 30 and 22 % for the marine, mixed and riverine estuary, respectively, while N filtering capacities, calculated in a similar fashion, range from 22 % for the marine estuary to 18 and 15 % for the mixed and the riverine estuaries. Sensitivity analysis performed by varying the rate constants for aerobic degradation, denitrification and nitrification over the range of values reported in the literature significantly widens these ranges for both C and N. Simulations for the year 2050 suggest that all estuaries will remain largely heterotrophic, although a slight improvement of the estuarine trophic status is predicted. In addition, our results suggest that, while the riverine and mixed systems will only marginally be affected by an increase in atmospheric pCO2, the marine estuary is likely to become a significant CO2 sink in its downstream section. In the decades to come, such a change in behavior might strengthen the overall CO2 sink of the estuary-coastal ocean continuum., SCOPUS: ar.j, info:eu-repo/semantics/published

Accurate assessment of anthropogenic carbon dioxide (CO2) emissions and their redistribution among the atmosphere, ocean, and terrestrial biosphere is important to better understand the global carbon cycle, support the development of climate policies, and project future climate change. Here we describe data sets and a methodology to quantify all major components of the global carbon budget, including their uncertainties, based on the combination of a range of data, algorithms, statistics, and model estimates and their interpretation by a broad scientific community. We discuss changes compared to previous estimates, consistency within and among components, alongside methodology and data limitations. CO2 emissions from fossil fuel combustion and cement production (EFF) are based on energy statistics and cement production data, respectively, while emissions from land-use change (ELUC), mainly deforestation, are based on combined evidence from land-cover-change data, fire activity associated with deforestation, and models. The global atmospheric CO2 concentration is measured directly and its rate of growth (GATM) is computed from the annual changes in concentration. The mean ocean CO2 sink (SOCEAN) is based on observations from the 1990s, while the annual anomalies and trends are estimated with ocean models. The variability in SOCEAN is evaluated with data products based on surveys of ocean CO2 measurements. The global residual terrestrial CO2 sink (SLAND) is estimated by the difference of the other terms of the global carbon budget and compared to results of independent dynamic global vegetation models forced by observed climate, CO2, and land-cover-change (some including nitrogen-carbon interactions). We compare the mean land and ocean fluxes and their variability to estimates from three atmospheric inverse methods for three broad latitude bands. All uncertainties are reported as ±1σ, reflecting the current capacity to characterise the annual estimates of each component of the global carbon budget. For the last decade available (2004-2013) EFF was 8.9 ± 0.4 GtC yr-1, ELUC 0.9 ± 0.5 GtC yr-1, GATM 4.3 ± 0.1 GtC yr-1, SOCEAN 2.6 ± 0.5 GtC yr-1, and SLAND 2.9 ± 0.8 GtC yr-1. For year 2013 alone, EFF grew to 9.9 ± 0.5 GtC yr-1, 2.3% above 2012, continuing the growth trend in these emissions, ELUC was 0.9 ± 0.5 GtC yr-1, GATM was 5.4 ± 0.2 GtC yr-1, SOCEAN was 2.9 ± 0.5 GtC yr-1, and SLAND was 2.5 ± 0.9 GtC yr-1. GATM was high in 2013, reflecting a steady increase in EFF and smaller and opposite changes between SOCEAN and SLAND compared to the past decade (2004-2013). The global atmospheric CO2 concentration reached 395.31 ± 0.10 ppm averaged over 2013. We estimate that EFF will increase by 2.5% (1.3-3.5%) to 10.1 ± 0.6 GtC in 2014 (37.0 ± 2.2 GtCO2 yr-1), 65% above emissions in 1990, based on projections of world gross domestic product and recent changes in the carbon intensity of the global economy. From this projection of EFF and assumed constant ELUC for 2014, cumulative emissions of CO2 will reach about 545 ± 55 GtC (2000 ± 200 GtCO2) for 1870-2014, about 75% from EFF and 25% from ELUC. This paper documents changes in the methods and data sets used in this new carbon budget compared with previous publications of this living data set (Le Quéré et al. 2013, 2014). All observations presented here can be downloaded from the Carbon Dioxide Information Analysis Center (doi:10.3334/CDIAC/GCP-2014)., 0, SCOPUS: ar.j, info:eu-repo/semantics/published

In the frame of the BIOGEST project, the fulltransient, one-dimensional, reactive-transportmodel CONTRASTE has been extended for thecomputation of biogases in the Scheldt estuary. The CONTRASTE model (Coupled, Networked, Transport-Reaction Algorithm for Strong T> idal Estuaries) provides a satisfactorydescription of the estuarine residualcirculation (including daily freshwaterdischarge and a complete description of thetide) and a flexible implementation of thevarious physico-chemical and biologicaltransformations, including bothkinetically-controlled and equilibriumreactions. The model allows resolution of thecomplex, nonlinear collective behaviour of thistype of system and investigation of thenon-steady-state phenomena which governestuarine dynamics. Variables currentlyimplemented in the model include salinity,suspended matter, oxygen, inorganic carbonspecies, degradable organic carbon andnitrogen, inorganic nitrogen species,freshwater and marine phytoplankton. Biologicalprocesses described are heterotrophicrespiration, primary production, nitrificationand denitrification. Equilibrium formulationsallow for DIC and NH4+/NH3speciation. Physical processes include gastransfer at the water/air interface, dependingon both wind speed and current velocity. pHprofiles are explicitly computed and constitutea very sensitive check of the overall modelconsistency. Results of the CONTRASTE model arein very good agreement with the measuredlongitudinal distribution of the variablesconsidered, in particular O2, pH,pCO2 and N2O concentrations. However,discrepancies are observed between thecalculated fluxes of CO2 and thoseestimated using an in situ floatingchamber. It is shown that the evaluation of gastransfer can be affected by serious errors ifthe variations due to changes in currentvelocity and water depth during one tidal cycleare not taken into consideration. The modelalso shows that the fluxes of biogases inestuaries are greatly influenced by thequasi-exponential increase of the exchangesurface area with decreasing distance to thesea. Our estimation of the total daily flux ofO2, CO2 and N2O is equal to+28500, −19000 and −17 kmoles.day−1respectively for the Scheldt estuary in July 1996.

This contribution reviews the role of the terrestrial-aquatic interface in the global carbon cycle. We highlight that carbon leakage through this interface has profound ramifications for the terrestrial carbon balance and for the anthropogenic CO2 budget. Our budget analysis identifies the need for an integrated process-based quantitative understanding of the terrestrial-aquatic interface that includes its response to anthropogenic perturbations. Complementary observational and modeling efforts in this direction are presented.

Massive short-term (4–8 wk) blooms of Phaeocystis have been observed in coastal North Sea waters in the spring for a number of years now. Researchers have shown that these algal blooms, which lead to eutrophication of the local water mass, are limited by the supply of inorganic nitrogen from the various bordering estuaries. We demonstrate using the case of a typical heavily polluted macrotidal estuary, the Scheldt in Belgium and the Netherlands, that the short duration of the algal blooms requires estuarine flux estimation methods with a high temporal resolution. We use the fully transient, multicomponent reactive transport model CONTRASTE to compute inorganic nitrogen fluxes through the mouth of the Scheldt estuary into the North Sea. The model simulations use a detailed dataset of upstream river discharges and solute concentrations along with tidal forcings for a 210 day period between December 1, 1994 and June 30, 1995. Our temporally resolved estimate shows that widely used estuarine flux estimation methods which rely on a steady-state approximation underestimate the inorganic nitrogen loading available to sustain primary production in the North Sea during the period of the algal bloom by 100%.

A one–dimensional, time–dependent transport model which includes tidal fluctuations has been developed to simulate the barotropic dynamics and the solute evolution in strong tidal estuaries. The model is used to estimate fluxes in a typical macrotidal estuary, the Scheldt in Belgium and The Netherlands. The results of the model are compared with those obtained with classical flux estimation methods which neglect the nonlinearities of the fluid motion as well as the nonstationary behaviour of solute transport. It is shown that in macrotidal systems, which are generally characterized by fairly long residence times, both contributions are significant. In particular, the residual water flow to the coastal waters differs markedly from the freshwater discharge and the solute dynamics arising from fluctuating conditions at the estuarine boundaries is significantly influenced by the history of the water flow. It is demonstrated that linear property–salinity plots can be obtained in a system characterized by transient (nonsteady–state) conditions. This result allows one to quantify the error associated with the widely used ‘apparent zero end–member’ (AZE) classical flux estimation methodology. Results demonstrate that the AZE technique, based on the analysis of mixing curves, introduces large errors in the estimation of the long–term residual constituent flux towards the coastal zone.

A coupled, fully transient, multicomponent reaction-transport model has been developed to estimate long-term fluxes of reactive compounds in strong tidal estuaries. The model is applied to a preliminary analysis of the carbon cycle in the Scheldt estuary in Belgium and The Netherlands. The model provides a realistic description of the residual circulation in a strong tidal estuary and includes the essential feedback mechanisms between interdependent chemical species. The model has been used to analyze the fundamentally transient nature of strong tidal estuaries and, in particular, the effect of these non-steady state conditions on the long-term fluxes of chemical species out of the estuary. The results indicate that flux estimation techniques based upon steady-state assumptions may result in significant errors. The model has also been used to investigate biogeochemical interactions characterized by a large spectrum of time scales, which it does by including simultaneous equilibrium reactions and kinetically-mediated processes. Simulations carried out with the model suggest that a formulation based upon microbially-mediated, kinetically-controlled reactions provides a superior description of solute profiles in the Scheldt estuary than does a global equilibrium redox formulation. The mixed equilibrium-kinetic formulation also makes it possible to track simultaneously two master variables: the redox state of the system and the pH. By providing strong constraints on the system, these two master variables can be used to test the model's self-consistency. The simulations carried out with the model suggest the pH profile in the Scheldt estuary is the result of a balance of biogeochemical reactions which produce H+ and degassing which consumes H+ and not the result of simple mixing between seawater and freshwater.

Redox processes, including degradation of organic contaminants, are often controlled by microorganisms residing in natural porous media like soils or aquifers. These environments are characterized by heterogeneities at various scales which influence the transport of chemical species and the spatial distribution of microorganisms. As a result, the accessibility of the chemical species by the resident microbial populations may be limited, altering the efficiency of the biodegradation process. Hence, the biodegradation rate of contaminants at large scales does not only depend on the degradation capacity of the indigenous microbial population but also on the heterogeneities of the hosting media at smaller scales. It is thus important to establish a link between effective reaction rates and various structural features of porous media which can be directly observed or measured. This link is urgently needed because explicit resolution of heterogeneities within large-scale reactive transport models is still limited by the available computational capacities. The present study introduces a reactive transport modeling approach to determine the influence of pore-scale heterogeneities on biogeochemical processes in porous media. For this purpose, a pore network model, which simulates flow and advective-diffusive transport of chemical species in heterogeneous pore networks is developed and coupled to the Biogeochemical Reaction Network Simulator (BRNS). The resulting coupled model (PNBRNS) is able to simulate the reactive transport of solutes in heterogeneous pore assemblies. The PNBRNS model is applied for the simulation of a test case of bioavailability and effective biodegradation rate of a dissolved contaminant in different pore networks, built using a discrete set of geostatistically derived pore-size or biomass distributions. Results show that the heterogeneity of the pore-size distribution has a significant impact on bioavailability while the heterogeneity of the biomass distribution only leads to minor effects. The model also includes intra-pore bioavailability restrictions using diffusion-limited biodegradation kinetics. The results indicate that intra-pore limitations lead to extra constrains on the biodegradation of contaminants, even in the presence of larger-scale structural heterogeneities.

A one‐dimensional reaction‐transport model is used to investigate the dynamics of methane gas in coastal sediments in response to intra‐annual variations in temperature and pressure. The model is applied to data from two shallow water sites in Eckernforde Bay (Germany) characterized by low and high rates of upward fluid advection. At both sites, organic matter is buried below the sulfate‐reducing zone to the methanogenic zone at sufficiently high rates to allow supersaturation of the pore water with dissolved methane and to form a free methane gas phase. The methane solubility concentration varies by similar magnitudes at both study sites in response to bottom water temperature changes and leads to pronounced peaks in the gas volume fraction in autumn when the methanic zone temperature is at a maximum. Yearly hydrostatic pressure variations have comparatively negligible effects on methane solubility. Field data suggest that no free gas escapes to the water column at any time of the year. Although the existence of gas migration cannot be substantiated by direct observation, a speculative mechanism for slow moving gas is proposed here. The model results reveal that free gas migrating upward into the undersaturated pore water will completely dissolve and subsequently be consumed above the free gas depth (FGD) by anaerobic oxidation of methane (AOM). This microbially mediated process maintains methane undersaturation above the FGD. Although the complexities introduced by seasonal changes in temperature lead to different seasonal trends for the depth‐integrated AOM rates and the FGD, both sites adhere to previously developed prognostic indicators for methane fluxes based on the FGD.

This study presents a first attempt to quantify the biogeochemical transformations and fluxes of carbon and nutrients along the entire mixing zone of the shallow, tidally-dominated estuary–coastal zone continuum of the Scheldt (Belgium/The Netherlands). A fully transient, two-dimensional, nested-grid hydrodynamic model of the continuum is coupled to the biogeochemical MIRO model for the coastal zone and the CONTRASTE model for the estuary. Transient model simulations are performed with a high spatial (80–750 m) and temporal (30 min) resolution over a period of one year (January–December 1995). The high temporal resolution allows including the short-term variability triggered by the tides, the freshwater discharge and the wind stress. System scale simulations provide time series of nutrient transformations and fluxes along the entire estuary–coastal zone continuum, as well as highly resolved nutrient inventories for the estuarine and the coastal zone sub-domains. Simulation results reveal that the balance between highly variable estuarine nutrient inputs and physical constrains set by the unsteady residual transport field exert an important control on the magnitude and succession of phytoplankton blooms and the ecosystem structure in the coastal zone. In addition, they suggest that the poorly surveyed estuarine–coastal zone interface plays a central role in the continuum. In this dynamic area, marked spatial concentration gradients develop and episodically lead to a reversal of material fluxes from the coast into the estuary. During distinct episodes of the productive period, euryhaline coastal diatoms intrude far upstream into the saline estuary. This intrusion reduces the estuarine nutrient concentrations and export fluxes, thereby reinforcing the nutrient limitation in the coastal area. As a consequence, the estuarine filter does not operate independently from the processes in the coastal zone. The dynamic interplay between the two ecosystems and the intense process rates operating at their transition, therefore, strongly supports our continuum approach.