Dearomatization drives complexity generation in freshwater organic matter.

Dissolved organic matter (DOM) is one of the most complex, dynamic and abundant sources of organic carbon, but its chemical reactivity remains uncertain1-3. Greater insights into DOM structural features could facilitate understanding its synthesis, turnover and processing in the global carbon cycle4,5. Here we use complementary multiplicity-edited 13C nuclear magnetic resonance (NMR) spectra to quantify key substructures assembling the carbon skeletons of DOM from four main Amazon rivers and two mid-size Swedish boreal lakes. We find that one type of reaction mechanism, oxidative dearomatization (ODA), widely used in organic synthetic chemistry to create natural product scaffolds6-10, is probably a key driver for generating structural diversity during processing of DOM that are rich in suitable polyphenolic precursor molecules. Our data suggest a high abundance of tetrahedral quaternary carbons bound to one oxygen and three carbon atoms (OCqC3 units). These units are rare in common biomolecules but could be readily produced by ODA of lignin-derived and tannin-derived polyphenols. Tautomerization of (poly)phenols by ODA creates non-planar cyclohexadienones, which are subject to immediate and parallel cycloadditions. This combination leads to a proliferation of structural diversity of DOM compounds from early stages of DOM processing, with an increase in oxygenated aliphatic structures. Overall, we propose that ODA is a key reaction mechanism for complexity acceleration in the processing of DOM molecules, creation of new oxygenated aliphatic molecules and that it could be prevalent in nature.

Environmental drivers of increased ecosystem respiration in a warming tundra.

Arctic and alpine tundra ecosystems are large reservoirs of organic carbon1,2. Climate warming may stimulate ecosystem respiration and release carbon into the atmosphere3,4. The magnitude and persistency of this stimulation and the environmental mechanisms that drive its variation remain uncertain5-7. This hampers the accuracy of global land carbon-climate feedback projections7,8. Here we synthesize 136 datasets from 56 open-top chamber in situ warming experiments located at 28 arctic and alpine tundra sites which have been running for less than 1 year up to 25 years. We show that a mean rise of 1.4 °C [confidence interval (CI) 0.9-2.0 °C] in air and 0.4 °C [CI 0.2-0.7 °C] in soil temperature results in an increase in growing season ecosystem respiration by 30% [CI 22-38%] (n = 136). Our findings indicate that the stimulation of ecosystem respiration was due to increases in both plant-related and microbial respiration (n = 9) and continued for at least 25 years (n = 136). The magnitude of the warming effects on respiration was driven by variation in warming-induced changes in local soil conditions, that is, changes in total nitrogen concentration and pH and by context-dependent spatial variation in these conditions, in particular total nitrogen concentration and the carbon:nitrogen ratio. Tundra sites with stronger nitrogen limitations and sites in which warming had stimulated plant and microbial nutrient turnover seemed particularly sensitive in their respiration response to warming. The results highlight the importance of local soil conditions and warming-induced changes therein for future climatic impacts on respiration.

Microbial carbon use efficiency promotes global soil carbon storage.

Soils store more carbon than other terrestrial ecosystems1,2. How soil organic carbon (SOC) forms and persists remains uncertain1,3, which makes it challenging to understand how it will respond to climatic change3,4. It has been suggested that soil microorganisms play an important role in SOC formation, preservation and loss5-7. Although microorganisms affect the accumulation and loss of soil organic matter through many pathways4,6,8-11, microbial carbon use efficiency (CUE) is an integrative metric that can capture the balance of these processes12,13. Although CUE has the potential to act as a predictor of variation in SOC storage, the role of CUE in SOC persistence remains unresolved7,14,15. Here we examine the relationship between CUE and the preservation of SOC, and interactions with climate, vegetation and edaphic properties, using a combination of global-scale datasets, a microbial-process explicit model, data assimilation, deep learning and meta-analysis. We find that CUE is at least four times as important as other evaluated factors, such as carbon input, decomposition or vertical transport, in determining SOC storage and its spatial variation across the globe. In addition, CUE shows a positive correlation with SOC content. Our findings point to microbial CUE as a major determinant of global SOC storage. Understanding the microbial processes underlying CUE and their environmental dependence may help the prediction of SOC feedback to a changing climate.

Sub-continental-scale carbon stocks of individual trees in African drylands.

The distribution of dryland trees and their density, cover, size, mass and carbon content are not well known at sub-continental to continental scales1-14. This information is important for ecological protection, carbon accounting, climate mitigation and restoration efforts of dryland ecosystems15-18. We assessed more than 9.9 billion trees derived from more than 300,000 satellite images, covering semi-arid sub-Saharan Africa north of the Equator. We attributed wood, foliage and root carbon to every tree in the 0-1,000 mm year-1 rainfall zone by coupling field data19, machine learning20-22, satellite data and high-performance computing. Average carbon stocks of individual trees ranged from 0.54 Mg C ha-1 and 63 kg C tree-1 in the arid zone to 3.7 Mg C ha-1 and 98 kg tree-1 in the sub-humid zone. Overall, we estimated the total carbon for our study area to be 0.84 (±19.8%) Pg C. Comparisons with 14 previous TRENDY numerical simulation studies23 for our area found that the density and carbon stocks of scattered trees have been underestimated by three models and overestimated by 11 models, respectively. This benchmarking can help understand the carbon cycle and address concerns about land degradation24-29. We make available a linked database of wood mass, foliage mass, root mass and carbon stock of each tree for scientists, policymakers, dryland-restoration practitioners and farmers, who can use it to estimate farmland tree carbon stocks from tablets or laptops.

Integrated global assessment of the natural forest carbon potential.

Forests are a substantial terrestrial carbon sink, but anthropogenic changes in land use and climate have considerably reduced the scale of this system1. Remote-sensing estimates to quantify carbon losses from global forests2-5 are characterized by considerable uncertainty and we lack a comprehensive ground-sourced evaluation to benchmark these estimates. Here we combine several ground-sourced6 and satellite-derived approaches2,7,8 to evaluate the scale of the global forest carbon potential outside agricultural and urban lands. Despite regional variation, the predictions demonstrated remarkable consistency at a global scale, with only a 12% difference between the ground-sourced and satellite-derived estimates. At present, global forest carbon storage is markedly under the natural potential, with a total deficit of 226 Gt (model range = 151-363 Gt) in areas with low human footprint. Most (61%, 139 Gt C) of this potential is in areas with existing forests, in which ecosystem protection can allow forests to recover to maturity. The remaining 39% (87 Gt C) of potential lies in regions in which forests have been removed or fragmented. Although forests cannot be a substitute for emissions reductions, our results support the idea2,3,9 that the conservation, restoration and sustainable management of diverse forests offer valuable contributions to meeting global climate and biodiversity targets.

Diagnosing destabilization risk in global land carbon sinks.

Global net land carbon uptake or net biome production (NBP) has increased during recent decades1. Whether its temporal variability and autocorrelation have changed during this period, however, remains elusive, even though an increase in both could indicate an increased potential for a destabilized carbon sink2,3. Here, we investigate the trends and controls of net terrestrial carbon uptake and its temporal variability and autocorrelation from 1981 to 2018 using two atmospheric-inversion models, the amplitude of the seasonal cycle of atmospheric CO2 concentration derived from nine monitoring stations distributed across the Pacific Ocean and dynamic global vegetation models. We find that annual NBP and its interdecadal variability increased globally whereas temporal autocorrelation decreased. We observe a separation of regions characterized by increasingly variable NBP, associated with warm regions and increasingly variable temperatures, lower and weaker positive trends in NBP and regions where NBP became stronger and less variable. Plant species richness presented a concave-down parabolic spatial relationship with NBP and its variability at the global scale whereas nitrogen deposition generally increased NBP. Increasing temperature and its increasing variability appear as the most important drivers of declining and increasingly variable NBP. Our results show increasing variability of NBP regionally that can be mostly attributed to climate change and that may point to destabilization of the coupled carbon-climate system.

Increasingly negative tropical water-interannual CO2 growth rate coupling.

Terrestrial ecosystems have taken up about 32% of the total anthropogenic CO2 emissions in the past six decades1. Large uncertainties in terrestrial carbon-climate feedbacks, however, make it difficult to predict how the land carbon sink will respond to future climate change2. Interannual variations in the atmospheric CO2 growth rate (CGR) are dominated by land-atmosphere carbon fluxes in the tropics, providing an opportunity to explore land carbon-climate interactions3-6. It is thought that variations in CGR are largely controlled by temperature7-10 but there is also evidence for a tight coupling between water availability and CGR11. Here, we use a record of global atmospheric CO2, terrestrial water storage and precipitation data to investigate changes in the interannual relationship between tropical land climate conditions and CGR under a changing climate. We find that the interannual relationship between tropical water availability and CGR became increasingly negative during 1989-2018 compared to 1960-1989. This could be related to spatiotemporal changes in tropical water availability anomalies driven by shifts in El Niño/Southern Oscillation teleconnections, including declining spatial compensatory water effects9. We also demonstrate that most state-of-the-art coupled Earth System and Land Surface models do not reproduce the intensifying water-carbon coupling. Our results indicate that tropical water availability is increasingly controlling the interannual variability of the terrestrial carbon cycle and modulating tropical terrestrial carbon-climate feedbacks.

The evolution of the marine carbonate factory.

Calcium carbonate formation is the primary pathway by which carbon is returned from the ocean-atmosphere system to the solid Earth1,2. The removal of dissolved inorganic carbon from seawater by precipitation of carbonate minerals-the marine carbonate factory-plays a critical role in shaping marine biogeochemical cycling1,2. A paucity of empirical constraints has led to widely divergent views on how the marine carbonate factory has changed over time3-5. Here we use geochemical insights from stable strontium isotopes to provide a new perspective on the evolution of the marine carbonate factory and carbonate mineral saturation states. Although the production of carbonates in the surface ocean and in shallow seafloor settings have been widely considered the predominant carbonate sinks for most of the history of the Earth6, we propose that alternative processes-such as porewater production of authigenic carbonates-may have represented a major carbonate sink throughout the Precambrian. Our results also suggest that the rise of the skeletal carbonate factory decreased seawater carbonate saturation states.

Global hotspots of salt marsh change and carbon emissions.

Salt marshes provide ecosystem services such as carbon sequestration1, coastal protection2, sea-level-rise (SLR) adaptation3 and recreation4. SLR5, storm events6, drainage7 and mangrove encroachment8 are known drivers of salt marsh loss. However, the global magnitude and location of changes in salt marsh extent remains uncertain. Here we conduct a global and systematic change analysis of Landsat satellite imagery from the years 2000-2019 to quantify the loss, gain and recovery of salt marsh ecosystems and then estimate the impact of these changes on blue carbon stocks. We show a net salt marsh loss globally, equivalent to an area double the size of Singapore (719 km2), with a loss rate of 0.28% year-1 from 2000 to 2019. Net global losses resulted in 16.3 (0.4-33.2, 90% confidence interval) Tg CO2e year-1 emissions from 2000 to 2019 and a 0.045 (-0.14-0.115) Tg CO2e year-1 reduction of carbon burial. Russia and the USA accounted for 64% of salt marsh losses, driven by hurricanes and coastal erosion. Our findings highlight the vulnerability of salt marsh systems to climatic changes such as SLR and intensification of storms and cyclones.

High aboveground carbon stock of African tropical montane forests.

Tropical forests store 40-50 per cent of terrestrial vegetation carbon1. However, spatial variations in aboveground live tree biomass carbon (AGC) stocks remain poorly understood, in particular in tropical montane forests2. Owing to climatic and soil changes with increasing elevation3, AGC stocks are lower in tropical montane forests compared with lowland forests2. Here we assemble and analyse a dataset of structurally intact old-growth forests (AfriMont) spanning 44 montane sites in 12 African countries. We find that montane sites in the AfriMont plot network have a mean AGC stock of 149.4 megagrams of carbon per hectare (95% confidence interval 137.1-164.2), which is comparable to lowland forests in the African Tropical Rainforest Observation Network4 and about 70 per cent and 32 per cent higher than averages from plot networks in montane2,5,6 and lowland7 forests in the Neotropics, respectively. Notably, our results are two-thirds higher than the Intergovernmental Panel on Climate Change default values for these forests in Africa8. We find that the low stem density and high abundance of large trees of African lowland forests4 is mirrored in the montane forests sampled. This carbon store is endangered: we estimate that 0.8 million hectares of old-growth African montane forest have been lost since 2000. We provide country-specific montane forest AGC stock estimates modelled from our plot network to help to guide forest conservation and reforestation interventions. Our findings highlight the need for conserving these biodiverse9,10 and carbon-rich ecosystems.

Deep-mantle krypton reveals Earth's early accretion of carbonaceous matter.

Establishing when, and from where, carbon, nitrogen and water were delivered to Earth is a fundamental objective in understanding the origin of habitable planets such as Earth. Yet, volatile delivery to Earth remains controversial1-5. Krypton isotopes provide insights on volatile delivery owing to their substantial isotopic variations among sources6-10, although pervasive atmospheric contamination has hampered analytical efforts. Here we present the full suite of krypton isotopes from the deep mantle of the Galápagos and Iceland plumes, which have the most primitive helium, neon and tungsten isotopic compositions11-16. Except for 86Kr, the krypton isotopic compositions are similar to a mixture of chondritic and atmospheric krypton. These results suggest early accretion of carbonaceous material by proto-Earth and rule out any combination of hydrodynamic loss with outgassing of the deep or shallow mantle to explain atmospheric noble gases. Unexpectedly, the deep-mantle sources have a deficit in the neutron-rich 86Kr relative to the average composition of carbonaceous meteorites, which suggests a nucleosynthetic anomaly. Although the relative depletion of neutron-rich isotopes on Earth compared with carbonaceous meteorites has been documented for a range of refractory elements1,17,18, our observations suggest such a depletion for a volatile element. This finding indicates that accretion of volatile and refractory elements occurred simultaneously, with krypton recording concomitant accretion of non-solar volatiles from more than one type of material, possibly including outer Solar System planetesimals.

A lithium-isotope perspective on the evolution of carbon and silicon cycles.

The evolution of the global carbon and silicon cycles is thought to have contributed to the long-term stability of Earth's climate1-3. Many questions remain, however, regarding the feedback mechanisms at play, and there are limited quantitative constraints on the sources and sinks of these elements in Earth's surface environments4-12. Here we argue that the lithium-isotope record can be used to track the processes controlling the long-term carbon and silicon cycles. By analysing more than 600 shallow-water marine carbonate samples from more than 100 stratigraphic units, we construct a new carbonate-based lithium-isotope record spanning the past 3 billion years. The data suggest an increase in the carbonate lithium-isotope values over time, which we propose was driven by long-term changes in the lithium-isotopic conditions of sea water, rather than by changes in the sedimentary alterations of older samples. Using a mass-balance modelling approach, we propose that the observed trend in lithium-isotope values reflects a transition from Precambrian carbon and silicon cycles to those characteristic of the modern. We speculate that this transition was linked to a gradual shift to a biologically controlled marine silicon cycle and the evolutionary radiation of land plants13,14.

Reducing the uncertainty in estimating soil microbial-derived carbon storage.

Soil organic carbon (SOC) is the largest carbon pool in terrestrial ecosystems and plays a crucial role in mitigating climate change and enhancing soil productivity. Microbial-derived carbon (MDC) is the main component of the persistent SOC pool. However, current formulas used to estimate the proportional contribution of MDC are plagued by uncertainties due to limited sample sizes and the neglect of bacterial group composition effects. Here, we compiled the comprehensive global dataset and employed machine learning approaches to refine our quantitative understanding of MDC contributions to total carbon storage. Our efforts resulted in a reduction in the relative standard errors in prevailing estimations by an average of 71% and minimized the effect of global variations in bacterial group compositions on estimating MDC. Our estimation indicates that MDC contributes approximately 758 Pg, representing approximately 40% of the global soil carbon stock. Our study updated the formulas of MDC estimation with improving the accuracy and preserving simplicity and practicality. Given the unique biochemistry and functioning of the MDC pool, our study has direct implications for modeling efforts and predicting the land-atmosphere carbon balance under current and future climate scenarios.

Phosphocholine-induced energy source shift alleviates mitochondrial dysfunction in lung cells caused by geospecific PM2.5 components.

Fine particulate matter (PM2.5) is globally recognized for its adverse implications on human health. Yet, remain limited the individual contribution of particular PM2.5 components to its toxicity, especially considering regional disparities. Moreover, prevention solutions for PM2.5-associated health effects are scarce. In the present study, we comprehensively characterized and compared the primary PM2.5 constituents and their altered metabolites from two locations: Taiyuan and Guangzhou. Analysis of year-long PM2.5 samples revealed 84 major components, encompassing organic carbon, elemental carbon, ions, metals, and organic chemicals. PM2.5 from Taiyuan exhibited higher contamination, associated health risks, dithiothreitol activity, and cytotoxicities than Guangzhou's counterpart. Applying metabolomics, BEAS-2B lung cells exposed to PM2.5 from both cities were screened for significant alterations. A correlation analysis revealed the metabolites altered by PM2.5 and the critical toxic PM2.5 components in both regions. Among the PM2.5-down-regulated metabolites, phosphocholine emerged as a promising intervention for PM2.5 cytotoxicities. Its supplementation effectively attenuated PM2.5-induced energy metabolism disorder and cell death via activating fatty acid oxidation and inhibiting Phospho1 expression. The highlighted toxic chemicals displayed combined toxicities, potentially counteracted by phosphocholine. Our study offered a promising functional metabolite to alleviate PM2.5-induced cellular disorder and provided insights into the geo-based variability in toxic PM2.5 components.

Patterns and trends of Northern Hemisphere snow mass from 1980 to 2018.

Warming surface temperatures have driven a substantial reduction in the extent and duration of Northern Hemisphere snow cover1-3. These changes in snow cover affect Earth's climate system via the surface energy budget, and influence freshwater resources across a large proportion of the Northern Hemisphere4-6. In contrast to snow extent, reliable quantitative knowledge on seasonal snow mass and its trend is lacking7-9. Here we use the new GlobSnow 3.0 dataset to show that the 1980-2018 annual maximum snow mass in the Northern Hemisphere was, on average, 3,062 ± 35 billion tonnes (gigatonnes). Our quantification is for March (the month that most closely corresponds to peak snow mass), covers non-alpine regions above 40° N and, crucially, includes a bias correction based on in-field snow observations. We compare our GlobSnow 3.0 estimates with three independent estimates of snow mass, each with and without the bias correction. Across the four datasets, the bias correction decreased the range from 2,433-3,380 gigatonnes (mean 2,867) to 2,846-3,062 gigatonnes (mean 2,938)-a reduction in uncertainty from 33% to 7.4%. On the basis of our bias-corrected GlobSnow 3.0 estimates, we find different continental trends over the 39-year satellite record. For example, snow mass decreased by 46 gigatonnes per decade across North America but had a negligible trend across Eurasia; both continents exhibit high regional variability. Our results enable a better estimation of the role of seasonal snow mass in Earth's energy, water and carbon budgets.

Emergent constraint on Arctic Ocean acidification in the twenty-first century.

The ongoing uptake of anthropogenic carbon by the ocean leads to ocean acidification, a process that results in a reduction in pH and in the saturation state of biogenic calcium carbonate minerals aragonite (Ωarag) and calcite (Ωcalc)1,2. Because of its naturally low Ωarag and Ωcalc (refs. 2,3), the Arctic Ocean is considered the region most susceptible to future acidification and associated ecosystem impacts4-7. However, the magnitude of projected twenty-first century acidification differs strongly across Earth system models8. Here we identify an emergent multi-model relationship between the simulated present-day density of Arctic Ocean surface waters, used as a proxy for Arctic deep-water formation, and projections of the anthropogenic carbon inventory and coincident acidification. By applying observations of sea surface density, we constrain the end of twenty-first century Arctic Ocean anthropogenic carbon inventory to 9.0 ± 1.6 petagrams of carbon and the basin-averaged Ωarag and Ωcalc to 0.76 ± 0.06 and 1.19 ± 0.09, respectively, under the high-emissions Representative Concentration Pathway 8.5 climate scenario. Our results indicate greater regional anthropogenic carbon storage and ocean acidification than previously projected3,8 and increase the probability that large parts of the mesopelagic Arctic Ocean will be undersaturated with respect to calcite by the end of the century. This increased rate of Arctic Ocean acidification, combined with rapidly changing physical and biogeochemical Arctic conditions9-11, is likely to exacerbate the impact of climate change on vulnerable Arctic marine ecosystems.

Forestation at the right time with the right species can generate persistent carbon benefits in China.

Previous evaluations on the biophysical potential of forest carbon sink have focused on forestation area distribution and the associated carbon stock for equilibrium-state forests after centuries-long growth. These approaches, however, have limited relevance for climate policies because they ignore the near-term and mid-term decadal carbon uptake dynamics and suitable forest species for forestation. This study developed a forestation roadmap to support China's "carbon neutrality" objective in 2060 by addressing three key questions of forestation: where, with what forest species, and when to afforest. The results yielded a high-confidence potential forestation map for China at a resolution of 1 km with the identified optimal native forest type or species. Our analysis revealed an additional 78 Mha suitable for forestation up to the 2060s, a 43% increase on the current forest area. Selecting forest species for maximal carbon stock in addition to maximizing local environmental suitability enabled almost a doubling in forest carbon sink potential. Progressive forestation of this area can fix a considerable amount of CO2 and compensate for the carbon sink decline in existing forests. Altogether, the entire forest ecosystem can support a persistent biophysical carbon sink potential of 0.4 Pg C y-1 by 2060 and 0.2 Pg C y-1 by 2100, offsetting 7 to 14% of the current national fossil CO2 emissions. Our research provides an example of building a forestation roadmap toward a sustained forest carbon sink, which creates a critical time window for the emission cuts required by the goal of carbon neutrality.

Increasing wildfires threaten historic carbon sink of boreal forest soils.

Boreal forest fires emit large amounts of carbon into the atmosphere primarily through the combustion of soil organic matter1-3. During each fire, a portion of this soil beneath the burned layer can escape combustion, leading to a net accumulation of carbon in forests over multiple fire events4. Climate warming and drying has led to more severe and frequent forest fires5-7, which threaten to shift the carbon balance of the boreal ecosystem from net accumulation to net loss1, resulting in a positive climate feedback8. This feedback will occur if organic-soil carbon that escaped burning in previous fires, termed 'legacy carbon', combusts. Here we use soil radiocarbon dating to quantitatively assess legacy carbon loss in the 2014 wildfires in the Northwest Territories of Canada2. We found no evidence for the combustion of legacy carbon in forests that were older than the historic fire-return interval of northwestern boreal forests9. In forests that were in dry landscapes and less than 60 years old at the time of the fire, legacy carbon that had escaped burning in the previous fire cycle was combusted. We estimate that 0.34 million hectares of young forests (<60 years) that burned in the 2014 fires could have experienced legacy carbon combustion. This implies a shift to a domain of carbon cycling in which these forests become a net source-instead of a sink-of carbon to the atmosphere over consecutive fires. As boreal wildfires continue to increase in size, frequency and intensity7, the area of young forests that experience legacy carbon combustion will probably increase and have a key role in shifting the boreal carbon balance.

Wetland carbon storage controlled by millennial-scale variation in relative sea-level rise.

Coastal wetlands (mangrove, tidal marsh and seagrass) sustain the highest rates of carbon sequestration per unit area of all natural systems1,2, primarily because of their comparatively high productivity and preservation of organic carbon within sedimentary substrates3. Climate change and associated relative sea-level rise (RSLR) have been proposed to increase the rate of organic-carbon burial in coastal wetlands in the first half of the twenty-first century4, but these carbon-climate feedback effects have been modelled to diminish over time as wetlands are increasingly submerged and carbon stores become compromised by erosion4,5. Here we show that tidal marshes on coastlines that experienced rapid RSLR over the past few millennia (in the late Holocene, from about 4,200 years ago to the present) have on average 1.7 to 3.7 times higher soil carbon concentrations within 20 centimetres of the surface than those subject to a long period of sea-level stability. This disparity increases with depth, with soil carbon concentrations reduced by a factor of 4.9 to 9.1 at depths of 50 to 100 centimetres. We analyse the response of a wetland exposed to recent rapid RSLR following subsidence associated with pillar collapse in an underlying mine and demonstrate that the gain in carbon accumulation and elevation is proportional to the accommodation space (that is, the space available for mineral and organic material accumulation) created by RSLR. Our results suggest that coastal wetlands characteristic of tectonically stable coastlines have lower carbon storage owing to a lack of accommodation space and that carbon sequestration increases according to the vertical and lateral accommodation space6 created by RSLR. Such wetlands will provide long-term mitigating feedback effects that are relevant to global climate-carbon modelling.