A highly alkaline-stable metal oxide@metal–organic framework composite for high-performance electrochemical energy storage

Most metal–organic frameworks (MOFs) hardly maintain their physical and chemical properties after exposure to alkaline aqueous solutions, thus precluding their use as potential electrode materials for electrochemical energy storage devices. Here, we present the design and synthesis of a highly alkaline-stable metal oxide@MOF composite, Co₃O₄ nanocube@Co-MOF (Co₃O₄@Co-MOF), via a controllable and facile one-pot hydrothermal method under highly alkaline conditions. The obtained composite possesses exceptional alkaline stability, retaining its original structure in 3.0 M KOH for at least 15 days. Benefitting from the exceptional alkaline stability, unique structure, and larger surface area, the Co₃O₄@Co-MOF composite shows a specific capacitance as high as 1020 F g⁻¹ at 0.5 A  g⁻¹ and a high cycling stability with only 3.3% decay after 5000 cycles at 5 A g⁻¹. The as-constructed solid-state flexible device exhibits a maximum energy density of 21.6 mWh cm⁻³.     

A highly efficient atomically thin curved PdIr bimetallene electrocatalyst

The multi-metallene with an ultrahigh surface area has great potential in precise tuning of surface heterogeneous d-electronic correlation by surface strain effect for the distinctive surface electronic structure, which is a brand new class of promising 2D electrocatalyst for sustainable energy device application. However, achieving such an atomically thin multi-metallene still presents a great challenge. Herein, we present a new synthetic method for an atomic-level palladium-iridium (PdIr) bimetallene with an average thickness of only ∼1.0 nm for achieving superior catalysis in the hydrogen evolution reaction (HER) and the formic acid oxidation reaction (FAOR). The curved PdIr bimetallene presents a top-ranked high electrochemical active area of 127.5 ± 10.8 m² g_Pd+Ir⁻¹ in the reported noble alloy materials, and exhibits a very low overpotential, ultrahigh activity and improved stability for HER and FAOR. DFT calculation reveals that the PdIr bimetallene herein has a unique lattice tangential strain, which can induce surface distortion while concurrently creating a variety of concave-convex featured micro-active regions formed by variously coordinated Pd sites agglomeration. Such a strong strain effect correlates the abnormal on-site active 4d¹⁰-t_2g-orbital Coulomb correlation potential and directly elevates orbital-electronegativity exposure within these active regions, resulting in a preeminent barrier-free energetic path for significant enhancement of FAOR and HER catalytic performance.     

Potential-tuned selective electrosynthesis of azoxy-, azo- and amino-aromatics over a CoP nanosheet cathode

Azoxy-, azo- and amino-aromatics are among the most widely used building blocks in materials science pharmaceuticals and synthetic chemistry, but their controllable and green synthesis has not yet been well established. Herein, a facile potential-tuned electrosynthesis of azoxy-, azo- and amino-aromatics via aqueous selective reduction of nitroarene feedstocks over a CoP nanosheet cathode is developed. A series of azoxy-, azo- and amino-compounds with excellent selectivity, good functional group tolerance and high yields are produced by applying different bias input. The synthetically significant and challenging asymmetric azoxy-aromatics can be controllably synthesized in moderate to good yields. The use of water as the hydrogen source makes this strategy remarkably fascinating and promising. In addition, deuterated aromatic amines with a high deuterium content can be readily obtained by using D₂O. By pairing with anodic oxidation of aliphatic amines to nitriles, synthetically useful building blocks can be simultaneously produced in a CoP||Ni₂P two-electrode electrolyzer. Only 1.25 V is required to achieve a current density of 20 mA cm⁻², which is much lower than that of overall water splitting (1.70 V). The paired oxidation and reduction reactions can also be driven using a 1.5 V battery to synthesize nitrile and azoxybenzene with good yields and selectivity, further emphasizing the flexibility and controllability of our method. This work paves the way for a promising approach to the green synthesis of valuable chemicals through potential-controlled electrosynthesis.     

Plasmonic evolution of atomically size-selected Au clusters by electron energy loss spectrum

The plasmonic response of gold clusters with atom number (N) = 100–70 000 was investigated using scanning transmission electron microscopy-electron energy loss spectroscopy. For decreasing N, the bulk plasmon remains unchanged above N = 887 but then disappears, while the surface plasmon firstly redshifts from 2.4 to 2.3 eV above N = 887 before blueshifting towards 2.6 eV down to N = 300, and finally splitting into three fine features. The surface plasmon''s excitation ratio is found to follow N^0.669, which is essentially R². An atomically precise evolution picture of plasmon physics is thus demonstrated according to three regimes: classical plasmon (N = 887–70 000), quantum confinement corrected plasmon (N = 300–887) and molecule related plasmon (N < 300).     

Exposed facet-controlled N2 electroreduction on distinct Pt3Fe nanostructures of nanocubes,nanorods and nanowires

Understanding the correlation between exposed surfaces and performances of controlled nanocatalysts can aid effective strategies to enhance electrocatalysis, but this is as yet unexplored for the nitrogen reduction reaction (NRR). Here, we first report controlled synthesis of well-defined Pt₃Fe nanocrystals with tunable morphologies (nanocube, nanorod and nanowire) as ideal model electrocatalysts for investigating the NRR on different exposed facets. The detailed electrocatalytic studies reveal that the Pt₃Fe nanocrystals exhibit shape-dependent NRR electrocatalysis. The optimized Pt₃Fe nanowires bounded with high-index facets exhibit excellent selectivity (no N₂H₄ is detected), high activity with NH₃ yield of 18.3 μg h⁻¹ mg⁻¹_cat (0.52 μg h⁻¹ cm⁻²_ECSA; ECSA: electrochemical active surface area) and Faraday efficiency of 7.3% at −0.05 V versus reversible hydrogen electrode, outperforming the {200} facet-enclosed Pt₃Fe nanocubes and {111} facet-enclosed Pt₃Fe nanorods. They also show good stability with negligible activity change after five cycles. Density functional theory calculations reveal that, with high-indexed facet engineering, the Fe-3d band is an efficient d-d coupling correlation center for boosting the Pt 5d-electronic exchange and transfer activities towards the NRR.     

Isotopic constraints confirm the significant role of microbial nitrogen oxides emissions from the land and ocean environment

Nitrogen oxides (NO_x, the sum of nitric oxide (NO) and N dioxide (NO₂)) emissions and deposition have increased markedly over the past several decades, resulting in many adverse outcomes in both terrestrial and oceanic environments. However, because the microbial NO_x emissions have been substantially underestimated on the land and unconstrained in the ocean, the global microbial NO_x emissions and their importance relative to the known fossil-fuel NO_x emissions remain unclear. Here we complied data on stable N isotopes of nitrate in atmospheric particulates over the land and ocean to ground-truth estimates of NO_x emissions worldwide. By considering the N isotope effect of NO_x transformations to particulate nitrate combined with dominant NO_x emissions in the land (coal combustion, oil combustion, biomass burning and microbial N cycle) and ocean (oil combustion, microbial N cycle), we demonstrated that microbial NO_x emissions account for 24 ± 4%, 58 ± 3% and 31 ± 12% in the land, ocean and global environment, respectively. Corresponding amounts of microbial NO_x emissions in the land (13.6 ± 4.7 Tg N yr⁻¹), ocean (8.8 ± 1.5 Tg N yr⁻¹) and globe (22.5 ± 4.7 Tg N yr⁻¹) are about 0.5, 1.4 and 0.6 times on average those of fossil-fuel NO_x emissions in these sectors. Our findings provide empirical constraints on model predictions, revealing significant contributions of the microbial N cycle to regional NO_x emissions into the atmospheric system, which is critical information for mitigating strategies, budgeting N deposition and evaluating the effects of atmospheric NO_x loading on the world.     

Thermophysical properties of the regolith on the lunar far side revealed by the in situ temperature probing of the Chang’E-4 mission

Temperature probes onboard the Chang’E-4 (CE-4) spacecraft provide the first in situ regolith temperature measurements from the far side of the Moon. We present these temperature measurements with a customized thermal model and reveal the particle size of the lunar regolith at the CE-4 landing site to be ∼15 μm on average over depth, which indicates an immature regolith below the surface. In addition, the conductive component of thermal conductivity is measured as ∼1.53 × 10^–3 W m^–1 K^–1 on the surface and ∼8.48 × 10^–3 W m^–1 K^–1 at a depth of 1 m. The average bulk density is ∼471 kg m^–3 on the surface and ∼824 kg m^–3 in the upper 30 cm of the lunar regolith. These thermophysical properties provide important additional ‘ground truth’ at the lunar far side, which is critical for the future analysis and interpretation of global temperature observations.     

Kinetic regulation of MXene with water-in-LiCl electrolyte for high-voltage micro-supercapacitors

MXenes are one of the key materials for micro-supercapacitors (MSCs), integrating miniaturized energy-storage components with microelectronics. However, the energy densities of MSCs are greatly hampered by MXenes’ narrow working potential window (typically ≤0.6 V) in aqueous electrolytes. Here, we report the fabrication of high-voltage MXene-MSCs through the efficient regulation of reaction kinetics in 2D Ti₃C₂T_x MXene microelectrodes using a water-in-LiCl (WIL, 20 m LiCl) salt gel electrolyte. Importantly, the intrinsic energy-storage mechanism of MXene microelectrodes in WIL, which is totally different from traditional electrolytes (1 m LiCl), was revealed through insitu and exsitu characterizations. We validated that the suppression of MXene oxidation at high anodic potential occurred due to the high content of WIL regulating anion intercalation in MXene electrodes, which effectively broadened the voltage window of MXene-MSCs. Remarkably, the symmetric planar MXene-MSCs presented a record operating voltage of 1.6 V, resulting in an exceptionally high volumetric energy density of 31.7 mWh cm⁻³. With the ultra-high ionic conductivity (69.5 mS cm⁻¹) and ultralow freezing point (−57°C) of the WIL gel electrolyte, our MSCs could be operated in a wide temperature range of −40 to 60°C, and worked for a long duration even at −40°C, demonstrative of its practicality in extreme environments.     

Unprecedented and highly stable lithium storage capacity of (001) faceted nanosheet-constructed hierarchically porous TiO2/rGO hybrid architecture for high-performance Li-ion batteries

Active crystal facets can generate special properties for various applications. Herein, we report a (001) faceted nanosheet-constructed hierarchically porous TiO₂/rGO hybrid architecture with unprecedented and highly stable lithium storage performance. Density functional theory calculations show that the (001) faceted TiO₂ nanosheets enable enhanced reaction kinetics by reinforcing their contact with the electrolyte and shortening the path length of Li⁺ diffusion and insertion-extraction. The reduced graphene oxide (rGO) nanosheets in this TiO₂/rGO hybrid largely improve charge transport, while the porous hierarchy at different length scales favors continuous electrolyte permeation and accommodates volume change. This hierarchically porous TiO₂/rGO hybrid anode material demonstrates an excellent reversible capacity of 250 mAh g^–1 at 1 C (1 C = 335 mA g^–1) at a voltage window of 1.0–3.0 V. Even after 1000 cycles at 5 C and 500 cycles at 10 C, the anode retains exceptional and stable capacities of 176 and 160 mAh g^–1, respectively. Moreover, the formed Li₂Ti₂O₄ nanodots facilitate reversed Li⁺ insertion-extraction during the cycling process. The above results indicate the best performance of TiO₂-based materials as anodes for lithium-ion batteries reported in the literature.     

Mass production of 2D materials by intermediate-assisted grinding exfoliation

The scalable and high-efficiency production of 2D materials is a prerequisite to their commercial use. Currently, only graphene and graphene oxide can be produced on a ton scale, and the inability to produce other 2D materials on such a large scale hinders their technological applications. Here we report a grinding exfoliation method that uses micro-particles as force intermediates to resolve applied compressive forces into a multitude of small shear forces, inducing the highly efficient exfoliation of layer materials. The method, referred to as intermediate-assisted grinding exfoliation (iMAGE), can be used for the large-scale production of many 2D materials. As an example, we have exfoliated bulk h-BN into 2D h-BN with large flake sizes, high quality and structural integrity, with a high exfoliation yield of 67%, a high production rate of 0.3 g h⁻¹ and a low energy consumption of 3.01 × 10⁶ J g⁻¹. The production rate and energy consumption are one to two orders of magnitude better than previous results. Besides h-BN, this iMAGE technology has been used to exfoliate various layer materials such as graphite, black phosphorus, transition metal dichalcogenides, and metal oxides, proving its universality. Molybdenite concentrate, a natural low-cost and abundant mineral, was used as a demo for the large-scale exfoliation production of 2D MoS₂ flakes. Our work indicates the huge potential of the iMAGE method to produce large amounts of various 2D materials, which paves the way for their commercial application.     

Enabling Mg metal anodes rechargeable in conventional electrolytes by fast ionic transport interphase

Rechargeable magnesium batteries have received extensive attention as the Mg anodes possess twice the volumetric capacity of their lithium counterparts and are dendrite-free. However, Mg anodes suffer from surface passivation film in most glyme-based conventional electrolytes, leading to irreversible plating/stripping behavior of Mg. Here we report a facile and safe method to obtain a modified Mg metal anode with a Sn-based artificial layer via ion-exchange and alloying reactions. In the artificial coating layer, Mg₂Sn alloy composites offer a channel for fast ion transport and insulating MgCl₂/SnCl₂ bestows the necessary potential gradient to prevent deposition on the surface. Significant improved ion conductivity of the solid electrolyte interfaces and decreased overpotential of Mg symmetric cells in Mg(TFSI)₂/DME electrolyte are obtained. The coated Mg anodes can sustain a stable plating/stripping process over 4000 cycles at a high current density of 6 mA cm⁻². This finding provides an avenue to facilitate fast ion diffusion kinetics of Mg metal anodes in conventional electrolytes.     

Correlating the electronic structures of metallic/semiconducting MoTe2 interface to its atomic structures

Contact interface properties are important in determining the performances of devices that are based on atomically thin two-dimensional (2D) materials, especially for those with short channels. Understanding the contact interface is therefore important to design better devices. Herein, we use scanning transmission electron microscopy, electron energy loss spectroscopy, and first-principles calculations to reveal the electronic structures within the metallic (1T^′)-semiconducting (2H) MoTe₂ coplanar phase boundary across a wide spectral range and correlate its properties to atomic structures. We find that the 2H-MoTe₂ excitonic peaks cross the phase boundary into the 1T^′ phase within a range of approximately 150 nm. The 1T^′-MoTe₂ crystal field can penetrate the boundary and extend into the 2H phase by approximately two unit-cells. The plasmonic oscillations exhibit strong angle dependence, that is a red-shift of π+σ (approximately 0.3–1.2 eV) occurs within 4 nm at 1T^′/2H-MoTe₂ boundaries with large tilt angles, but there is no shift at zero-tilted boundaries. These atomic-scale measurements reveal the structure–property relationships of the 1T^′/2H-MoTe₂ boundary, providing useful information for phase boundary engineering and device development based on 2D materials.     

Anthropogenic emission is the main contributor to the rise of atmospheric methane during 1993–2017

Atmospheric methane (CH₄) concentrations have shown a puzzling resumption in growth since 2007 following a period of stabilization from 2000 to 2006. Multiple hypotheses have been proposed to explain the temporal variations in CH₄ growth, and attribute the rise of atmospheric CH₄ either to increases in emissions from fossil fuel activities, agriculture and natural wetlands, or to a decrease in the atmospheric chemical sink. Here, we use a comprehensive ensemble of CH₄ source estimates and isotopic δ¹³C-CH₄ source signature data to show that the resumption of CH₄ growth is most likely due to increased anthropogenic emissions. Our emission scenarios that have the fewest biases with respect to isotopic composition suggest that the agriculture, landfill and waste sectors were responsible for 53 ± 13% of the renewed growth over the period 2007–2017 compared to 2000–2006; industrial fossil fuel sources explained an additional 34 ± 24%, and wetland sources contributed the least at 13 ± 9%. The hypothesis that a large increase in emissions from natural wetlands drove the decrease in atmospheric δ¹³C-CH₄ values cannot be reconciled with current process-based wetland CH₄ models. This finding suggests the need for increased wetland measurements to better understand the contemporary and future role of wetlands in the rise of atmospheric methane and climate feedback. Our findings highlight the predominant role of anthropogenic activities in driving the growth of atmospheric CH₄ concentrations.     

Encapsulating metal organic framework into hollow mesoporous carbon sphere as efficient oxygen bifunctional electrocatalyst

Applying metal organic frameworks (MOFs) in electrochemical systems is a currently emerging field owing to the rich metal nodes and highly specific surface area of MOFs. However, the problems for MOFs that need to be solved urgently are poor electrical conductivity and low ion transport. Here we present a facile in situ growth method for the rational synthesis of MOFs@hollow mesoporous carbon spheres (HMCS) yolk–shell-structured hybrid material for the first time. The size of the encapsulated Zeolitic Imidazolate Framework-67 (ZIF-67) is well controlled to 100 nm due to the spatial confinement effect of HMCS, and the electrical conductivity of ZIF-67 is also increased significantly. The ZIF@HMCS-25% hybrid material obtained exhibits a highly efficient oxygen reduction reaction activity with 0.823 V (vs. reversible hydrogen electrode) half-wave potential and an even higher kinetic current density (J_K = 13.8 mA cm⁻²) than commercial Pt/C. ZIF@HMCS-25% also displays excellent oxygen evolution reaction performance and the overpotential of ZIF@HMCS-25% at 10 mA cm⁻² is 407 mV. In addition, ZIF@HMCS-25% is further employed as an air electrode for a rechargeable Zn–air battery, exhibiting a high power density (120.2 mW cm⁻² at 171.4 mA cm⁻²) and long-term charge/discharge stability (80 h at 5 mA cm⁻²). This MOFs@HMCS yolk–shell design provides a versatile method for the application of MOFs as electrocatalysts directly.     

The role of China's terrestrial carbon sequestration 2010–2060 in offsetting energy-related CO2 emissions

Energy consumption dominates annual CO₂ emissions in China. It is essential to significantly reduce CO₂ emissions from energy consumption to reach national carbon neutrality by 2060, while the role of terrestrial carbon sequestration in offsetting energy-related CO₂ emissions cannot be underestimated. Natural climate solutions (NCS), including improvements in terrestrial carbon sequestration, represent readily deployable options to offset anthropogenic greenhouse gas emissions. However, the extent to which China''s terrestrial carbon sequestration in the future, especially when target-oriented managements (TOMs) are implemented, can help to mitigate energy-related CO₂ emissions is far from certain. By synthesizing available findings and using several parameter-sparse empirical models that have been calibrated and/or fitted against contemporary measurements, we assessed China''s terrestrial carbon sequestration over 2010–2060 and its contribution to offsetting national energy-related CO₂ emissions. We show that terrestrial C sequestration in China will increase from 0.375 ± 0.056 (mean ± standard deviation) Pg C yr⁻¹ in the 2010s to 0.458 ± 0.100 Pg C yr⁻¹ under RCP2.6 and 0.493 ± 0.108 Pg C yr⁻¹ under the RCP4.5 scenario in the 2050s, when TOMs are implemented. The majority of carbon sequestration comes from forest, accounting for 67.8–71.4% of the total amount. China''s terrestrial ecosystems can offset 12.2–15.0% and 13.4–17.8% of energy-related peak CO₂ emissions in 2030 and 2060, respectively. The implementation of TOMs contributes 11.9% of the overall terrestrial carbon sequestration in the 2020s and 23.7% in the 2050s. The most likely strategy to maximize future NCS effectiveness is a full implementation of all applicable cost-effective NCS pathways in China. Our findings highlight the role of terrestrial carbon sequestration in offsetting energy-related CO₂ emissions and put forward future needs in the context of carbon neutrality.     

Robust prediction of hourly PM2.5 from meteorological data using LightGBM

Retrieving historical fine particulate matter (PM_2.5) data is key for evaluating the long-term impacts of PM_2.5 on the environment, human health and climate change. Satellite-based aerosol optical depth has been used to estimate PM_2.5, but estimations have largely been undermined by massive missing values, low sampling frequency and weak predictive capability. Here, using a novel feature engineering approach to incorporate spatial effects from meteorological data, we developed a robust LightGBM model that predicts PM_2.5 at an unprecedented predictive capacity on hourly (R² = 0.75), daily (R² = 0.84), monthly (R² = 0.88) and annual (R² = 0.87) timescales. By taking advantage of spatial features, our model can also construct hourly gridded networks of PM_2.5. This capability would be further enhanced if meteorological observations from regional stations were incorporated. Our results show that this model has great potential in reconstructing historical PM_2.5 datasets and real-time gridded networks at high spatial-temporal resolutions. The resulting datasets can be assimilated into models to produce long-term re-analysis that incorporates interactions between aerosols and physical processes.     

Ultra-small hollow ternary alloy nanoparticles for efficient hydrogen evolution reaction

Hollow nanoparticles with large specific surface area and high atom utilization are promising catalysts for the hydrogen evolution reaction (HER). We describe herein the design and synthesis of a series of ultra-small hollow ternary alloy nanostructures using a simple one-pot strategy. The same technique was demonstrated for hollow PtNiCu nanoparticles, hollow PtCoCu nanoparticles and hollow CuNiCo nanoparticles. During synthesis, the displacement reaction and oxidative etching played important roles in the formation of hollow structures. Moreover, our hollow PtNiCu and PtCoCu nanoparticles were single crystalline, with an average diameter of 5 nm. Impressively, ultra-small hollow PtNiCu nanoparticles, containing only 10% Pt, exhibited greater electrocatalytic HER activity and stability than a commercial Pt/C catalyst. The overpotential of hollow PtNiCu nanoparticles at 10 mA cm⁻² was 28 mV versus reversible hydrogen electrode (RHE). The mass activity was 4.54 A mg_Pt⁻¹ at −70 mV versus RHE, which is 5.62-fold greater than that of a commercial Pt/C system (0.81 A mg_Pt⁻¹). Through analyses of bonding and antibonding orbital filling, density functional theory calculations demonstrated that the bonding strength of different metals to the hydrogen intermediate (H^*) was in the order of Pt > Co > Ni > Cu. The excellent HER performance of our hollow PtNiCu nanoparticles derives from moderately synergistic interactions between the three metals and H^*. This work demonstrates a new strategy for the design of low-cost and high-activity HER catalysts.     

Integration of bio-inspired lanthanide-transition metal cluster and P-doped carbon nitride for efficient photocatalytic overall water splitting

Photosynthesis in nature uses the Mn₄CaO₅ cluster as the oxygen-evolving center to catalyze the water oxidation efficiently in photosystem II. Herein, we demonstrate bio-inspired heterometallic LnCo₃ (Ln = Nd, Eu and Ce) clusters, which can be viewed as synthetic analogs of the CaMn₄O₅ cluster. Anchoring LnCo₃ on phosphorus-doped graphitic carbon nitrides (PCN) shows efficient overall water splitting without any sacrificial reagents. The NdCo₃/PCN-c photocatalyst exhibits excellent water splitting activity and a quantum efficiency of 2.0% at 350 nm. Ultrafast transient absorption spectroscopy revealed the transfer of a photoexcited electron and hole into the PCN and LnCo₃ for hydrogen and oxygen evolution reactions, respectively. A density functional theory (DFT) calculation showed the cooperative water activation on lanthanide and O−O bond formation on transition metal for water oxidation. This work not only prepares a synthetic model of a bio-inspired oxygen-evolving center but also provides an effective strategy to realize light-driven overall water splitting.     

Efficient potential-tuning strategy through p-type doping for designing cathodes with ultrahigh energy density

Designing new cathodes with high capacity and moderate potential is the key to breaking the energy density ceiling imposed by current intercalation chemistry on rechargeable batteries. The carbonaceous materials provide high capacities but their low potentials limit their application to anodes. Here, we show that Fermi level tuning by p-type doping can be an effective way of dramatically raising electrode potential. We demonstrate that Li(Na)BCF₂/Li(Na)B₂C₂F₂ exhibit such change in Fermi level, enabling them to accommodate Li⁺(Na⁺) with capacities of 290–400 (250–320) mAh g⁻¹ at potentials of 3.4–3.7 (2.7–2.9) V, delivering ultrahigh energy densities of 1000–1500 Wh kg⁻¹. This work presents a new strategy in tuning electrode potential through electronic band structure engineering.     

Empirical estimates of regional carbon budgets imply reduced global soil heterotrophic respiration

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 2000–2009. 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.