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1.
Proc Natl Acad Sci U S A ; 120(17): e2217900120, 2023 Apr 25.
Artigo em Inglês | MEDLINE | ID: mdl-37068241

RESUMO

The United States is the world's largest oil/gas methane emitter according to current national reports. Reducing these emissions is a top priority in the US government's climate action plan. Here, we use a 2010 to 2019 high-resolution inversion of surface and satellite observations of atmospheric methane to quantify emission trends for individual oil/gas production regions in North America and relate them to production and infrastructure. We estimate a mean US oil/gas methane emission of 14.8 (12.4 to 16.5) Tg a-1 for 2010 to 2019, 70% higher than reported by the US Environmental Protection Agency. While emissions in Canada and Mexico decreased over the period, US emissions increased from 2010 to 2014, decreased until 2017, and rose again afterward. Increases were driven by the largest production regions (Permian, Anadarko, Marcellus), while emissions in the smaller production regions generally decreased. Much of the year-to-year emission variability can be explained by oil/gas production rates, active well counts, and new wells drilled, with the 2014 to 2017 decrease driven by reduction in new wells and the 2017 to 2019 surge driven by upswing of production. We find a steady decrease in the oil/gas methane intensity (emission per unit methane gas production) for almost all major US production regions. The mean US methane intensity decreased from 3.7% in 2010 to 2.5% in 2019. If the methane intensity for the oil/gas supply chain continues to decrease at this pace, we may expect a 32% decrease in US oil/gas emissions by 2030 despite projected increases in production.

2.
Proc Natl Acad Sci U S A ; 114(45): 12081-12085, 2017 11 07.
Artigo em Inglês | MEDLINE | ID: mdl-29078277

RESUMO

Nitrous oxide (N2O) has a global warming potential that is 300 times that of carbon dioxide on a 100-y timescale, and is of major importance for stratospheric ozone depletion. The climate sensitivity of N2O emissions is poorly known, which makes it difficult to project how changing fertilizer use and climate will impact radiative forcing and the ozone layer. Analysis of 6 y of hourly N2O mixing ratios from a very tall tower within the US Corn Belt-one of the most intensive agricultural regions of the world-combined with inverse modeling, shows large interannual variability in N2O emissions (316 Gg N2O-N⋅y-1 to 585 Gg N2O-N⋅y-1). This implies that the regional emission factor is highly sensitive to climate. In the warmest year and spring (2012) of the observational period, the emission factor was 7.5%, nearly double that of previous reports. Indirect emissions associated with runoff and leaching dominated the interannual variability of total emissions. Under current trends in climate and anthropogenic N use, we project a strong positive feedback to warmer and wetter conditions and unabated growth of regional N2O emissions that will exceed 600 Gg N2O-N⋅y-1, on average, by 2050. This increasing emission trend in the US Corn Belt may represent a harbinger of intensifying N2O emissions from other agricultural regions. Such feedbacks will pose a major challenge to the Paris Agreement, which requires large N2O emission mitigation efforts to achieve its goals.

3.
ACS Nano ; 2024 Feb 09.
Artigo em Inglês | MEDLINE | ID: mdl-38334290

RESUMO

LiBH4 is one of the most promising candidates for use in all-solid-state lithium batteries. However, the main challenges of LiBH4 are the poor Li-ion conductivity at room temperature, excessive dendrite formation, and the narrow voltage window, which hamper practical application. Herein, we fabricate a flexible polymeric electronic shielding layer on the particle surfaces of LiBH4. The electronic conductivity of the primary LiBH4 is reduced by 2 orders of magnitude, to 1.15 × 10-9 S cm-1 at 25 °C, due to the high electron affinity of the electronic shielding layer; this localizes the electrons around the BH4- anions, which eliminates electronic leakage from the anionic framework and leads to a 68-fold higher critical electrical bias for dendrite growth on the particle surfaces. Contrary to the previously reported work, the shielding layer also ensures fast Li-ion conduction due to the fast-rotational dynamics of the BH4- species and the high Li-ion (carrier) concentration on the particle surfaces. In addition, the flexibility of the layer guarantees its structural integrity during Li plating and stripping. Therefore, our LiBH4-based solid-state electrolyte exhibits a high critical current density (11.43 mA cm-2) and long cycling stability of 5000 h (5.70 mA cm-2) at 25 °C. More importantly, the electrolyte had a wide operational temperature window (-30-150 °C). We believe that our findings provide a perspective with which to avoid dendrite formation in hydride solid-state electrolytes and provide high-performance all-solid-state lithium batteries.

4.
Nat Commun ; 14(1): 4948, 2023 Aug 16.
Artigo em Inglês | MEDLINE | ID: mdl-37587101

RESUMO

Reducing methane emissions from fossil fuel exploitation (oil, gas, coal) is an important target for climate policy, but current national emission inventories submitted to the United Nations Framework Convention on Climate Change (UNFCCC) are highly uncertain. Here we use 22 months (May 2018-Feb 2020) of satellite observations from the TROPOMI instrument to better quantify national emissions worldwide by inverse analysis at up to 50 km resolution. We find global emissions of 62.7 ± 11.5 (2σ) Tg a-1 for oil-gas and 32.7 ± 5.2 Tg a-1 for coal. Oil-gas emissions are 30% higher than the global total from UNFCCC reports, mainly due to under-reporting by the four largest emitters including the US, Russia, Venezuela, and Turkmenistan. Eight countries have methane emission intensities from the oil-gas sector exceeding 5% of their gas production (20% for Venezuela, Iraq, and Angola), and lowering these intensities to the global average level of 2.4% would reduce global oil-gas emissions by 11 Tg a-1 or 18%.

5.
Adv Mater ; 35(45): e2304285, 2023 Nov.
Artigo em Inglês | MEDLINE | ID: mdl-37487246

RESUMO

LiBH4 is a promising solid-state electrolyte (SE) due to its thermodynamic stability to Li. However, poor Li-ion conductivities at room temperature, low oxidative stabilities, and severe dendrite growth hamper its application. In this work, a partial dehydrogenation strategy is adopted to in situ generate an electronic blocking layer dispersed of LiH, addressing the above three issues simultaneously. The electrically insulated LiH reduces the electronic conductivity by two orders of magnitude, leading to a 32.0-times higher critical electrical bias for dendrite growth on the particle surfaces than that of the counterpart. Additionally, this layer not only promotes the Li-ion conductance by stimulating coordinated rotations of BH4 - and B12 H12 2- , contributing to a Li-ion conductivity of 1.38 × 10-3 S cm-1 at 25 °C, but also greatly enhances oxidation stability by localizing the electron density on BH4 - , extending its voltage window to 6.0 V. Consequently, this electrolyte exhibits an unprecedented critical current density (CCD) of 15.12 mA cm-2 at 25 °C, long-term Li plating and stripping stability for 2700 h, and a wide temperature window for dendrite inhibition from -30 to 150 °C. Its Li-LiCoO2 cell displays high reversibility within 3.0-5.0 V. It is believed that this work provides a clear direction for solid-state hydride electrolytes.

6.
J Environ Qual ; 51(3): 312-324, 2022 May.
Artigo em Inglês | MEDLINE | ID: mdl-35357715

RESUMO

Changing precipitation has the potential to alter nitrous oxide (N2 O) emissions from agricultural regions. In this study, we applied the Coupled Model Intercomparison Project Phase 5 end-of-century RCP 8.5 (business as usual) precipitation projections for the U.S. Upper Midwest and examined the effects of mean precipitation changes, characterized by increased early-season rainfall and decreased mid- to late-season rainfall, on N2 O emissions from a conventionally managed corn (Zea mays L.) cropping system grown in an indoor mesocosm facility over four growing seasons. We also assessed the response of N2 O emissions to over 1,000 individual rain events. Nitrous oxide emissions were most strongly correlated with water-filled pore space (WFPS) and soil nitrogen (N) status. After rain events, the change in N2 O emissions, relative to pre-rain emissions, was more likely to be positive when soil NO3 - was >40 mg N kg-1 soil and soil NH4 + was >10 mg N kg-1 soil and was more likely to be negative when soil NO3 - was >40 mg N kg-1 soil and soil NH4 + was <10 mg N kg-1 soil. Similarly, hourly N2 O emissions remained <5 nmol m- 2 s-1 when combined NH4 + + NO3 - was <20 mg N kg-1 soil or NH4 + and NO3 - were <5 and 20 mg N kg-1 soil, respectively. Rain event magnitude did not substantially affect the change in N2 O flux. Finally, growing-season N2 O emissions, soil moisture, and inorganic N content were not affected by the future precipitation pattern. Near-optimal soil WFPS combined with soil N concentrations above the identified thresholds favor higher N2 O emissions.


Assuntos
Óxido Nitroso , Solo , Agricultura , Nitrogênio/análise , Óxido Nitroso/análise , Chuva , Água , Zea mays
7.
J Geophys Res Biogeosci ; 123(2): 646-659, 2018 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-33614365

RESUMO

The methane (CH4) budget and its source partitioning are poorly constrained in the Midwestern United States. We used tall tower (185 m) aerodynamic flux measurements and atmospheric scale factor Bayesian inversions to constrain the monthly budget and to partition the total budget into natural (e.g., wetlands) and anthropogenic (e.g., livestock, waste, and natural gas) sources for the period June 2016 to September 2017. Aerodynamic flux observations indicated that the landscape was a CH4 source with a mean annual CH4 flux of +13.7 ± 0.34 nmol m-2 s-1 and was rarely a net sink. The scale factor Bayesian inversion analyses revealed a mean annual source of +12.3 ± 2.1 nmol m-2 s-1. Flux partitioning revealed that the anthropogenic source (7.8 ± 1.6 Tg CH4 yr-1) was 1.5 times greater than the bottom-up gridded United States Environmental Protection Agency inventory, in which livestock and oil/gas sources were underestimated by 1.8-fold and 1.3-fold, respectively. Wetland emissions (4.0 ± 1.2 Tg CH4 yr-1) were the second largest source, accounting for 34% of the total budget. The temporal variability of total CH4 emissions was dominated by wetlands with peak emissions occurring in August. In contrast, emissions from oil/gas and other anthropogenic sources showed relatively weak seasonality.

8.
IEEE Trans Image Process ; 21(11): 4581-92, 2012 Nov.
Artigo em Inglês | MEDLINE | ID: mdl-22736647

RESUMO

In environmental monitoring applications, having multiple cameras focus on common scenery increases robustness of the system. To save energy based on user demand, successive refinement image coding is important, as it allows us to progressively request better image quality. By exploiting the broadcast nature and correlation between multiview images, we investigate a two-camera setup and propose a novel two-encoder successive refinement scheme which imitates a ping-pong game. For the bivariate Gaussian case, we prove that this scheme is successively refinable on the theoretical rate-distortion limit of distributed coding (Wagner surface) under arbitrary settings. For stereo-view images, we develop a practical successive refinement coding algorithm using the same idea. The simulation results show that this scheme operates close to the distributed coding bound.

9.
Ying Yong Sheng Tai Xue Bao ; 18(1): 94-100, 2007 Jan.
Artigo em Chinês | MEDLINE | ID: mdl-17396506

RESUMO

With pot experiment and soil nitrogen desorption model, this paper studied the characteristics of nitrogen desorption in vegetable garden soil, and their effects on the NO3- -N concentration of soil leachate. The results showed that soil leachate NO3- -N concentration had a non-linear relationship with the parameters Q, Cli and C1/lamda of soil nitrogen, but the relationship became linear when these eigenvalues were relatively low. A conception of hi-curve cross point was put forward to assess the soil NO3- -N loss potential. When the eigenvalues were higher than the hi-curve cross point X0, the NO3- -N concentration in soil leachate would be increased rapidly in non-linear form, while on the contrary, the increase would be maintained at a lower level.


Assuntos
Nitratos/análise , Nitrogênio/análise , Solo/análise , Verduras/crescimento & desenvolvimento , Adsorção , Fertilizantes/análise , Nitrogênio/química , Chuva
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