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1.
Environ Sci Technol ; 2024 Feb 07.
Artigo em Inglês | MEDLINE | ID: mdl-38325813

RESUMO

Tropical wetlands contribute ∼30% of the global methane (CH4) budget. Limited observational constraints on tropical wetland CH4 emissions lead to large uncertainties and disparities in representing emissions. In this work, we combine remote sensing observations with atmospheric and wetland models to investigate dry season wetland CH4 emissions from the Pantanal region of South America. We incorporate inundation maps generated from the Cyclone Global Navigation Satellite System (CYGNSS) satellite constellation together with traditional inundation maps to generate an ensemble of wetland CH4 emission realizations. We challenge these realizations with daily satellite observations for May-July when wetland CH4 emission predictions diverge. We find that the CYGNSS inundation products predict larger emissions in May, in better agreement with observations. We use the model ensemble to generate an empirical observational constraint on CH4 emissions independent of choice of inundation map, finding large dry season wetland CH4 emissions (31.7 ± 13.6 and 32.0 ± 20.2 mg CH4/m2/day in May and June/July during 2018/2019, respectively). These May/June/July emissions are 2-3 times higher than current models, suggesting that annual wetland emissions may be higher than traditionally simulated. Observed trends in the early dry season indicate that dynamics during this period are of importance in representing tropical wetland CH4 behaviors.

2.
Environ Sci Technol ; 58(3): 1509-1517, 2024 Jan 23.
Artigo em Inglês | MEDLINE | ID: mdl-38189232

RESUMO

Natural gas flaring is a common practice employed in many United States (U.S.) oil and gas regions to dispose of gas associated with oil production. Combustion of predominantly hydrocarbon gas results in the production of nitrogen oxides (NOx). Here, we present a large field data set of in situ sampling of real world flares, quantifying flaring NOx production in major U.S. oil production regions: the Bakken, Eagle Ford, and Permian. We find that a single emission factor does not capture the range of the observed NOx emission factors within these regions. For all three regions, the median emission factors fall within the range of four emission factors used by the Texas Commission for Environmental Quality. In the Bakken and Permian, the distribution of emission factors exhibits a heavy tail such that basin-average emission factors are 2-3 times larger than the value employed by the U.S. Environmental Protection Agency. Extrapolation to basin scale emissions using auxiliary satellite assessments of flare volumes indicates that NOx emissions from flares are skewed, with 20%-30% of the flares responsible for 80% of basin-wide flaring NOx emissions. Efforts to reduce flaring volume through alternative gas capture methods would have a larger impact on the NOx oil and gas budget than current inventories indicate.


Assuntos
Poluentes Atmosféricos , Gás Natural , Estados Unidos , Poluentes Atmosféricos/análise , Gases , Texas , Óxidos de Nitrogênio
3.
Proc Natl Acad Sci U S A ; 120(15): e2215275120, 2023 Apr 11.
Artigo em Inglês | MEDLINE | ID: mdl-37011214

RESUMO

The Gulf of Mexico is the largest offshore fossil fuel production basin in the United States. Decisions on expanding production in the region legally depend on assessments of the climate impact of new growth. Here, we collect airborne observations and combine them with previous surveys and inventories to estimate the climate impact of current field operations. We evaluate all major on-site greenhouse gas emissions, carbon dioxide (CO2) from combustion, and methane from losses and venting. Using these findings, we estimate the climate impact per unit of energy of produced oil and gas (the carbon intensity). We find high methane emissions (0.60 Tg/y [0.41 to 0.81, 95% confidence interval]) exceeding inventories. This elevates the average CI of the basin to 5.3 g CO2e/MJ [4.1 to 6.7] (100-y horizon) over twice the inventories. The CI across the Gulf varies, with deep water production exhibiting a low CI dominated by combustion emissions (1.1 g CO2e/MJ), while shallow federal and state waters exhibit an extraordinarily high CI (16 and 43 g CO2e/MJ) primarily driven by methane emissions from central hub facilities (intermediaries for gathering and processing). This shows that production in shallow waters, as currently operated, has outsized climate impact. To mitigate these climate impacts, methane emissions in shallow waters must be addressed through efficient flaring instead of venting and repair, refurbishment, or abandonment of poorly maintained infrastructure. We demonstrate an approach to evaluate the CI of fossil fuel production using observations, considering all direct production emissions while allocating to all fossil products.

4.
Science ; 377(6614): 1566-1571, 2022 09 30.
Artigo em Inglês | MEDLINE | ID: mdl-36173866

RESUMO

Flaring is widely used by the fossil fuel industry to dispose of natural gas. Industry and governments generally assume that flares remain lit and destroy methane, the predominant component of natural gas, with 98% efficiency. Neither assumption, however, is based on real-world observations. We calculate flare efficiency using airborne sampling across three basins responsible for >80% of US flaring and combine these observations with unlit flare prevalence surveys. We find that both unlit flares and inefficient combustion contribute comparably to ineffective methane destruction, with flares effectively destroying only 91.1% (90.2, 91.8; 95% confidence interval) of methane. This represents a fivefold increase in methane emissions above present assumptions and constitutes 4 to 10% of total US oil and gas methane emissions, highlighting a previously underappreciated methane source and mitigation opportunity.

5.
Atmos Chem Phys ; 21(2): 951-971, 2021 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-33613665

RESUMO

We apply airborne measurements across three seasons (summer, winter and spring 2017-2018) in a multi-inversion framework to quantify methane emissions from the US Corn Belt and Upper Midwest, a key agricultural and wetland source region. Combing our seasonal results with prior fall values we find that wetlands are the largest regional methane source (32 %, 20 [16-23] Gg/d), while livestock (enteric/manure; 25 %, 15 [14-17] Gg/d) are the largest anthropogenic source. Natural gas/petroleum, waste/landfills, and coal mines collectively make up the remainder. Optimized fluxes improve model agreement with independent datasets within and beyond the study timeframe. Inversions reveal coherent and seasonally dependent spatial errors in the WetCHARTs ensemble mean wetland emissions, with an underestimate for the Prairie Pothole region but an overestimate for Great Lakes coastal wetlands. Wetland extent and emission temperature dependence have the largest influence on prediction accuracy; better representation of coupled soil temperature-hydrology effects is therefore needed. Our optimized regional livestock emissions agree well with the Gridded EPA estimates during spring (to within 7 %) but are ∼25 % higher during summer and winter. Spatial analysis further shows good top-down and bottom-up agreement for beef facilities (with mainly enteric emissions) but larger (∼30 %) seasonal discrepancies for dairies and hog farms (with >40 % manure emissions). Findings thus support bottom-up enteric emission estimates but suggest errors for manure; we propose that the latter reflects inadequate treatment of management factors including field application. Overall, our results confirm the importance of intensive animal agriculture for regional methane emissions, implying substantial mitigation opportunities through improved management.

6.
J Geophys Res Biogeosci ; 125(1)2020 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-33614366

RESUMO

Agriculture and waste are thought to account for half or more of the U.S. anthropogenic methane source. However, current bottom-up inventories contain inherent uncertainties from extrapolating limited in situ measurements to larger scales. Here, we employ new airborne methane measurements over the U.S. Corn Belt and Upper Midwest, among the most intensive agricultural regions in the world, to quantify emissions from an array of key agriculture and waste point sources. Nine of the largest concentrated animal feeding operations in the region and two sugar processing plants were measured, with multiple revisits during summer (August 2017), winter (January 2018), and spring (May-June 2018). We compare the top-down fluxes with state-of-science bottom-up estimates informed by U.S. Environmental Protection Agency methodology and site-level animal population and management practices. Top-down point source emissions are consistent with bottom-up estimates for beef concentrated animal feeding operations but moderately lower for dairies (by 37% on average) and significantly lower for sugar plants (by 80% on average). Swine facility results are more variable. The assumed bottom-up seasonality for manure methane emissions is not apparent in the aircraft measurements, which may be due to on-site management factors that are difficult to capture accurately in national-scale inventories. If not properly accounted for, such seasonal disparities could lead to source misattribution in top-down assessments of methane fluxes.

7.
Geophys Res Lett ; 46(14): 8500-8507, 2019 Jul 28.
Artigo em Inglês | MEDLINE | ID: mdl-31762518

RESUMO

Urban emissions remain an underexamined part of the methane budget. Here we present and interpret aircraft observations of six old and leak-prone major cities along the East Coast of the United States. We use direct observations of methane (CH4), carbon dioxide (CO2), carbon monoxide (CO), ethane (C2H6), and their correlations to quantify CH4 emissions and attribute to natural gas. We find the five largest cities emit 0.85 (0.63, 1.12) Tg CH4/year, of which 0.75 (0.49, 1.10) Tg CH4/year is attributed to natural gas. Our estimates, which include all thermogenic methane sources including end use, are more than twice that reported in the most recent gridded EPA inventory, which does not include end-use emissions. These results highlight that current urban inventory estimates of natural gas emissions are substantially low, either due to underestimates of leakage, lack of inclusion of end-use emissions, or some combination thereof.

8.
Appl Opt ; 57(10): 2519-2532, 2018 Apr 01.
Artigo em Inglês | MEDLINE | ID: mdl-29714236

RESUMO

We generate a supercontinuum (SC) spectrum ranging from 1.57 µm to 12 µm (20 dB bandwidth) with a soft glass fiber cascade consisting of ZrF4-BaF2-LaF3-AlF3-NaF fiber, As2S3 fiber, and As2Se3 fiber pumped by a nanosecond thulium master oscillator power amplifier system. The highest on-time average power generated is 417 mW at 33% duty cycle. We observe a near-diffraction-limit beam quality across the wavelength range from 3 µm to 12 µm, even though the As2Se3 fiber is multimode below 12 µm. Our study also shows that parameters of the As2Se3 fiber, such as numerical aperture, core size, and core/cladding composition, have significant effects on the long wavelength edge of the generated SC spectrum. Our results suggest that the high numerical aperture of 0.76 and low-loss As2Se3/GeAs2Se5 core/cladding material all contribute to broad SC generation in the long-wave infrared spectral region. Also, among our results, 10 µm core diameter selenide fiber yields the best spectral expansion, while the 12 µm core diameter selenide fiber yields the highest output power.

9.
Opt Lett ; 43(2): 296-299, 2018 Jan 15.
Artigo em Inglês | MEDLINE | ID: mdl-29328264

RESUMO

We demonstrate an all-fiber supercontinuum source that generates a continuous spectrum from 1.6 µm to >11 µm with 417 mW on-time average power at 33% duty cycle. By utilizing a master oscillator power amplifier pump with three amplification stages and concatenating solid core ZBLAN, arsenic sulfide, and arsenic selenide fibers, we shift 1550 nm light to ∼4.5 µm, ∼6.5 µm, and >11 µm, respectively. With 69 mW past 7.5 µm, this source provides both high power and broad spectral expansion, while outputting a single fundamental mode.

10.
Opt Lett ; 42(14): 2770-2773, 2017 Jul 15.
Artigo em Inglês | MEDLINE | ID: mdl-28708165

RESUMO

A proof-of-concept heterodyne-enhanced chirped laser dispersion spectroscopy system is presented. In remote sensing systems where low return powers are expected, the addition of an optical local oscillator and subsequent nonlinear processing can provide improved performance in chirped laser dispersion spectroscopy. Details about the system configuration, phase noise cancellation, and experimental verification are discussed.

11.
Sensors (Basel) ; 15(9): 21315-26, 2015 Aug 28.
Artigo em Inglês | MEDLINE | ID: mdl-26343670

RESUMO

Existing technologies for quantifying methane emissions are often limited to single point sensors, making large area environmental observations challenging. We demonstrate the operation of a remote, multi-path system using Chirped Laser Dispersion Spectroscopy (CLaDS) for quantification of atmospheric methane concentrations over extended areas, a technology that shows potential for monitoring emissions from wetlands.

12.
Appl Opt ; 54(33): 9844-7, 2015 Nov 20.
Artigo em Inglês | MEDLINE | ID: mdl-26836547

RESUMO

Utilizing the fundamentals of chirped laser dispersion spectroscopy, an alternative method of fiber dispersion measurement is presented. The dispersion of the device under test is probed through the interaction of copropagating electromagnetic waves and subsequent heterodyne detection and frequency demodulation. Measurement of the dispersion parameter, D, is possible with this direct measurement scheme.

13.
Opt Express ; 21(12): 14649-55, 2013 Jun 17.
Artigo em Inglês | MEDLINE | ID: mdl-23787653

RESUMO

We report new approaches for signal generation in Chirped Laser Dispersion Spectroscopy (CLaDS). Two optical arrangements based on electro-optical modulators significantly reduce CLaDS system complexity and enable optimum performance when applied to detection of GHz-wide molecular transitions. Proof-of-principle experiments in the near-infrared spectral range are presented and potential strategies for application in the mid-infrared are discussed.


Assuntos
Lasers , Sistemas Microeletromecânicos/instrumentação , Dispositivos Ópticos , Semicondutores , Análise Espectral/instrumentação , Telecomunicações/instrumentação , Desenho de Equipamento , Análise de Falha de Equipamento
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