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  • 1
    Online Resource
    Online Resource
    Anthropogenic emissions of methane in the United States
    Proceedings of the National Academy of Sciences ; 2013
    In:  Proceedings of the National Academy of Sciences Vol. 110, No. 50 ( 2013-12-10), p. 20018-20022
    Details
    In: Proceedings of the National Academy of Sciences, Proceedings of the National Academy of Sciences, Vol. 110, No. 50 ( 2013-12-10), p. 20018-20022
    Abstract: This study quantitatively estimates the spatial distribution of anthropogenic methane sources in the United States by combining comprehensive atmospheric methane observations, extensive spatial datasets, and a high-resolution atmospheric transport model. Results show that current inventories from the US Environmental Protection Agency (EPA) and the Emissions Database for Global Atmospheric Research underestimate methane emissions nationally by a factor of ∼1.5 and ∼1.7, respectively. Our study indicates that emissions due to ruminants and manure are up to twice the magnitude of existing inventories. In addition, the discrepancy in methane source estimates is particularly pronounced in the south-central United States, where we find total emissions are ∼2.7 times greater than in most inventories and account for 24 ± 3% of national emissions. The spatial patterns of our emission fluxes and observed methane–propane correlations indicate that fossil fuel extraction and refining are major contributors (45 ± 13%) in the south-central United States. This result suggests that regional methane emissions due to fossil fuel extraction and processing could be 4.9 ± 2.6 times larger than in EDGAR, the most comprehensive global methane inventory. These results cast doubt on the US EPA’s recent decision to downscale its estimate of national natural gas emissions by 25–30%. Overall, we conclude that methane emissions associated with both the animal husbandry and fossil fuel industries have larger greenhouse gas impacts than indicated by existing inventories.
    Type of Medium: Online Resource
    ISSN: 0027-8424 , 1091-6490
    URL: Article
    DOI: 10.1073/pnas.1314392110
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    Language: English
    Publisher: Proceedings of the National Academy of Sciences
    Publication Date: 2013
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  • 2
    Online Resource
    Online Resource
    Seasonal fluxes of carbonyl sulfide in a midlatitude forest
    Proceedings of the National Academy of Sciences ; 2015
    In:  Proceedings of the National Academy of Sciences Vol. 112, No. 46 ( 2015-11-17), p. 14162-14167
    Details
    In: Proceedings of the National Academy of Sciences, Proceedings of the National Academy of Sciences, Vol. 112, No. 46 ( 2015-11-17), p. 14162-14167
    Abstract: Carbonyl sulfide (OCS), the most abundant sulfur gas in the atmosphere, has a summer minimum associated with uptake by vegetation and soils, closely correlated with CO 2 . We report the first direct measurements to our knowledge of the ecosystem flux of OCS throughout an annual cycle, at a mixed temperate forest. The forest took up OCS during most of the growing season with an overall uptake of 1.36 ± 0.01 mol OCS per ha (43.5 ± 0.5 g S per ha, 95% confidence intervals) for the year. Daytime fluxes accounted for 72% of total uptake. Both soils and incompletely closed stomata in the canopy contributed to nighttime fluxes. Unexpected net OCS emission occurred during the warmest weeks in summer. Many requirements necessary to use fluxes of OCS as a simple estimate of photosynthesis were not met because OCS fluxes did not have a constant relationship with photosynthesis throughout an entire day or over the entire year. However, OCS fluxes provide a direct measure of ecosystem-scale stomatal conductance and mesophyll function, without relying on measures of soil evaporation or leaf temperature, and reveal previously unseen heterogeneity of forest canopy processes. Observations of OCS flux provide powerful, independent means to test and refine land surface and carbon cycle models at the ecosystem scale.
    Type of Medium: Online Resource
    ISSN: 0027-8424 , 1091-6490
    URL: Article
    DOI: 10.1073/pnas.1504131112
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    Language: English
    Publisher: Proceedings of the National Academy of Sciences
    Publication Date: 2015
    detail.hit.zdb_id: 209104-5
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  • 3
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    Online Resource
    Preserving Montreal Protocol Climate Benefits by Limiting HFCs
    American Association for the Advancement of Science (AAAS) ; 2012
    In:  Science Vol. 335, No. 6071 ( 2012-02-24), p. 922-923
    Details
    In: Science, American Association for the Advancement of Science (AAAS), Vol. 335, No. 6071 ( 2012-02-24), p. 922-923
    Abstract: The Montreal Protocol is perhaps the most successful international environmental treaty, responsible for global phaseout of the consumption and production of ozone-depleting substances (ODSs), e.g., chlorofluorocarbons (CFCs) and hydrochlorofluorocarbons (HCFCs). Hydrofluorocarbons (HFCs), which do not destroy stratospheric ozone, were considered long-term substitutes for ODSs and are not controlled by the Montreal Protocol. Because most HFCs are potent greenhouse gases (GHGs), they are included in the Kyoto Protocol. But climate benefits provided by this protocol are limited as they apply only to developed countries and over a short time (2008–2012). As we describe below, with no impending global controls on HFCs, inclusion of HFCs under the Montreal Protocol offers a path, starting in the short term, to preserve the climate benefits already achieved by this protocol.
    Type of Medium: Online Resource
    ISSN: 0036-8075 , 1095-9203
    URL: Article
    DOI: 10.1126/science.1216414
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    Language: English
    Publisher: American Association for the Advancement of Science (AAAS)
    Publication Date: 2012
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  • 4
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    Online Resource
    A Net Sink for Atmospheric CH 3 Br in the East Pacific Ocean
    American Association for the Advancement of Science (AAAS) ; 1995
    In:  Science Vol. 267, No. 5200 ( 1995-02-17), p. 1002-1005
    Details
    In: Science, American Association for the Advancement of Science (AAAS), Vol. 267, No. 5200 ( 1995-02-17), p. 1002-1005
    Type of Medium: Online Resource
    ISSN: 0036-8075 , 1095-9203
    URL: Article
    DOI: 10.1126/science.267.5200.1002
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    Language: English
    Publisher: American Association for the Advancement of Science (AAAS)
    Publication Date: 1995
    detail.hit.zdb_id: 128410-1
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  • 5
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    Online Resource
    COS-derived GPP relationships with temperature and light help explain high-latitude atmospheric CO 2 seasonal cycle amplification
    Proceedings of the National Academy of Sciences ; 2021
    In:  Proceedings of the National Academy of Sciences Vol. 118, No. 33 ( 2021-08-17)
    Details
    In: Proceedings of the National Academy of Sciences, Proceedings of the National Academy of Sciences, Vol. 118, No. 33 ( 2021-08-17)
    Abstract: In the Arctic and Boreal region (ABR) where warming is especially pronounced, the increase of gross primary production (GPP) has been suggested as an important driver for the increase of the atmospheric CO 2 seasonal cycle amplitude (SCA). However, the role of GPP relative to changes in ecosystem respiration (ER) remains unclear, largely due to our inability to quantify these gross fluxes on regional scales. Here, we use atmospheric carbonyl sulfide (COS) measurements to provide observation-based estimates of GPP over the North American ABR. Our annual GPP estimate is 3.6 (2.4 to 5.5) PgC · y −1 between 2009 and 2013, the uncertainty of which is smaller than the range of GPP estimated from terrestrial ecosystem models (1.5 to 9.8 PgC · y −1 ). Our COS-derived monthly GPP shows significant correlations in space and time with satellite-based GPP proxies, solar-induced chlorophyll fluorescence, and near-infrared reflectance of vegetation. Furthermore, the derived monthly GPP displays two different linear relationships with soil temperature in spring versus autumn, whereas the relationship between monthly ER and soil temperature is best described by a single quadratic relationship throughout the year. In spring to midsummer, when GPP is most strongly correlated with soil temperature, our results suggest the warming-induced increases of GPP likely exceeded the increases of ER over the past four decades. In autumn, however, increases of ER were likely greater than GPP due to light limitations on GPP, thereby enhancing autumn net carbon emissions. Both effects have likely contributed to the atmospheric CO 2 SCA amplification observed in the ABR.
    Type of Medium: Online Resource
    ISSN: 0027-8424 , 1091-6490
    URL: Article
    DOI: 10.1073/pnas.2103423118
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    Language: English
    Publisher: Proceedings of the National Academy of Sciences
    Publication Date: 2021
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  • 6
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    Online Resource
    Toward a better understanding and quantification of methane emissions from shale gas development
    Proceedings of the National Academy of Sciences ; 2014
    In:  Proceedings of the National Academy of Sciences Vol. 111, No. 17 ( 2014-04-29), p. 6237-6242
    Details
    In: Proceedings of the National Academy of Sciences, Proceedings of the National Academy of Sciences, Vol. 111, No. 17 ( 2014-04-29), p. 6237-6242
    Abstract: The identification and quantification of methane emissions from natural gas production has become increasingly important owing to the increase in the natural gas component of the energy sector. An instrumented aircraft platform was used to identify large sources of methane and quantify emission rates in southwestern PA in June 2012. A large regional flux, 2.0–14 g CH 4 s −1 km −2 , was quantified for a ∼2,800-km 2 area, which did not differ statistically from a bottom-up inventory, 2.3–4.6 g CH 4 s −1 km −2 . Large emissions averaging 34 g CH 4 /s per well were observed from seven well pads determined to be in the drilling phase, 2 to 3 orders of magnitude greater than US Environmental Protection Agency estimates for this operational phase. The emissions from these well pads, representing ∼1% of the total number of wells, account for 4–30% of the observed regional flux. More work is needed to determine all of the sources of methane emissions from natural gas production, to ascertain why these emissions occur and to evaluate their climate and atmospheric chemistry impacts.
    Type of Medium: Online Resource
    ISSN: 0027-8424 , 1091-6490
    URL: Article
    DOI: 10.1073/pnas.1316546111
    RVK:
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    Language: English
    Publisher: Proceedings of the National Academy of Sciences
    Publication Date: 2014
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  • 7
    Online Resource
    Online Resource
    Continued emissions of carbon tetrachloride from the United States nearly two decades after its phaseout for dispersive uses
    Proceedings of the National Academy of Sciences ; 2016
    In:  Proceedings of the National Academy of Sciences Vol. 113, No. 11 ( 2016-03-15), p. 2880-2885
    Details
    In: Proceedings of the National Academy of Sciences, Proceedings of the National Academy of Sciences, Vol. 113, No. 11 ( 2016-03-15), p. 2880-2885
    Abstract: National-scale emissions of carbon tetrachloride (CCl 4 ) are derived based on inverse modeling of atmospheric observations at multiple sites across the United States from the National Oceanic and Atmospheric Administration’s flask air sampling network. We estimate an annual average US emission of 4.0 (2.0–6.5) Gg CCl 4 y −1 during 2008–2012, which is almost two orders of magnitude larger than reported to the US Environmental Protection Agency (EPA) Toxics Release Inventory (TRI) (mean of 0.06 Gg y −1 ) but only 8% (3–22%) of global CCl 4 emissions during these years. Emissive regions identified by the observations and consistently shown in all inversion results include the Gulf Coast states, the San Francisco Bay Area in California, and the Denver area in Colorado. Both the observation-derived emissions and the US EPA TRI identified Texas and Louisiana as the largest contributors, accounting for one- to two-thirds of the US national total CCl 4 emission during 2008–2012. These results are qualitatively consistent with multiple aircraft and ship surveys conducted in earlier years, which suggested significant enhancements in atmospheric mole fractions measured near Houston and surrounding areas. Furthermore, the emission distribution derived for CCl 4 throughout the United States is more consistent with the distribution of industrial activities included in the TRI than with the distribution of other potential CCl 4 sources such as uncapped landfills or activities related to population density (e.g., use of chlorine-containing bleach).
    Type of Medium: Online Resource
    ISSN: 0027-8424 , 1091-6490
    URL: Article
    DOI: 10.1073/pnas.1522284113
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    Language: English
    Publisher: Proceedings of the National Academy of Sciences
    Publication Date: 2016
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  • 8
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    Online Resource
    Global emissions of refrigerants HCFC-22 and HFC-134a: Unforeseen seasonal contributions
    Proceedings of the National Academy of Sciences ; 2014
    In:  Proceedings of the National Academy of Sciences Vol. 111, No. 49 ( 2014-12-09), p. 17379-17384
    Details
    In: Proceedings of the National Academy of Sciences, Proceedings of the National Academy of Sciences, Vol. 111, No. 49 ( 2014-12-09), p. 17379-17384
    Abstract: HCFC-22 (CHClF 2 ) and HFC-134a (CH 2 FCF 3 ) are two major gases currently used worldwide in domestic and commercial refrigeration and air conditioning. HCFC-22 contributes to stratospheric ozone depletion, and both species are potent greenhouse gases. In this work, we study in situ observations of HCFC-22 and HFC-134a taken from research aircraft over the Pacific Ocean in a 3-y span [HIaper-Pole-to-Pole Observations (HIPPO) 2009–2011] and combine these data with long-term ground observations from global surface sites [National Oceanic and Atmospheric Administration (NOAA) and Advanced Global Atmospheric Gases Experiment (AGAGE) networks] . We find the global annual emissions of HCFC-22 and HFC-134a have increased substantially over the past two decades. Emissions of HFC-134a are consistently higher compared with the United Nations Framework Convention on Climate Change (UNFCCC) inventory since 2000, by 60% more in recent years (2009–2012). Apart from these decadal emission constraints, we also quantify recent seasonal emission patterns showing that summertime emissions of HCFC-22 and HFC-134a are two to three times higher than wintertime emissions. This unforeseen large seasonal variation indicates that unaccounted mechanisms controlling refrigerant gas emissions are missing in the existing inventory estimates. Possible mechanisms enhancing refrigerant losses in summer are ( i ) higher vapor pressure in the sealed compartment of the system at summer high temperatures and ( ii ) more frequent use and service of refrigerators and air conditioners in summer months. Our results suggest that engineering (e.g., better temperature/vibration-resistant system sealing and new system design of more compact/efficient components) and regulatory (e.g., reinforcing system service regulations) steps to improve containment of these gases from working devices could effectively reduce their release to the atmosphere.
    Type of Medium: Online Resource
    ISSN: 0027-8424 , 1091-6490
    URL: Article
    DOI: 10.1073/pnas.1417372111
    RVK:
    TA 1000
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    Language: English
    Publisher: Proceedings of the National Academy of Sciences
    Publication Date: 2014
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  • 9
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    Role of atmospheric oxidation in recent methane growth
    Proceedings of the National Academy of Sciences ; 2017
    In:  Proceedings of the National Academy of Sciences Vol. 114, No. 21 ( 2017-05-23), p. 5373-5377
    Details
    In: Proceedings of the National Academy of Sciences, Proceedings of the National Academy of Sciences, Vol. 114, No. 21 ( 2017-05-23), p. 5373-5377
    Abstract: The growth in global methane (CH 4 ) concentration, which had been ongoing since the industrial revolution, stalled around the year 2000 before resuming globally in 2007. We evaluate the role of the hydroxyl radical (OH), the major CH 4 sink, in the recent CH 4 growth. We also examine the influence of systematic uncertainties in OH concentrations on CH 4 emissions inferred from atmospheric observations. We use observations of 1,1,1-trichloroethane (CH 3 CCl 3 ), which is lost primarily through reaction with OH, to estimate OH levels as well as CH 3 CC 3 emissions, which have uncertainty that previously limited the accuracy of OH estimates. We find a 64–70% probability that a decline in OH has contributed to the post-2007 methane rise. Our median solution suggests that CH 4 emissions increased relatively steadily during the late 1990s and early 2000s, after which growth was more modest. This solution obviates the need for a sudden statistically significant change in total CH 4 emissions around the year 2007 to explain the atmospheric observations and can explain some of the decline in the atmospheric 13 CH 4 / 12 CH 4 ratio and the recent growth in C 2 H 6 . Our approach indicates that significant OH-related uncertainties in the CH 4 budget remain, and we find that it is not possible to implicate, with a high degree of confidence, rapid global CH 4 emissions changes as the primary driver of recent trends when our inferred OH trends and these uncertainties are considered.
    Type of Medium: Online Resource
    ISSN: 0027-8424 , 1091-6490
    URL: Article
    DOI: 10.1073/pnas.1616426114
    RVK:
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    Language: English
    Publisher: Proceedings of the National Academy of Sciences
    Publication Date: 2017
    detail.hit.zdb_id: 209104-5
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  • 10
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    Decline in the Tropospheric Abundance of Halogen from Halocarbons: Implications for Stratospheric Ozone Depletion
    American Association for the Advancement of Science (AAAS) ; 1996
    In:  Science Vol. 272, No. 5266 ( 1996-05-31), p. 1318-1322
    Details
    In: Science, American Association for the Advancement of Science (AAAS), Vol. 272, No. 5266 ( 1996-05-31), p. 1318-1322
    Type of Medium: Online Resource
    ISSN: 0036-8075 , 1095-9203
    URL: Article
    DOI: 10.1126/science.272.5266.1318
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    Language: English
    Publisher: American Association for the Advancement of Science (AAAS)
    Publication Date: 1996
    detail.hit.zdb_id: 128410-1
    detail.hit.zdb_id: 2066996-3
    detail.hit.zdb_id: 2060783-0
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