scholarly journals Temporary pause in the growth of atmospheric ethane and propane in 2015–2018

2021 ◽  
Author(s):  
Hélène Angot ◽  
Connor Davel ◽  
Christine Wiedinmyer ◽  
Gabrielle Pétron ◽  
Jashan Chopra ◽  
...  
Keyword(s):  
Northern Hemisphere ◽  
Mole Fraction ◽  
Atmospheric Transport ◽  
Ambient Air ◽  
Potential Contribution ◽  
Back Trajectories ◽  
Oil And Natural Gas ◽  
Regional Emissions

Abstract. Atmospheric non-methane hydrocarbons (NMHCs) play an important role in the formation of secondary organic aerosols and ozone. After a multidecade global decline in atmospheric mole fractions of ethane and propane – the most abundant atmospheric NMHCs – previous work has shown a reversal of this trend with increasing atmospheric abundances from 2009 to 2015 in the Northern Hemisphere. These concentration increases were attributed to the unprecedented growth in oil and natural gas (O&NG) production in North America. Here, we supplement this trend analysis building on the long-term (2008–2010; 2012–2020) high-resolution (~3-hour) record of ambient air C2-C7 NMHCs from in-situ measurements at the Greenland Environmental Observatory at Summit station (GEOSummit, 72.58° N, 38.48° W, 3210 m above sea level). We confirm previous findings that the ethane mole fraction significantly increased by +69.0 [+47.4, +73.2; 95 % confidence interval] ppt per year from January 2010 to December 2014. Subsequent measurements, however, reveal a significant decrease by −58.4 [−64.1, −48.9] ppt per year from January 2015 to December 2018. A similar reversal is found for propane. The upturn observed after 2019 suggests, however, that the pause in the growth of atmospheric ethane and propane might only have been temporary. The analysis of 2012–2019 air mass back-trajectories shows that this pause in mole fraction increases can neither be attributed to changes in atmospheric transport nor to changes in regional emissions. Discrete samples collected at other northern-hemisphere baseline sites under the umbrella of the NOAA cooperative global air sampling network show a similar decrease in 2015–2018 and suggest a hemispheric pattern. Here, we further discuss the potential contribution of biomass burning and O&NG emissions, the main sources of ethane and propane, and we conclude that O&NG activities likely played a role in these recent changes. This study, however, highlights the crucial need for better constrained emission inventories.

scholarly journals Temporary pause in the growth of atmospheric ethane and propane in 2015–2018

2021 ◽  
Vol 21 (19) ◽  
pp. 15153-15170
Author(s):  
Hélène Angot ◽  
Connor Davel ◽  
Christine Wiedinmyer ◽  
Gabrielle Pétron ◽  
Jashan Chopra ◽  
...  
Keyword(s):  
Organic Aerosols ◽  
Ambient Air ◽  
Potential Contribution ◽  
Emission Inventories ◽  
Sampling Network ◽  
Oil And Natural Gas ◽  
Northern Hemispheric ◽  
Similar Decrease

Abstract. Atmospheric non-methane hydrocarbons (NMHCs) play an important role in the formation of secondary organic aerosols and ozone. After a multidecadal global decline in atmospheric mole fractions of ethane and propane – the most abundant atmospheric NMHCs – previous work has shown a reversal of this trend with increasing atmospheric abundances from 2009 to 2015 in the Northern Hemisphere. These concentration increases were attributed to the unprecedented growth in oil and natural gas (O&NG) production in North America. Here, we supplement this trend analysis building on the long-term (2008–2010; 2012–2020) high-resolution (∼3 h) record of ambient air C2–C7 NMHCs from in situ measurements at the Greenland Environmental Observatory at Summit station (GEOSummit, 72.58 ∘ N, 38.48 ∘ W; 3210 m above sea level). We confirm previous findings that the ethane mole fraction significantly increased by +69.0 [+47.4, +73.2; 95 % confidence interval] ppt yr−1 from January 2010 to December 2014. Subsequent measurements, however, reveal a significant decrease by −58.4 [−64.1, −48.9] ppt yr−1 from January 2015 to December 2018. A similar reversal is found for propane. The upturn observed after 2019 suggests, however, that the pause in the growth of atmospheric ethane and propane might only have been temporary. Discrete samples collected at other northern hemispheric baseline sites under the umbrella of the NOAA cooperative global air sampling network show a similar decrease in 2015–2018 and suggest a hemispheric pattern. Here, we further discuss the potential contribution of biomass burning and O&NG emissions (the main sources of ethane and propane) and conclude that O&NG activities likely played a role in these recent changes. This study highlights the crucial need for better constrained emission inventories.

scholarly journals Global emissions of HFC-143a (CH<sub>3</sub>CF<sub>3</sub>) and HFC-32 (CH<sub>2</sub>F<sub>2</sub>) from in situ and air archive atmospheric observations

2014 ◽  
Vol 14 (17) ◽  
pp. 9249-9258 ◽  
Author(s):  
S. O'Doherty ◽  
M. Rigby ◽  
J. Mühle ◽  
D. J. Ivy ◽  
B. R. Miller ◽  
...  
Keyword(s):  
Growth Rate ◽  
Mole Fraction ◽  
Radiative Forcing ◽  
Transport Model ◽  
Atmospheric Transport ◽  
Lower Troposphere ◽  
Emission Rates ◽  
Global Emission ◽  
Atmospheric Observations

Abstract. High-frequency, in situ observations from the Advanced Global Atmospheric Gases Experiment (AGAGE), for the period 2003 to 2012, combined with archive flask measurements dating back to 1977, have been used to capture the rapid growth of HFC-143a (CH3CF3) and HFC-32 (CH2F2) mole fractions and emissions into the atmosphere. Here we report the first in situ global measurements of these two gases. HFC-143a and HFC-32 are the third and sixth most abundant hydrofluorocarbons (HFCs) respectively and they currently make an appreciable contribution to the HFCs in terms of atmospheric radiative forcing (1.7 ± 0.04 and 0.7 ± 0.02 mW m−2 in 2012 respectively). In 2012 the global average mole fraction of HFC-143a was 13.4 ± 0.3 ppt (1σ) in the lower troposphere and its growth rate was 1.4 ± 0.04 ppt yr−1; HFC-32 had a global mean mole fraction of 6.2 ± 0.2 ppt and a growth rate of 1.1 ± 0.04 ppt yr−1 in 2012. The extensive observations presented in this work have been combined with an atmospheric transport model to simulate global atmospheric abundances and derive global emission estimates. It is estimated that 23 ± 3 Gg yr−1 of HFC-143a and 21 ± 11 Gg yr−1 of HFC-32 were emitted globally in 2012, and the emission rates are estimated to be increasing by 7 ± 5% yr−1 for HFC-143a and 14 ± 11% yr−1 for HFC-32.

scholarly journals Global emissions of HFC-143a (CH<sub>3</sub>CF<sub>3</sub>) and HFC-32 (CH<sub>2</sub>F<sub>2</sub>) from in situ and air archive atmospheric observations

2014 ◽  
Vol 14 (5) ◽  
pp. 6471-6500 ◽  
Author(s):  
S. O'Doherty ◽  
M. Rigby ◽  
J. Mühle ◽  
D. J. Ivy ◽  
B. R. Miller ◽  
...  
Keyword(s):  
Growth Rate ◽  
Mole Fraction ◽  
Radiative Forcing ◽  
Transport Model ◽  
Atmospheric Transport ◽  
Lower Troposphere ◽  
Emission Rates ◽  
Global Emission ◽  
Atmospheric Observations

Abstract. High frequency, in situ observations from the Advanced Global Atmospheric Gases Experiment (AGAGE), for the period 2003 to 2012, combined with archive flask measurements dating back to 1977, have been used to capture the rapid growth of HFC-143a (CH3CF3) and HFC-32 (CH2F2) mole fractions and emissions into the atmosphere. Here we report the first in situ global measurements of these two gases. HFC-143a and HFC-32 are the third and sixth most abundant HFCs respectively and they currently make an appreciable contribution to the HFCs in terms of atmospheric radiative forcing (1.7 and 0.7 mW m2 in 2012, respectively). In 2012 the global average mole fraction of HFC-143a was 13.4 ± 0.3 ppt (1-sigma) in the lower troposphere and its growth rate was 1.4 ± 0.04 ppt yr−1; HFC-32 had a global mean mole fraction of 6.2 ± 0.2 ppt and a growth rate of 1.1 ± 0.04 ppt yr−1 in 2012. The extensive observations presented in this work have been combined with an atmospheric transport model to simulate global atmospheric abundances and derive global emission estimates. It is estimated that 23 ± 3 Gg yr−1 of HFC-143a and 21 ± 11 Gg yr−1 of HFC-32 were emitted globally in 2012, and the emission rates are estimated to be increasing 7 ± 5% yr−1 for HFC-143a and 14 ± 11% yr−1 for HFC-32.

scholarly journals TransCom N<sub>2</sub>O model inter-comparison – Part 1: Assessing the influence of transport and surface fluxes on tropospheric N<sub>2</sub>O variability

2014 ◽  
Vol 14 (2) ◽  
pp. 2307-2362 ◽  
Author(s):  
R. L. Thompson ◽  
P. K. Patra ◽  
K. Ishijima ◽  
E. Saikawa ◽  
M. Corazza ◽  
...  
Keyword(s):  
Northern Hemisphere ◽  
Seasonal Cycle ◽  
Large Scale ◽  
Atmospheric Transport ◽  
Lower Troposphere ◽  
Vertical Gradient ◽  
Surface Fluxes ◽  
Meridional Transport ◽  
Mixing Ratios

Abstract. We present a comparison of chemistry-transport models (TransCom-N2O) to examine the importance of atmospheric transport and surface fluxes on the variability of N2O mixing ratios in the troposphere. Six different models and two model variants participated in the inter-comparison and simulations were made for the period 2006 to 2009. In addition to N2O, simulations of CFC-12 and SF6 were made by a subset of four of the models to provide information on the models proficiency in stratosphere-troposphere exchange (STE) and meridional transport, respectively. The same prior emissions were used by all models to restrict differences among models to transport and chemistry alone. Four different N2O flux scenarios totalling between 14 and 17 Tg N yr−1 (for 2005) globally were also compared. The modelled N2O mixing ratios were assessed against observations from in-situ stations, discrete air sampling networks, and aircraft. All models adequately captured the large-scale patterns of N2O and the vertical gradient from the troposphere to the stratosphere and most models also adequately captured the N2O tropospheric growth rate. However, all models underestimated the inter-hemispheric N2O gradient by at least 0.33 ppb (equivalent to 1.5 Tg N), which, even after accounting for an overestimate of emissions in the Southern Ocean of circa 1.0 Tg N, points to a likely underestimate of the Northern Hemisphere source by up to 0.5 Tg N and/or an overestimate of STE in the Northern Hemisphere. Comparison with aircraft data reveal that the models overestimate the amplitude of the N2O seasonal cycle at Hawaii (21° N, 158° W) below circa 6000 m, suggesting an overestimate of the importance of stratosphere to troposphere transport in the lower troposphere at this latitude. In the Northern Hemisphere, most of the models that provided CFC-12 simulations captured the phase of the CFC-12, seasonal cycle, indicating a reasonable representation of the timing of STE. However, for N2O all models simulated a too early minimum by 2 to 3 months owing to errors in the seasonal cycle in the prior soil emissions, which is still not adequately represented by terrestrial biosphere models. In the Southern Hemisphere, most models failed to capture the N2O and CFC-12 seasonality at Cape Grim, Tasmania, and all failed at the South Pole, whereas for SF6, all models could capture the seasonality at all sites, suggesting that there are large errors in modeled vertical transport in high southern latitudes.

scholarly journals Mixing processes and exchanges in the tropical and the subtropical UT/LS

2008 ◽  
Vol 8 (3) ◽  
pp. 10627-10664
Author(s):  
R. James ◽  
B. Legras
Keyword(s):  
Mixing Time ◽  
Chemical Compositions ◽  
Mixing Processes ◽  
Mixing Properties ◽  
Back Trajectories ◽  
Air Masses ◽  
Upper Troposphere ◽  
The Tropics

Abstract. Both in situ measurements and satellite observations indicate evidence of mixing in the upper troposphere (UT) and the lower-stratosphere (LS). In this study, the measurements performed during the Pre-AVE and Costa-Rica AVE campaigns are analysed with diffusive back-trajectories to assess mixing properties in the tropical and the subtropical UT/LS. A description of cross-tropopause pathways and mixing time scales is provided. In the subtropics, Troposphere-Stratosphere mixing processes are found to differ in the vicinity of the tropopause and at higher altitudes. Below 350 K, the mixing line observed during Pre-AVE is shown to result from fast and local cross-tropopause irreversible exchange, involving two initially distant air masses with distinct chemical compositions. For measurements located above 350 K, mixing of the tropospheric air in the subtropical stratosphere occurs over a period of a month, the origins of the tropospheric source being localised in the tropical UT and the tropical boundary layer. In the tropics, quantitative reconstructions of CO and O3 profiles above 360 K are obtained for one month back-trajectories calculations, pointing out that long term mixing is essential to determine the chemical composition in the tropical ascent. In particular, the existence of two-way meridional irreversible exchanges between 360 and 450 K is found to export tropical air in the subtropical stratosphere and to entrain old stratospheric air in the tropical ascent. Calculations of the Lagrangian mean age of air is shown to be in qualitative agreement with the CO2 observations and diabatic calculations.

scholarly journals Long-term ambient air-stable cubic CsPbBr3 perovskite quantum dots using molecular bromine

2019 ◽  
Vol 1 (9) ◽  
pp. 3388-3391 ◽  
Author(s):  
Surakcha Thapa ◽  
Karishma Bhardwaj ◽  
Siddhant Basel ◽  
Sajan Pradhan ◽  
Charlotte J. Eling ◽  
...  
Keyword(s):  
Quantum Dots ◽  
Decisive Role ◽  
Ambient Air ◽  
Molecular Bromine ◽  
Perovskite Nanocrystals ◽  
Perovskite Quantum Dots

Temperature and precursor-controlled in situ generated, oleylammonium halide species from molecular bromine and amine plays decisive role in the synthesis of long-term ambient stable and emission tunable CsPbBr3 perovskite nanocrystals.

scholarly journals Atmospheric histories and emissions of chlorofluorocarbons CFC-13 (CClF<sub>3</sub>), ΣCFC-114 (C<sub>2</sub>Cl<sub>2</sub>F<sub>4</sub>), and CFC-115 (C<sub>2</sub>ClF<sub>5</sub>)

2018 ◽  
Vol 18 (2) ◽  
pp. 979-1002 ◽  
Author(s):  
Martin K. Vollmer ◽  
Dickon Young ◽  
Cathy M. Trudinger ◽  
Jens Mühle ◽  
Stephan Henne ◽  
...  
Keyword(s):  
Mole Fraction ◽  
Transport Model ◽  
Atmospheric Transport ◽  
Global Analysis ◽  
Large Fraction ◽  
Ambient Air ◽  
Atmospheric Observations ◽  
Transport Patterns ◽  
The 1960S ◽  
Global Emissions

Abstract. Based on observations of the chlorofluorocarbons CFC-13 (chlorotrifluoromethane), ΣCFC-114 (combined measurement of both isomers of dichlorotetrafluoroethane), and CFC-115 (chloropentafluoroethane) in atmospheric and firn samples, we reconstruct records of their tropospheric histories spanning nearly 8 decades. These compounds were measured in polar firn air samples, in ambient air archived in canisters, and in situ at the AGAGE (Advanced Global Atmospheric Gases Experiment) network and affiliated sites. Global emissions to the atmosphere are derived from these observations using an inversion based on a 12-box atmospheric transport model. For CFC-13, we provide the first comprehensive global analysis. This compound increased monotonically from its first appearance in the atmosphere in the late 1950s to a mean global abundance of 3.18 ppt (dry-air mole fraction in parts per trillion, pmol mol−1) in 2016. Its growth rate has decreased since the mid-1980s but has remained at a surprisingly high mean level of 0.02 ppt yr−1 since 2000, resulting in a continuing growth of CFC-13 in the atmosphere. ΣCFC-114 increased from its appearance in the 1950s to a maximum of 16.6 ppt in the early 2000s and has since slightly declined to 16.3 ppt in 2016. CFC-115 increased monotonically from its first appearance in the 1960s and reached a global mean mole fraction of 8.49 ppt in 2016. Growth rates of all three compounds over the past years are significantly larger than would be expected from zero emissions. Under the assumption of unchanging lifetimes and atmospheric transport patterns, we derive global emissions from our measurements, which have remained unexpectedly high in recent years: mean yearly emissions for the last decade (2007–2016) of CFC-13 are at 0.48 ± 0.15 kt yr−1 (> 15 % of past peak emissions), of ΣCFC-114 at 1.90 ± 0.84 kt yr−1 (∼ 10 % of peak emissions), and of CFC-115 at 0.80 ± 0.50 kt yr−1 (> 5 % of peak emissions). Mean yearly emissions of CFC-115 for 2015–2016 are 1.14 ± 0.50 kt yr−1 and have doubled compared to the 2007–2010 minimum. We find CFC-13 emissions from aluminum smelters but if extrapolated to global emissions, they cannot account for the lingering global emissions determined from the atmospheric observations. We find impurities of CFC-115 in the refrigerant HFC-125 (CHF2CF3) but if extrapolated to global emissions, they can neither account for the lingering global CFC-115 emissions determined from the atmospheric observations nor for their recent increases. We also conduct regional inversions for the years 2012–2016 for the northeastern Asian area using observations from the Korean AGAGE site at Gosan and find significant emissions for ΣCFC-114 and CFC-115, suggesting that a large fraction of their global emissions currently occur in northeastern Asia and more specifically on the Chinese mainland.

scholarly journals Evaluation of a cavity ring-down spectrometer for in situ observations of <sup>13</sup>CO<sub>2</sub>

2013 ◽  
Vol 6 (2) ◽  
pp. 301-308 ◽  
Author(s):  
F. R. Vogel ◽  
L. Huang ◽  
D. Ernst ◽  
L. Giroux ◽  
S. Racki ◽  
...  
Keyword(s):  
Co2 Concentration ◽  
Ambient Air ◽  
In Situ Monitoring ◽  
Wide Spread ◽  
Isotope Ratio Mass Spectrometer ◽  
In Situ Observations ◽  
One Year ◽  
Cavity Ring Down

Abstract. With the emergence of wide-spread application of new optical techniques to monitor δ13C in atmospheric CO2 there is a growing need to ensure well-calibrated measurements. We characterized one commonly available instrument, a cavity ring-down spectrometer (CRDS) system used for continuous in situ monitoring of atmospheric 13CO2. We found no dependency of δ13C on the CO2 concentration in the range of 303–437 ppm. We designed a calibration scheme according to the diagnosed instrumental drifts and established a quality assurance protocol. We find that the repeatability (1-σ) of measurements is 0.25‰ for 10 min and 0.15‰ for 20 min integrated averages, respectively. Due to a spectral overlap, our instrument displays a cross-sensitivity to CH4 of 0.42 ± 0.024‰ ppm−1. Our ongoing target measurements yield standard deviations of δ13C from 0.22‰ to 0.28‰ for 10 min averages. We furthermore estimate the reproducibility of our system for ambient air samples from weekly measurements of a long-term target gas to be 0.18‰. We find only a minuscule offset of 0.002 ± 0.025‰ between the CRDS and Environment Canada's isotope ratio mass spectrometer (IRMS) results for four target gases used over the course of one year.

scholarly journals Atmospheric histories and emissions of chlorofluorocarbons CFC-13(CClF<sub>3</sub>), CFC-114 (C<sub>2</sub>Cl<sub>2</sub>F<sub>4</sub>), and CFC-115 (C<sub>2</sub>ClF<sub>5</sub>)

2017 ◽  
Author(s):  
Martin K. Vollmer ◽  
Dickon Young ◽  
Cathy M. Trudinger ◽  
Jens Mühle ◽  
Stephan Henne ◽  
...  
Keyword(s):  
Mole Fraction ◽  
Transport Model ◽  
Atmospheric Transport ◽  
Global Analysis ◽  
Large Fraction ◽  
Ambient Air ◽  
North East ◽  
The North ◽  
High Level ◽  
Global Emissions

Abstract. Based on observations of three chlorofluorocarbons, CFC-13 (chlorotrifluoromethane), CFC-114 (dichlorotetrafluoroethane) and CFC-115 (chloropentafluoroethane) in atmospheric and firn samples, we reconstruct records of their tropospheric histories spanning nearly eight decades. These compounds were measured in polar firn air samples, in ambient air archived in canisters, and in-situ at the AGAGE (Advanced Global Atmospheric Gases Experiment) network and affiliated sites. Global emissions to the atmosphere are derived from these observations using an inversion based on a 12-box atmospheric transport model. For CFC-13, we provide the first comprehensive global analysis. This compound increased monotonically from its first appearance in the atmosphere in the late 1950s to a mean global abundance of 3.18 ppt (dry air mole fraction in parts-per-trillion, pmol mol−-1) in 2016. Its growth rate has decreased since the mid 1980s but has remained at a surprisingly high level of 0.02 ppt yr−1 since the late 2000s. CFC-114 increased from its appearance in the 1950s to a maximum of 16.6 ppt in the early 2000s, and has since slightly declined to 16.3 ppt in 2016. CFC-115 increased monotonically from its first appearance in the 1960s and reached a global mean mole fraction of 8.52 ppt in 2016. Growth rates of all three compounds over the past years are significantly larger than would be expected from zero emissions. Under the assumption of unaltered lifetimes and atmospheric transport patterns, we derive global emissions from our measurements, which have remained unexpectedly high in recent years: Mean yearly emissions for the last decade (2007–2016) of CFC-13 are at 0.48 ± 0.15 kt yr−1 (> 15 % of past peak emissions), of CFC-114 at 1.90 ± 0.84 kt yr−1 (~ 10 % of peak emissions), and of CFC-115 at 0.80 ± 0.50 kt yr−1 (> 5 % of peak emissions). Mean yearly emissions of CFC-115 for 2014–2016 are 1.08 ± 0.50 kt yr−1 and have more than doubled compared to 2009. Cumulative global emissions for CFC-114 derived from observations through 2016 exceed the global cumulative production derived from reported inventory data by > 10 % while those for CFC-115 agree well. We find CFC-13 emissions from aluminum smelters and impurities of CFC-115 in the refrigerant HFC-125 (CHF2CF3) but if extrapolated to global emissions neither of them can account for the lingering global emissions determined from the atmospheric observations. We also conduct regional inversions for the years 2012–2016 for the north-east Asian area using observations from the Korean Gosan AGAGE site and find significant emissions for CFC-114 and CFC-115, suggesting that a large fraction of their global emissions currently occur in north-eastern Asia and more specifically on the Chinese mainland.

Lead halide–templated crystallization of methylamine-free perovskite for efficient photovoltaic modules

Science ◽  
2021 ◽  
Vol 372 (6548) ◽  
pp. 1327-1332
Author(s):  
Tongle Bu ◽  
Jing Li ◽  
Hengyi Li ◽  
Congcong Tian ◽  
Jie Su ◽  
...  
Keyword(s):  
Perovskite Solar Cells ◽  
Ambient Air ◽  
Large Area ◽  
Photovoltaic Modules ◽  
Α Phase ◽  
Slot Die ◽  
Δ Phase ◽  
Lead Halide

Upscaling efficient and stable perovskite layers is one of the most challenging issues in the commercialization of perovskite solar cells. Here, a lead halide–templated crystallization strategy is developed for printing formamidinium (FA)–cesium (Cs) lead triiodide perovskite films. High-quality large-area films are achieved through controlled nucleation and growth of a lead halide•N-methyl-2-pyrrolidone adduct that can react in situ with embedded FAI/CsI to directly form α-phase perovskite, sidestepping the phase transformation from δ-phase. A nonencapsulated device with 23% efficiency and excellent long-term thermal stability (at 85°C) in ambient air (~80% efficiency retention after 500 hours) is achieved with further addition of potassium hexafluorophosphate. The slot die–printed minimodules achieve champion efficiencies of 20.42% (certified efficiency 19.3%) and 19.54% with an active area of 17.1 and 65.0 square centimeters, respectively.

Sign in / Sign up

Export Citation Format

Share Document