An improved method for mobile characterisation of &amp;lt;i&amp;gt;δ&amp;lt;/i&amp;gt;&amp;lt;sup&amp;gt;13&amp;lt;/sup&amp;gt;CH&amp;lt;sub&amp;gt;4&amp;lt;/sub&amp;gt; source signatures and its application in Germany

Hoheisel, Antje; Yeman, Christiane; Dinger, Florian; Eckhardt, Henrik; Schmidt, Martina

doi:10.5194/amt-12-1123-2019

Cited by 39 publications

(52 citation statements)

References 33 publications

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“…This strengthens the confidence in source attribution using these tracers. The fossil δ 13 C signature of bag samples from natural gas leaks in Hamburg (δ 13 C = -41.9 ± 1.0 ‰) is higher than recently reported in the city of Heidelberg (δ 13 C = −46.1 ± 0.8 ‰ (Hoheisel et al, 2019)). This shows that within one country δ 13 C from NGDN can vary from one region to another.…”

Section: Discussioncontrasting

confidence: 61%

Methane mapping, emission quantification and attribution in two European cities; Utrecht, NL and Hamburg, DE

Maazallahi¹,

Menoud²,

Zavala-Araiza³

et al. 2020

Preprint

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Abstract. Characterizing and attributing methane (CH4) emissions across varying scales is important from environmental, safety, and economic perspectives, and is essential for designing and evaluating effective mitigation strategies. Mobile real-time measurements of CH4 in ambient air offer a fast and effective method to identify and quantify local CH4 emissions in urban areas. We carried out extensive campaigns to measure CH4 mole fractions at the street level in Utrecht, The Netherlands (2018 and 2019) and Hamburg, Germany (2018). One hundred and forty five leak indications (LIs, i.e., methane enhancements of more than 10 % above background levels) were detected in Hamburg and 81 in Utrecht. Measurements of the ethane / methane ratio (C2 / C1), methane / carbon dioxide ratio (CH4 / CO2), and CH4 isotope composition (δ13C and δD) show that in Hamburg about 1/3 of the LIs, and in Utrecht 2/3 of the LIs (based on a limited set of C2/C1 measurements), were of fossil fuel origin. We find that in both cities the largest emission rates in the identified LI distribution are from fossil fuel sources. In Hamburg, the lower emission rates in the identified LI distribution are often associated with biogenic characteristics, and partly combustion. Extrapolation of detected LI rates along the roads driven to the gas distribution pipes in the entire road network yields total emissions from sources that can be quantified in the street-level surveys of 440 ± 70 t/yr from all sources in Hamburg, and 150 ± 50 t/yr for Utrecht. In Hamburg, C2/C1, CH4/CO2, and isotope-based source attribution analyses shows that 50–80 % of all emissions originate from the natural gas distribution network, in Utrecht more limited attribution indicates that 70–90 % of the emissions are of fossil origin. Our results confirm previous observations that a few large LIs, creating a heavy tail, are responsible for a significant proportion of fossil CH4 emissions. In Utrecht, 1/3 of total emissions originated from one LI and in Hamburg > 1/4 from 2 LIs. In Hamburg, the local gas utility detected only 20 % of the LIs that were identified as from a fossil source, but the largest leaks were located and fixed quickly once the LIs were shared.

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Section: Discussioncontrasting

confidence: 61%

Methane mapping, emission quantification and attribution in two European cities; Utrecht, NL and Hamburg, DE

Maazallahi¹,

Menoud²,

Zavala-Araiza³

et al. 2020

Preprint

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“…The measurement set-up used here is the same as in the field (Section 2.4). The general principle of the setup is comparable to the previous works (e.g., Hoheisel et al, 2019;Lopez et al, 2017;Rella et al, 2015). As the instrument is not dedicated to C2H6 measurements, the vibrations induced by the motion of the car cause noise in the instrument readouts.…”

Section: Controlled-release Experiments Setupmentioning

confidence: 80%

“…Second, by accumulating air in the AirCore (Karion et al 2010;Rella et al 2015;Lopez et al 2017) while moving through the plume and eventually reinjecting the AirCore's air into the analyzer while stopped. Previously, the AirCore tool was successfully used as part of a mobile measurement setup to determine the isotopic composition of the methane source (Rella et al 2015;Hoheisel et al 2019;Lopez et al 2017) and to determine C2H6:CH4 ratio (Lopez et al 2017).…”

Section: Controlled-release Experiments Setupmentioning

confidence: 99%

Ethane measurement by Picarro CRDS G2201-i in laboratory and field conditions: potential and limitations

Defratyka¹,

Paris²,

Kwok³

et al. 2020

Preprint

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Abstract. Ethane can be used as a tracer gas to distinguish methane sources, both at the local and global scale. Currently, ethane can be successfully measured using flasks or dedicated in-situ analyzers. In our study, we consider the possibility of using the CRDS Picarro G2201-i instrument, dedicated to isotopic CH4 and CO2, for suitable measurements of ethane:methane ratio in mobile field, near-source conditions. Our work was divided into three steps. First, laboratory tests were run to characterize the instrument in stationary conditions. Then the instrument performance was tested in the field, as part of a controlled release experiment and finally during mobile measurements focused on gas compressor stations. The results from the field are compared with the results from other instruments, dedicated to ethane measurements. Our study clearly shows the potential of using the CRDS G2201-i instrument to determine the ethane:methane ratio in methane plumes in mobile condition with an ethane uncertainty of 50 ppb. Assuming typical ethane to methane ratio ranging between 0 and 0.1 ppb ppb−1 we conclude that the instrument can correctly estimate the “true” ethane to methane ratio within 1-sigma uncertainty in CH4 enhancements of 1 ppm or more as can be found in the vicinity of strongly emitting sites (such as natural gas compressor station).

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“…The major benefits of laser spectrometric techniques include their potential for automation and continuous measurement, allowing deployment outside a usual laboratory setting, and their ability to measure more than one isotope system simultaneously. Measurements by laser spectroscopy have been proven in studies measuring enhanced CH 4 mole fractions near sources (Bergamaschi et al, ; Hoheisel et al, ; Santoni et al, ). In the analysis of ambient air samples using an inline preconcentration method, precisions of 0.1‰ and 0.5‰ for δ 13 C‐CH 4 and δD‐CH 4 , respectively, were demonstrated, which were subsequently also shown in a field study alongside measurements by IRMS (Röckmann et al, ).…”

Section: Measurementsmentioning

confidence: 99%

“…Studies show it may be important to implement long-term measurements quantifying temporal variation (Fisher et al, 2017;Sriskantharajah et al, 2012). The availability of relatively inexpensive off-the-shelf spectrometers could help to fill in the large gaps in source signature characterization in the coming years (Hoheisel et al, 2019).…”

Section: Isotopic Ratio Measurementsmentioning

confidence: 99%

Advancing Scientific Understanding of the Global Methane Budget in Support of the Paris Agreement

Ganesan

Schwietzke²,

Poulter

et al. 2019

Global Biogeochemical Cycles

107

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The 2015 Paris Agreement of the United Nations Framework Convention on Climate Change aims to keep global average temperature increases well below 2 °C of preindustrial levels in the Year 2100. Vital to its success is achieving a decrease in the abundance of atmospheric methane (CH4), the second most important anthropogenic greenhouse gas. If this reduction is to be achieved, individual nations must make and meet reduction goals in their nationally determined contributions, with regular and independently verifiable global stock taking. Targets for the Paris Agreement have been set, and now the capability must follow to determine whether CH4 reductions are actually occurring. At present, however, there are significant limitations in the ability of scientists to quantify CH4 emissions accurately at global and national scales and to diagnose what mechanisms have altered trends in atmospheric mole fractions in the past decades. For example, in 2007, mole fractions suddenly started rising globally after a decade of almost no growth. More than a decade later, scientists are still debating the mechanisms behind this increase. This study reviews the main approaches and limitations in our current capability to diagnose the drivers of changes in atmospheric CH4 and, crucially, proposes ways to improve this capability in the coming decade. Recommendations include the following: (i) improvements to process‐based models of the main sectors of CH4 emissions—proposed developments call for the expansion of tropical wetland flux measurements, bridging remote sensing products for improved measurement of wetland area and dynamics, expanding measurements of fossil fuel emissions at the facility and regional levels, expanding country‐specific data on the composition of waste sent to landfill and the types of wastewater treatment systems implemented, characterizing and representing temporal profiles of crop growing seasons, implementing parameters related to ruminant emissions such as animal feed, and improving the detection of small fires associated with agriculture and deforestation; (ii) improvements to measurements of CH4 mole fraction and its isotopic variations—developments include greater vertical profiling at background sites, expanding networks of dense urban measurements with a greater focus on relatively poor countries, improving the precision of isotopic ratio measurements of 13CH4, CH3D, 14CH4, and clumped isotopes, creating isotopic reference materials for international‐scale development, and expanding spatial and temporal characterization of isotopic source signatures; and (iii) improvements to inverse modeling systems to derive emissions from atmospheric measurements—advances are proposed in the areas of hydroxyl radical quantification, in systematic uncertainty quantification through validation of chemical transport models, in the use of source tracers for estimating sector‐level emissions, and in the development of time and space resolved national inventories. These and other recommendations are proposed for...

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An improved method for mobile characterisation of <i>δ</i><sup>13</sup>CH<sub>4</sub> source signatures and its application in Germany

Cited by 39 publications

References 33 publications

Methane mapping, emission quantification and attribution in two European cities; Utrecht, NL and Hamburg, DE

Methane mapping, emission quantification and attribution in two European cities; Utrecht, NL and Hamburg, DE

Ethane measurement by Picarro CRDS G2201-i in laboratory and field conditions: potential and limitations

Advancing Scientific Understanding of the Global Methane Budget in Support of the Paris Agreement

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