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 spaceresolved national inventories. These and other recommendations are proposed for the major areas of CH4 science with the aim of improving capability in the coming decade to quantify atmospheric CH4 budgets on the scales necessary for the success of climate policies. Plain Language Summary Methane is the second largest contributor to climate warming from human activities since preindustrial times. Reducing human‐made emissions by half is a major component of the 2015 Paris Agreement target to keep global temperature increases well below 2 °C. In parallel to the methane emission reductions pledged by individual nations, new capabilities are needed to determine independently whether these reductions are actually occurring and whether methane concentrations in the atmosphere are changing for reasons that are clearly understood. At present signiﬁcant challenges limit the ability of scientists to identify the mechanisms causing changes in atmospheric methane. This study reviews current and emerging tools in methane science and proposes major advances needed in the coming decade to achieve this crucial capability. We recommend further developing the models that simulate the processes behind methane emissions, improving atmospheric measurements of methane and its major carbon and hydrogen isotopes, and advancing abilities to infer the rates of methane being emitted and removed from the atmosphere from these measurements. The improvements described here will play a major role in assessing emissions commitments as more cities, states, and countries report methane emission inventories and commit to speciﬁc emission reduction targets.

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

Megacities, with their large and complex infrastructures, are significant sources of methane emissions. To develop a simple, low-cost methodology to quantify these globally important methane sources, this study focuses on mobile measurements of methane (CH4) and its isotopic composition in Paris. Data collected between September 2018 to March 2019 resulted in 17 days of measurements, which provided spatial distribution of street-level methane mixing ratios, source type identification, and emission quantification. Consequently, 90 potential leaks were detected in Paris sorted into three leak categories: natural gas distribution network emissions (63%), sewage network emissions (33%), and emissions from heating furnaces of buildings (4%). The latter category has not previously been reported in urban methane studies. Accounting for the detectable emissions from the ground, the total estimated CH4 emission rate of Paris was 5000 L/min (190 t/yr), with the largest contribution from gas leaks (56%). This ranks Paris as a city with medium CH4 emissions. Two areas of clusters were found, where 22% and 56% of the total potential emissions of Paris were observed. Our findings suggest that the natural gas distribution network, the sewage system, and furnaces of buildings are ideal targets for street-level CH4 emission reduction efforts for Paris.

https://pubs.acs.org/doi/pdf/10.1021/acs.est.1c00859

Mapping Urban Methane Sources in Paris, France

Cosmogenic nuclide techniques

Radiocarbon (14C) measurements offer a unique investigative tool to study methane emissions by identifying fossil-fuel methane in air. Fossil-fuel methane is devoid of 14C and, when emitted to the atmosphere, causes a strong decrease in the ratio of radiocarbon to total carbon in methane (Δ14CH4). By observing the changes in Δ14CH4, the fossil fraction of methane emissions can be quantified. Presently, there are very few published Δ14CH4 measurements, mainly because it is challenging to collect and process the large volumes of air needed for radiocarbon measurements. We present a new sampling system that collects enough methane carbon for high precision Δ14CH4 measurements without having to transport large volumes of air. The system catalytically combusts CH4 into CO2 and adsorbs the combustion-derived CO2 onto a molecular sieve trap, after first removing CO2, CO, and H2O. Tests using reference air show a Δ14CH4 measurement repeatability of 5.4‰, similar or better than the precision in the most recent reported measurements. We use the system to produce the first Δ14CH4 measurements in central London and show that day-to-day differences in Δ14CH4 in these samples can be attributed to fossil methane input. The new system could be deployed in a range of settings to investigate CH4 sources.

Efficient Sampling of Atmospheric Methane for Radiocarbon Analysis and Quantification of Fossil Methane.

As unavoidable by-products of the combustion of organic matter, the sources of carcinogenic polycyclic aromatic hydrocarbons (PAHs) are an area of great research interest in environmental monitorin...

The importance of compound-specific radiocarbon analysis in source identification of polycyclic aromatic hydrocarbons: A critical review

Methane contributes substantially to global warming as the second most important anthropogenic greenhouse gas. Radiocarbon (14C) measurements of atmospheric methane can be used as a source apportionment tool, as they allow distinction between thermogenic and biogenic methane sources. However, these measurements remain scarce due to labor-intensive methods required. A new setup for the preparation of atmospheric methane samples for radiocarbon analysis is presented. The system combines a methane preconcentration line with a preparative gas chromatography technique to isolate pure methane samples for a compound-specific radiocarbon analysis. In order to minimize sample preparation time, we designed a simplified preconcentration line for the extraction of methane from 50 L atmospheric air, which corresponds to 50 µg C as required for a reliable 14C analysis of methane-derived CO2 gas measurement with accelerator mass spectrometry (AMS). The system guarantees a quantitative extraction of methane from atmospheric air samples for 14C analysis, with a good repeatability and a low processing blank. The setup was originally designed for the measurement of samples with low methane concentrations, but it can also be adapted to apportion sources from environmental compartments with high methane levels such as freshwaters or wetlands.

/pdf/compound-specific-radiocarbon-analysis-of-atmospheric-mmuxnflp5i.pdf

Compound-Specific Radiocarbon Analysis of Atmospheric Methane: A New Preconcentration and Purification Setup

We present the current performance of the in situ radiocarbon (14C) extraction line at the University of Bern with an improved extraction and combustion system. After three major steps of improvement, the extraction of sample CO2 gas now takes place inside a platinum crucible, supported by an outer quartz-glass crucible. This setup allows us to operate the line as a closed system for several samples without breaking the vacuum. Measurements of procedural blanks and samples from our reference strewn field, Jiddat al Harasis 073, performed in our system all show a good reproducibility and, for the strewn field samples, consistency with published data. We describe each improvement step in detail, discussing the advantages and disadvantages of all tested setups. By sharing our knowledge, we aim to inform and prevent others from making the same or similar detours in establishing 14C extraction systems for extraterrestrial samples.

https://www.cambridge.org/core/services/aop-cambridge-core/content/view/S0033822220000387

An update on the performance of the in situ 14c extraction line at the university of bern

Through the investigation of terrestrial ages of meteorites from Oman, we aim to better understand the time scales of meteorite accumulation and erosion in Oman and the meteorite flux in the past. Here, we present 14C and 14C‐10Be terrestrial ages of seven ordinary chondrite strewn fields and two unpaired single meteorites from the Sultanate of Oman. After critical evaluation of multiple data for each strewn field, we propose “best estimate terrestrial ages,” typically based on 14C/10Be. For objects for which complex irradiation histories are known or suspected, terrestrial ages were calculated solely using 14C. The best estimate strewn field ages range from 8.1 ± 3.0 ka (SaU 001) to 35.2 ± 5.1 ka (Dho 005). Including two previously dated strewn fields, the mean and median age of nine Oman strewn fields is 15.9 ± 12.3 and 13.6 ka, respectively. The new data show a general good agreement with data previously obtained in a different laboratory, and we observe a similar general correlation between strewn field ages and mean weathering grade as in previous work based on individual meteorites. Weathering degree W4 is reached for dated samples after 20–35 ka. While the age statistics of strewn fields does not show the previously observed lack of young events, the low abundance of young (0–5 ka) individual meteorites as compared with older (~20 ka) meteorites is confirmed by our data and remains unexplained.

Terrestrial ages of seven meteorite strewn fields and two single unpaired meteorites from the Sultanate of Oman determined using 14C and 10Be

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Compound-Specific Radiocarbon Analysis of Atmospheric Methane: A New Preconcentration and Purification Setup

An update on the performance of the in situ 14c extraction line at the university of bern

Terrestrial ages of seven meteorite strewn fields and two single unpaired meteorites from the Sultanate of Oman determined using 14C and 10Be