Locating and Quantifying Methane Emissions by Inverse Analysis of Path-Integrated Concentration Data Using a Markov-Chain Monte Carlo Approach

ACS Earth Space Chem. 2022 Sep 15;6(9):2190-2198. doi: 10.1021/acsearthspacechem.2c00093. Epub 2022 Jul 8.

Abstract

The action to reduce anthropogenic greenhouse gas emissions is severely constrained by the difficulty of locating sources and quantifying their emission rates. Methane emissions by the energy sector are of particular concern. We report results achieved with a new area monitoring approach using laser dispersion spectroscopy to measure path-averaged concentrations along multiple beams. The method is generally applicable to greenhouse gases, but this work is focused on methane. Nineteen calibrated methane releases in four distinct configurations, including three separate blind trials, were made within a flat test area of 175 m by 175 m. Using a Gaussian plume gas dispersion model, driven by wind velocity data, we calculate the data anticipated for hundreds of automatically proposed candidate source configurations. The Markov-chain Monte Carlo analysis finds source locations and emission rates whose calculated path-averaged concentrations are consistent with those measured and associated uncertainties. This approach found the correct number of sources and located them to be within <9 m in more than 75% of the cases. The relative accuracy of the mass emission rate results was highly correlated to the localization accuracy and better than 30% in 70% of the cases. The discrepancies for mass emission rates were <2 kg/h for 95% of the cases.