Atmospheric Methane Enhancements Related with Natural Gas Usage in the Greater Houston Area

Natural gas (NG) usage as a replacement of oil and coal has increased significantly in the U.S in recent years. Despite the benefits associated with this fuel, leakage from NG distribution systems and in-use uncombusted NG (e.g., compressed natural gas vehicles) can be relevant sources of methane (CH4) emissions in urban centers. Methane, the main constituent of NG, is a potent greenhouse gas impacting the chemistry of the atmosphere, whose emission might outweigh the potential environmental advantages of NG use. Although the Greater Houston area (GHA) is the fifth-largest metropolitan area in the U.S, no studies on the potential impact of NG usage on atmospheric CH4 levels have been published in the scientific literature to date. In this work, a mobile-based study of CH4 and ethane (C2H6) concentration levels in eight residential zones with different expected probability of NG leakage in the GHA was conducted in the summer of 2016. A novel laser-based sensor system for simultaneous detection of CH4 and C2H6 was developed and deployed in a mid-sized vehicle, and monitoring of these gas species was conducted for over 14 days covering 250 road miles. Both linear discriminant and cluster analyses were performed to assess the spatial variability of atmospheric CH4 concentrations in the GHA. These analyses showed clear differences in the CH4 mixing ratios in an inter- and intra-neighborhood level and indicated the presence of high CH4 concentration clusters mainly located in the central and west central parts of the GHA. Source discrimination analyses based on orthogonal regression analysis and a Keeling-like plot method were conducted to establish the predominant origin of CH4 in the identified high concentration clusters and in over 30 CH4 concentration peaks observed during the field campaign. Results of these analyses indicate that thermogenic sources of CH4 (e.g., NG) were predominant in short-duration concentration spikes (lasting less than 10 minutes), while CH4 with a biogenic origin was mainly related with large-area concentration events (duration above 10 minutes). The content of C2H6 in the thermogenic-related peak events (2.7-5.9%) agreed with the composition of the NG distributed in the GHA, indicating the potential relevance of NG usage on CH4 enhancements observed in the Houston atmosphere.