Study of the daily and seasonal atmospheric CH4 mixing ratio variability in a rural Spanish region using Rn-222 tracer

Abstract

The ClimaDat station at Gredos (GIC3) has been continuously measuring atmospheric (dry air) mixing ratios of carbon dioxide (CO2) and methane (CH4), as well as meteorological parameters, since November 2012. In this study we investigate the atmospheric variability of CH4 mixing ratios between 2013 and 2015 at GIC3 with the help of co-located observations of 222Rn concentrations, modelled 222Rn fluxes and modelled planetary boundary layer heights (PBLHs). Both daily and seasonal changes in atmospheric CH4 can be better understood with the help of atmospheric concentrations of 222Rn (and the corresponding fluxes). On a daily timescale, the variation in the PBLH is the main driver for 222Rn and CH4 variability while, on monthly timescales, their atmospheric variability seems to depend on emission changes. To understand (changing) CH4 emissions, nocturnal fluxes of CH4 were estimated using two methods: the radon tracer method (RTM) and a method based on the EDGARv4.2 bottom-up emission inventory, both using FLEXPARTv9.0.2 footprints. The mean value of RTM-based methane fluxes (FR_CH4) is 0.11¿mg CH4¿m-2¿h-1 with a standard deviation of 0.09 or 0.29¿mg CH4¿m-2¿h-1 with a standard deviation of 0.23¿mg CH4¿m-2¿h-1 when using a rescaled 222Rn map (FR_CH4_rescale). For our observational period, the mean value of methane fluxes based on the bottom-up inventory (FE_CH4) is 0.33¿mg CH4¿m-2¿h-1 with a standard deviation of 0.08¿mg CH4¿m-2¿h-1. Monthly CH4 fluxes based on RTM (both FR_CH4 and FR_CH4_rescale) show a seasonality which is not observed for monthly FE_CH4 fluxes. During January–May, RTM-based CH4 fluxes present mean values 25¿% lower than during June–December. This seasonal increase in methane fluxes calculated by RTM for the GIC3 area appears to coincide with the arrival of transhumant livestock at GIC3 in the second half of the year.