Influence of atmospheric stability and transport on CH4 concentrations in northern Spain

• Published in: The Science of the total environment 2016-04, Vol.550, p.157-166
• Main Authors: García, M. Ángeles, Sánchez, M. Luisa, Pérez, Isidro A., Ozores, Marta I., Pardo, Nuria
• Format: Article
• Language: English
• Subjects: Atmospheric stability; Background concentration; Backward trajectories; Methane; Richardson number
• ISSN: 0048-9697; 1879-1026
• DOI: 10.1016/j.scitotenv.2016.01.099

Continuous methane (CH4) concentrations were measured in Northern Spain over two years (2011–2012) by multi-point sampling at 1.8, 3.7 and 8.3m using a Picarro analyser. The technique is based on cavity ring-down spectroscopy. The contrast in mean concentrations was about 1.2ppb, with 95th percentiles differing by 2.2ppb and mean minimum concentrations proving similar. Temporal variations of CH4 were also analysed, with a similar seasonal variability being found for the three heights. The highest CH4 concentrations were obtained in late autumn and winter and the lowest in summer, yielding a range of 52ppb. This variation may depend on the active photochemical reaction with OH radical during a period of intense solar radiation and changes in soil conditions together with variations in emissions. Peak concentration levels were recorded at night-time, between 5:00–7:00 GMT, with mean values ranging between 1920 and 1923ppb. The lowest value, around 1884ppb, was obtained at 16:00 GMT. This diurnal variation was mainly related to vertical mixing and photochemistry. Therefore, CH4 concentrations were also examined using the bulk Richardson number (RB) as a stability indicator. Four groups were distinguished: unstable cases, situations with pure shear flow, transitional stages and drainage flows. The highest contrast in mean CH4 concentrations between lower and upper heights was obtained for the transition and drainage cases, mainly associated to high concentrations from nearby sources. The impact of long range transport was analysed by means of 3-day isobaric backward air mass trajectories, which were calculated taking into account origins from Europe, Africa, the Atlantic Ocean and Local conditions. Assessment of the results showed the influence of S and SE wind sectors, especially with Local conditions associated with low winds. Finally, an estimation of the background CH4 concentration in the study period provided an average value of about 1892ppb. [Display omitted] •Dry CH4 concentrations obtained with a multi-point sampling system were analysed.•Daily and yearly patterns were similar for the different heights.•Air mass trajectories, mainly S-SE sectors, influencing CH4 concentrations•Conditions for background levels were established.