TY - JOUR

T1 - Nitric acid from volcanoes.

AU - Mather, T. A.

AU - Allen, A. G.

AU - Davison, Brian

AU - Pyle, D. M.

AU - Oppenheimer, C.

AU - McGonigle, A. J. S.

PY - 2004/1/30

Y1 - 2004/1/30

N2 - Atmospheric cycling of nitric acid and other nitrogen-bearing compounds is an important biogeochemical process, with significant implications for ecosystems and human health. Volcanoes are rarely considered as part of the global nitrogen cycle, but here we show that they release a previously unconsidered flux of HNO3 vapour to the atmosphere. We report the first measurements of nitric acid vapour in the persistent plumes from four volcanoes: Masaya (Nicaragua); Etna (Italy); and Villarrica and Lascar (Chile). Mean near-source volcanic plume concentrations of HNO3 range from 1.8 to 5.6 Wmol m33, an enrichment of one to two orders of magnitude over background (0.1^1.5 Wmol m33). Using mean molar HNO3/SO2 ratios of 0.01, 0.02, 0.05, and 0.07 for Villarrica, Masaya, Etna, and Lascar respectively, combined with SO2 flux measurements, we calculate gaseous HNO3 fluxes from each of these volcanic systems, and extend this to estimate the global flux from high-temperature, non-explosive volcanism to be V0.02^ 0.06 Tg (N) yr31. While comparatively small on the global scale, this flux could have important implications for regional fixed N budgets. The precise mechanism for the emission of this HNO3 remains unclear but we suggest that thermal nitrogen fixation followed by rapid oxidation of the product NO is most likely. In explosive, ash-rich plumes NO may result from, or at least be supplemented by, production from volcanic lightning rather than thermal N fixation. We have calculated NO production via this route to be of the order of 0.02 Tg (N) yr31.

AB - Atmospheric cycling of nitric acid and other nitrogen-bearing compounds is an important biogeochemical process, with significant implications for ecosystems and human health. Volcanoes are rarely considered as part of the global nitrogen cycle, but here we show that they release a previously unconsidered flux of HNO3 vapour to the atmosphere. We report the first measurements of nitric acid vapour in the persistent plumes from four volcanoes: Masaya (Nicaragua); Etna (Italy); and Villarrica and Lascar (Chile). Mean near-source volcanic plume concentrations of HNO3 range from 1.8 to 5.6 Wmol m33, an enrichment of one to two orders of magnitude over background (0.1^1.5 Wmol m33). Using mean molar HNO3/SO2 ratios of 0.01, 0.02, 0.05, and 0.07 for Villarrica, Masaya, Etna, and Lascar respectively, combined with SO2 flux measurements, we calculate gaseous HNO3 fluxes from each of these volcanic systems, and extend this to estimate the global flux from high-temperature, non-explosive volcanism to be V0.02^ 0.06 Tg (N) yr31. While comparatively small on the global scale, this flux could have important implications for regional fixed N budgets. The precise mechanism for the emission of this HNO3 remains unclear but we suggest that thermal nitrogen fixation followed by rapid oxidation of the product NO is most likely. In explosive, ash-rich plumes NO may result from, or at least be supplemented by, production from volcanic lightning rather than thermal N fixation. We have calculated NO production via this route to be of the order of 0.02 Tg (N) yr31.

KW - ¢xed nitrogen

KW - nitrogen cycle

KW - volcanic emissions

KW - volcanic lightning

U2 - 10.1016/S0012-821X(03)00640-X

DO - 10.1016/S0012-821X(03)00640-X

M3 - Journal article

VL - 218

SP - 17

EP - 30

JO - Earth and Planetary Science Letters

JF - Earth and Planetary Science Letters

SN - 0012-821X

IS - 1-2

ER -