Sulfate geoengineering impact on methane transport and lifetime: results from 
the Geoengineering Model Intercomparison Project (GeoMIP) 

 

https://www.atmos-chem-phys.net/17/11209/2017/ 

 

Daniele Visioni1,2, Giovanni Pitari1, Valentina Aquila3, Simone Tilmes4, Irene 
Cionni5, Glauco Di Genova2, and Eva Mancini1,2 1Department of Physical and 
Chemical Sciences, Università dell'Aquila, 67100 L'Aquila, Italy
2CETEMPS, Università dell'Aquila, 67100 L'Aquila, Italy
3GESTAR/Johns Hopkins University, Department of Earth and Planetary Science, 
3400 N Charles Street, Baltimore, MD 21218, USA
4National Center for Atmospheric Research, Boulder, CO 80305, USA
5ENEA, Ente per le Nuove Tecnologie, l'Energia e l'Ambiente, 00123 Rome, Italy

Received: 05 Jul 2017 – Discussion started: 11 Jul 2017
Revised: 07 Sep 2017 – Accepted: 11 Sep 2017 – Published: 21 Sep 2017

Abstract. Sulfate geoengineering (SG), made by sustained injection of SO2 in 
the tropical lower stratosphere, may impact the CH4 abundance through several 
photochemical mechanisms affecting tropospheric OH and hence the methane 
lifetime. (a) The reflection of incoming solar radiation increases the 
planetary albedo and cools the surface, with a tropospheric H2O decrease. (b) 
The tropospheric UV budget is upset by the additional aerosol scattering and 
stratospheric ozone changes: the net effect is meridionally not uniform, with a 
net decrease in the tropics, thus producing less tropospheric O(1D). (c) The 
extratropical downwelling motion from the lower stratosphere tends to increase 
the sulfate aerosol surface area density available for heterogeneous chemical 
reactions in the mid-to-upper troposphere, thus reducing the amount of NOx and 
O3 production. (d) The tropical lower stratosphere is warmed by solar and 
planetary radiation absorption by the aerosols. The heating rate perturbation 
is highly latitude dependent, producing a stronger meridional component of the 
Brewer–Dobson circulation. The net effect on tropospheric OH due to the 
enhanced stratosphere–troposphere exchange may be positive or negative 
depending on the net result of different superimposed species perturbations 
(CH4, NOy, O3, SO4) in the extratropical upper troposphere and lower 
stratosphere (UTLS). In addition, the atmospheric stabilization resulting from 
the tropospheric cooling and lower stratospheric warming favors an additional 
decrease of the UTLS extratropical CH4 by lowering the horizontal eddy mixing. 
Two climate–chemistry coupled models are used to explore the above radiative, 
chemical and dynamical mechanisms affecting CH4 transport and lifetime 
(ULAQ-CCM and GEOSCCM). The CH4 lifetime may become significantly longer (by 
approximately 16 %) with a sustained injection of 8 Tg-SO2 yr−1 starting in the 
year 2020, which implies an increase of tropospheric CH4 (200 ppbv) and a 
positive indirect radiative forcing of sulfate geoengineering due to CH4 
changes (+0.10 W m−2 in the 2040–2049 decade and +0.15 W m−2 in the 2060–2069 
decade).

 

 

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