https://www.nature.com/articles/s43247-020-00058-7

Experimental reaction rates constrain estimates of ozone response to
calcium carbonate geoengineering
Zhen Dai, Debra K. Weisenstein, […]David W. Keith
Communications Earth & Environment volume 1, Article number: 63 (2020) Cite
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Abstract
Stratospheric solar geoengineering (SG) would impact ozone by heterogeneous
chemistry. Evaluating these risks and methods to reduce them will require
both laboratory and modeling work. Prior model-only work showed that CaCO3
particles would reduce, or even reverse ozone depletion. We reduce
uncertainties in ozone response to CaCO3 via experimental determination of
uptake coefficients and model evaluation. Specifically, we measure uptake
coefficients of HCl and HNO3 on CaCO3 as well as HNO3 and ClONO2 on CaCl2
at stratospheric temperatures using a flow tube setup and a flask
experiment that determines cumulative long-term uptake of HCl on CaCO3. We
find that particle ageing causes significant decreases in uptake
coefficients on CaCO3. We model ozone response incorporating the
experimental uptake coefficients in the AER-2D model. With our new
empirical reaction model, the global mean ozone column is reduced by up to
3%, whereas the previous work predicted up to 27% increase for the same SG
scenario. This result is robust under our experimental uncertainty and many
other assumptions. We outline systematic uncertainties that remain and
provide three examples of experiments that might further reduce
uncertainties of CaCO3 SG. Finally, we highlight the importance of the link
between experiments and models in studies of SG.

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