• Peer-Reviewed
Communications Earth & Environment · 2020

Experimental reaction rates constrain estimates of ozone response to calcium carbonate geoengineering

Zhen Dai, Debra K. Weisenstein, Frank N. Keutsch and David W. Keith

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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