Ice nucleation by cellulose and its potential contribution to ice formation in clouds

Abstract

Ice particles in the atmosphere influence clouds, precipitation and climate, and often form with help from aerosols that serve as ice-nucleating particles. Biological particles1, including non-proteinaceous ones2,3, contribute to the diverse spectrum of ice-nucleating particles4,5. However, little is known about their atmospheric abundance and ice nucleation efficiency, and their role in clouds and the climate system is poorly constrained6. One biological particle type, cellulose, has been shown to exist in an airborne form that is prevalent throughout the year even at remote and elevated locations7,8. Here we report experiments in a cloud simulation chamber9 to demonstrate that microcrystalline cellulose particles can act as efficient ice-nucleating particles in simulated supercooled clouds. In six immersion mode freezing experiments, we measured the ice nucleation active surface-site densities of aerosolized cellulose across a range of temperatures. Using these active surface-site densities, we developed parameters describing the ice nucleation ability of these particles10 and applied them to observed atmospheric cellulose and plant debris concentrations in a global aerosol model. We find that ice nucleation by cellulose becomes significant (>0.1 l−1) below about −21 °C, temperatures relevant to mixed-phase clouds. We conclude that the ability of cellulose to act as ice-nucleating particles requires a revised quantification of their role in cloud formation and precipitation.

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Figure 1: Surface area distributions of cellulose particles.
Figure 2: Ice nucleation active surface-site density spectra for immersion freezing of MCC particles.
Figure 3: Average potential INP spectra.

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Acknowledgements

The authors acknowledge partial financial support by the Helmholtz Association through its research programme ‘Atmosphere and Climate (ATMO)’ and the Deutsche Forschungsgemeinschaft (DFG) through the Research Unit FOR 1525 (INUIT, grant No MO668/4-1, KO2944/2-1 and HO4612/1-1). This work was partly supported by JSPS KAKENHI Grant Number 23244095. O. Seland, D. Olivié and A. Kirkevåg are acknowledged for providing the CAM4-Oslo simulations. Technical support from T. Kisely for the BET measurements is acknowledged. N.Hiranuma acknowledges A. Abdelmonem, C. Anquetil-Deck and T. C. J. Hill for useful discussion on BINPs. N.Hiranuma and O.M. thank P. Weidler for the XRD measurements and data interpretation. E. Jantsch and T. Koop thank C. Budke for helpful suggestions on the BINARY experiments. The authors also express their thanks for technical support from S. Shutthanandan and G. Kulkarni with the HIM measurements. HIM research was performed in the Environmental Molecular Science Laboratory, a DOE Office of Science User Facility sponsored by the Office of Biological and Environmental Research and located at Pacific Northwest National Laboratory.

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M.M. and O.M. proposed the framework of this collaborative project. N.Hiranuma and O.M. principally designed and conceived the experiments with subsequent input on experimental techniques from M.M., K.Y., T.T. and A.S.; K.Y., T.T. and A.S. performed the experiments with assistance and contributions from N.Hiranuma and O.M. using the DCECC at MRI. SEM on collected filters was carried out by A.K. and N.Hoffmann at KIT. E.J. and T.K. conceived, performed and analysed the BINARY experiments. N.Hiranuma and C.H. analysed the results and wrote the manuscript. All authors discussed the results and contributed to the final version of manuscript.

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Correspondence to N. Hiranuma.

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The authors declare no competing financial interests.

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Hiranuma, N., Möhler, O., Yamashita, K. et al. Ice nucleation by cellulose and its potential contribution to ice formation in clouds. Nature Geosci 8, 273–277 (2015). https://doi.org/10.1038/ngeo2374

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