Low-temperature atomic layer deposition of SiO2/Al2O3 multilayer structures constructed on self-standing films of cellulose nanofibrils

Matti Putkonen, Perttu Sippola, Laura Svärd, Timo Sajavaara, Jari Vartiainen, Iain Buchanan, Ulla Forsström, Pekka Simell, Tekla Tammelin (Corresponding Author)

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    In this paper, we have optimized a low-temperature atomic layer deposition (ALD) of SiO2 using AP-LTO® 330 and ozone (O3) as precursors, and demonstrated its suitability to surface-modify temperature-sensitive bio-based films of cellulose nanofibrils (CNFs). The lowest temperature for the thermal ALD process was 80°C when the silicon precursor residence time was increased by the stop-flow mode. The SiO2 film deposition rate was dependent on the temperature varying within 1.5-2.2 Å cycle-1 in the temperature range of 80-350°C, respectively. The low-temperature SiO2 process that resulted was combined with the conventional trimethyl aluminium + H2O process in order to prepare thin multilayer nanolaminates on self-standing CNF films. One to six stacks of SiO2/Al2O3 were deposited on the CNF films, with individual layer thicknesses of 3.7 nm and 2.6 nm, respectively, combined with a 5 nm protective SiO2 layer as the top layer. The performance of the multilayer hybrid nanolaminate structures was evaluated with respect to the oxygen and water vapour transmission rates. Six stacks of SiO2/Al2O with a total thickness of approximately 35 nm efficiently prevented oxygen and water molecules from interacting with the CNF film. The oxygen transmission rates analysed at 80% RH decreased from the value for plain CNF film of 130 ml m-2 d-1 to 0.15 ml m-2 d-1, whereas the water transmission rates lowered from 630 ± 50 g m-2 d-1 down to 90 ± 40 g m-2 d-1.This article is part of a discussion meeting issue 'New horizons for cellulose nanotechnology'.

    Original languageEnglish
    Article number20170037
    JournalPhilosophical Transactions of the Royal Society A: Mathematical, Physical and Engineering Sciences
    Issue number2112
    Publication statusPublished - 13 Feb 2018
    MoE publication typeA1 Journal article-refereed


    The research has received funding from the European Union Seventh Framework Programme (FP7/2007-2013, Grant agreement no 603519; FP7-ICT-2013-10, Grant agreement no 611230), Academy of Finland Project ID 263577 (M.P.) and Academy of Finland Project ID 300367 (T.T.). Acknowledgements. Ms Katja Pettersson is thanked for the AFM imaging and Ms Mirja Nygård for the SEM imaging. Mr Vesa Kunnari and Mr Timo Kaljunen are acknowledged for the CNF film production.


    • Cellulose nanofibrils
    • Diffusion barrier
    • Hybrid multilayers
    • Low-temperature atomic layer deposition
    • SiO
    • Water sensitivity


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