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Unveiling the controversial mechanism of reversible Na storage in TiO2 nanotube arrays: Amorphous versus anatase TiO2

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Abstract

Due to their inherent safety, low cost, and structural stability, TiO2 nanostructures represent a suitable choice as anode materials in sodium-ion batteries. In the recent years, various hypotheses have been proposed regarding the actual mechanism of the reversible insertion of sodium ions in the TiO2 structure, and previous reports are often controversial in this respect. Interestingly, when tested as binder- and conducting additive-free electrodes in laboratory-scale sodium cells, amorphous and crystalline (anatase) TiO2 nanotubular arrays obtained by simple anodic oxidation exhibit peculiar and intrinsically different electrochemical responses. In particular, after the initial electrochemical activation, anatase TiO2 shows excellent rate capability and very stable long-term cycling performance with larger specific capacities, and thus a clearly superior response compared with the amorphous counterpart. To obtain deeper insight, the present materials are thoroughly characterized by scanning electron microscopy and ex situ X-ray diffraction, and the insertion of sodium ions in the TiO2 bulk phases is systematically modeled by density functional theory calculations. The present results may contribute to the development of more systematic screening approaches to identify suitable active materials for highly efficient sodium-based energy storage systems.

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Acknowledgements

Authors would like to thank Mr. Mauro Raimondo for the surface and cross-sectional FESEM/EDX analysis of the as-prepared samples. Prof. Drabold D. A. is kindly acknowledged for providing the amorphous TiO2 coordinates. The computing resources and the related technical support used for this work have been provided by CRESCO/ENEAGRID High Performance Computing infrastructure and its staff [70]. CRESCO/ ENEAGRID High Performance Computing infrastructure is funded by ENEA, the Italian National Agency for New Technologies, Energy and Sustainable Economic Development and by Italian and European research programs, see http://www.cresco.enea.it/english for information. Part of this work is carried out within the activities “Ricerca Sistema Elettrico” funded through contributions to research and development by the Italian Ministry of Economic Development.

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Authors and Affiliations

  1. GAME Lab, CHENERGY Group, Department of Applied Science and Technology - DISAT, Politecnico di Torino, Corso Duca degli Abruzzi 24, 10129, Torino, Italy

    Federico Bella, Giuseppina Meligrana & Claudio Gerbaldi

  2. Department of Chemical Sciences, University of Naples Federico II, Via Cintia 21, University Campus of Monte Sant’Angelo, 80126, Napoli, Italy

    Ana B. Muñoz-García & Michele Pavone

  3. MPMNT Group, Department of Applied Science and Technology - DISAT, Politecnico di Torino, Corso Duca degli Abruzzi 24, 10129, Torino, Italy

    Andrea Lamberti

  4. LITHOPS S.r.l., Strada del Portone 61, 10137, Torino, Italy

    Matteo Destro

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  1. Federico Bella
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Correspondence to Federico Bella or Claudio Gerbaldi.

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Bella, F., Muñoz-García, A.B., Meligrana, G. et al. Unveiling the controversial mechanism of reversible Na storage in TiO2 nanotube arrays: Amorphous versus anatase TiO2 . Nano Res. 10, 2891–2903 (2017). https://doi.org/10.1007/s12274-017-1656-6

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