Polar surface structure of oxide nanocrystals revealed with solid-state NMR spectroscopy

Chen, Junchao; Wu, Xin Ping; Hope, Michael A.; Qian, Kun; Halat, David M.; Liu, Tao; Li, Yuhong; Shen, Li; Ke, Xiaokang; Wen, Yujie; Du, Jia Huan; Magusin, Pieter C. M. M.; Paul, Subhradip; Ding, Weiping; Gong, Xue Qing; Grey, Clare P.; Peng, Luming

Abstract

© 2019, The Author(s). Compared to nanomaterials exposing nonpolar facets, polar-faceted nanocrystals often exhibit unexpected and interesting properties. The electrostatic instability arising from the intrinsic dipole moments of polar facets, however, leads to different surface configurations in many cases, making it challenging to extract detailed structural information and develop structure-property relations. The widely used electron microscopy techniques are limited because the volumes sampled may not be representative, and they provide little chemical bonding information with low contrast of light elements. With ceria nanocubes exposing (100) facets as an example, here we show that the polar surface structure of oxide nanocrystals can be investigated by applying 17O and 1H solid-state NMR spectroscopy and dynamic nuclear polarization, combined with DFT calculations. Both CeO4-termination reconstructions and hydroxyls are present for surface polarity compensation and their concentrations can be quantified. These results open up new possibilities for investigating the structure and properties of oxide nanostructures with polar facets.

Citation

Chen, J., Wu, X. P., Hope, M. A., Qian, K., Halat, D. M., Liu, T., …Peng, L. (2019). Polar surface structure of oxide nanocrystals revealed with solid-state NMR spectroscopy. Nature Communications, 10(1), Article 5420. https://doi.org/10.1038/s41467-019-13424-7

• Journal Article Type: Article
• Acceptance Date: Nov 7, 2019
• Online Publication Date: Nov 28, 2019
• Publication Date: Dec 1, 2019
• Deposit Date: Dec 13, 2019
• Publicly Available Date: Dec 17, 2019
• Journal: Nature Communications
• Electronic ISSN: 2041-1723
• Publisher: Nature Publishing Group
• Peer Reviewed: Peer Reviewed
• Volume: 10
• Issue: 1
• Article Number: 5420
• DOI: https://doi.org/10.1038/s41467-019-13424-7
• Keywords: General Biochemistry, Genetics and Molecular Biology; General Physics and Astronomy; General Chemistry
• Public URL: https://nottingham-repository.worktribe.com/output/3547963
• Additional Information: Received: 6 March 2019; Accepted: 7 November 2019; First Online: 28 November 2019; : The authors declare no competing interests.