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

doi:10.1038/s41467-019-13424-7

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

Journal Article · 27 November 2019 · Nature Communications

DOI: https://doi.org/10.1038/s41467-019-13424-7 · OSTI ID:1591836

^[1];

^[2];

^[3]; Qian, Kun ^[1];

^[3]; Liu, Tao ^[3]; Li, Yuhong ^[1]; Shen, Li ^[1]; Ke, Xiaokang ^[1];

^[1];

^[1]; Magusin, Pieter C. M. M. ^[3];

^[4]; Ding, Weiping ^[1]; Gong, Xue-Qing ^[5]; Grey, Clare P. ^[3];

^[1]

Nanjing Univ. (China)
East China Univ. of Science and Technology, Shanghai (China); Univ. of Minnesota, Minneapolis, MN (United States)
Univ. of Cambridge (United Kingdom)
Univ. of Nottingham (United Kingdom)
East China Univ. of Science and Technology, Shanghai (China)

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.

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Research Organization:: Energy Frontier Research Centers (EFRC) (United States). Northeastern Center for Chemical Energy Storage (NECCES); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: AC02-05CH11231; SC0012583

OSTI ID:: 1591836

Journal Information:: Nature Communications, Journal Name: Nature Communications Journal Issue: 1 Vol. 10; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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

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