Volume 17, Issue 52 2102109
Research Article

X-Ray Spectromicroscopy Investigation of Heterogeneous Sodiation in Hard Carbon Nanosheets with Vertically Oriented (002) Planes

Xuehai Tan

Xuehai Tan

Department of Chemical and Materials Engineering, University of Alberta, Edmonton, Alberta, T6G 2V4 Canada

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Keren Jiang

Keren Jiang

Department of Chemical and Materials Engineering, University of Alberta, Edmonton, Alberta, T6G 2V4 Canada

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Shengli Zhai

Shengli Zhai

Department of Chemical and Materials Engineering, University of Alberta, Edmonton, Alberta, T6G 2V4 Canada

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Jigang Zhou

Jigang Zhou

Canadian Light Source Inc., University of Saskatchewan, 44 Innovation Boulevard, Saskatoon, Saskatchewan, S7N 2V3 Canada

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Jian Wang

Jian Wang

Canadian Light Source Inc., University of Saskatchewan, 44 Innovation Boulevard, Saskatoon, Saskatchewan, S7N 2V3 Canada

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Ken Cadien

Ken Cadien

Department of Chemical and Materials Engineering, University of Alberta, Edmonton, Alberta, T6G 2V4 Canada

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Zhi Li

Corresponding Author

Zhi Li

Department of Chemical and Materials Engineering, University of Alberta, Edmonton, Alberta, T6G 2V4 Canada

E-mail: [email protected]

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First published: 15 October 2021
Citations: 5

Abstract

Hard carbon (HC) is a promising anode material for sodium-ion batteries, but the performance remains unsatisfactory and the sodiation mechanism in HC is one of the most debated topics. Here, from self-assembled cellulose nanocrystal sheets with crystallographic texture, unique HC nanosheets with vertically oriented (002) planes are fabricated and used as a model HC to investigate the sodiation mechanisms using synchrotron scanning transmission X-ray microscopy (STXM) coupled with analytical transmission electron microscopy (TEM). The model HC simplifies the 3D sodiation in a typical HC particle into a 2D sodiation, which facilitates the visualization of phase transformation at different states of charge. The results for the first time unveil that the sodiation in HC initiates heterogeneously, with multiple propagation fronts proceeding simultaneously, eventually merging into larger aggregates. The spatial correlation between the preferential adsorption and nucleation sites suggests that the heterogeneous nucleation is driven by the local Na-ion concentration, which is determined by defects or heteroatoms that have strong binding to Na ions. By identifying intercalation as the dominant sodium storage mechanism in the model HC, the findings highlight the importance of engineering the graphene layer orientation and the structural heterogeneity of edge sites to enhance the performances.

Conflict of Interest

The authors declare no conflict of interest.

Data Availability Statement

The data that supports the findings of this study are available in the supplementary material of this article.

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