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Insights on the Mechanism of Na-Ion Storage in Soft Carbon Anode

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† Department of Chemistry, Oregon State University, Corvallis, Oregon, 97331, United States
‡ Environmental Molecular Sciences Laboratory, Pacific Northwest National Laboratory, Richland, Washington 99352, United States
§ Materials Science and Engineering Program, University of California, Riverside, California, 92521, United States
*E-mail: [email protected]
*E-mail: [email protected]
*E-mail: [email protected]
Cite this: Chem. Mater. 2017, 29, 5, 2314–2320
Publication Date (Web):February 27, 2017
https://doi.org/10.1021/acs.chemmater.6b05474
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    Abstract

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    Graphite is the commercial anode for lithium-ion batteries; however, it fails to extend its success to sodium-ion batteries. Recently, we demonstrated that a low-cost amorphous carbon—soft carbon exhibits remarkable rate performance and stable cycling life of Na-ion storage. However, its Na-ion storage mechanism has remained elusive, which has plagued further development of such carbon anodes. Here, we remedy this shortfall by presenting the results from an integrated set of experimental and computational studies that, for the first time, reveal the storage mechanism for soft carbon. We find that sodium ions intercalate into graphenic layers, leading to an irreversible quasi-plateau at ∼0.5 V versus Na+/Na as well as an irreversible expansion seen by in situ transmission electron microscopy (TEM) and X-ray diffraction (XRD). Such a high-potential plateau is correlated to the defective local structure inside the turbostratic stacking of soft carbon and the associated high-binding energies with Na ions, suggesting a trapping mechanism. On the other hand, soft carbon exhibits long sloping regions above and below the quasi-plateau during the first sodiation, where the sloping regions present highly reversible behavior. It is attributed to the more defects contained by soft carbon revealed by neutron total scattering and the associated pair distribution function studies.

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    • Sodation/desodiation profile of Na ions in hard carbon, PTCDA structure, schematic diagram of in situ TEM of SC-1600, ex situ XRD patterns of SC-900, BET results, and GITT profile of SC-900 are included

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