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Origin of enhanced reversible Na ion storage in hard carbon anodes through p-type molecular doping

Authors
Lee, Gi-HyeokHwang, TaesoonKim, Jae-BumYang, JunghoonZou, FengCho, MaenghyoKang, Yong-Mook
Issue Date
10-8월-2022
Publisher
ROYAL SOC CHEMISTRY
Citation
JOURNAL OF MATERIALS CHEMISTRY A, v.10, no.31, pp.16506 - 16513
Indexed
SCIE
SCOPUS
Journal Title
JOURNAL OF MATERIALS CHEMISTRY A
Volume
10
Number
31
Start Page
16506
End Page
16513
URI
https://scholar.korea.ac.kr/handle/2021.sw.korea/143784
DOI
10.1039/d2ta02295h
ISSN
2050-7488
Abstract
Na-ion batteries (SIBs) require novel anode materials which have high ion storage capability and low working voltage to make SIBs competitive compared to Li-ion batteries (LIBs). From this perspective, we present the origin of improved electrochemical performances of phosphate doped hard carbon (P-HC) which can meet the two requirements mentioned above through combining experiment with the calculations of atomic/electronic structures. We disclosed that the capacity enhancement is accompanied by the changed voltage profile, which results from the introduced phosphate functional groups. The emerged redox peak turned out to be generated by the electrochemical reaction of Na ions near the phosphate-carbon environment. First-principles calculations elaborated that the phosphate introduction here generates electron holes near the Fermi level that is generally considered as evidence of p-type semiconductors to improve electronic conductivity. This expectation has been proven by comparatively measuring the electrical conductivities of pristine hard carbon and P-HC. A close investigation into charge distribution indicated that the electron hole is generated mainly by the higher reducibility of the doped phosphate than the surrounding carbon atoms in P-HC. This discovery well explains the underlying principles for the enhanced electrochemical performance of P-HC, thereby showing a way to design highly functional hard carbon structures toward higher capacity with Na ions.
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공과대학 (신소재공학부)
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