Orbital hybridization states of carbon functionalize the alkali-ion storage capability of hard carbons

Experimentally, hard carbons (HCs) synthesized under different conditions always show various alkali-ion ( e.g. , Li + , Na + , and K + ) storage capabilities. However, the diversity of the precursor and the uncertain amorphous microstructure make it difficult to fully understand the origination of...

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Published in:Journal of materials chemistry. A, Materials for energy and sustainability Materials for energy and sustainability, 2023-02, Vol.11 (6), p.2947-2956
Main Authors: Yang, Ying, Huang, Chenli, Zhao, Ruirui, Gao, Zhonghui, Qi, Xiaoqun, Zhang, Wang, Lu, Xing, Qie, Long, Huang, Yunhui
Format: Article
Language:English
Subjects:
Batteries
Buckminsterfullerene
Carbon
Electrochemistry
Electrode materials
Fullerenes
Hybridization
Ion storage
Lithium
Metal ions
Precursors
Sodium
Specific capacity
Spectrometry
Storage
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Summary:Experimentally, hard carbons (HCs) synthesized under different conditions always show various alkali-ion ( e.g. , Li + , Na + , and K + ) storage capabilities. However, the diversity of the precursor and the uncertain amorphous microstructure make it difficult to fully understand the origination of the electrochemical variety of HCs. Herein, fullerene (C 60 ), a heteroatom-free and structure-confirmed precursor, is chosen to build "pure" carbon models (C 60 - T s ) for exploring the correlations between inherent characteristics and alkali-ion storage behaviors in HCs. The electrochemical results indicate that the C 60 -800 sample exhibits the highest specific capacity and best rate capability for Li + , Na + , and K + storage. Various spectrometric characterizations and theoretical simulations demonstrate that the extra capacity of C 60 -800 mainly originates from the higher ratio of sp 3 and sp 2 -hybridized carbon atoms (sp 3 /sp 2 -C). The existence of sp 3 -C could affect the local electronic distribution around sp 2 -C and even lower the absorption energy of alkali-ions. This work presents a novel orbital hybridization state-related strategy for designing high-capacity electrode materials of alkali-ion batteries. A series of "pure" hard carbon models, built using C 60 as precursor, help to correlate the alkali-ion ( e.g. , Li + , Na + , and K + ) storage behaviour of hard carbons to orbital hybridization states of carbon atoms.
ISSN:2050-7488
2050-7496
DOI:10.1039/d2ta08691c