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Ultra-high Areal Capacity Realized in Three-Dimensional Holey Graphene/SnO2 Composite Anodes.

ABSTRACT: Nanostructured alloy-type electrode materials and its composites have shown extraordinary promise for lithium-ion batteries (LIBs) with exceptional gravimetric capacity. However, studies to date are usually limited to laboratory cells with too low mass loading (and thus too low areal capacity) to exert significant practical impact. Herein, by impregnating micrometer-sized SnO2/graphene composites into 3D holey graphene frameworks (HGF), we show that a well-designed 3D-HGF/SnO2 composite anode with a high mass loading of 12 mg cm-2 can deliver an ultra-high areal capacity up to 14.5 mAh cm-2 under current density of 0.2 mA cm-2 and stable areal capacity of 9.5 mAh cm-2 under current density of 2.4 mA cm-2, considerably outperforming those in the state-of-art research devices or commercial devices. This robust realization of high areal capacity defines a critical step to capturing the full potential of high-capacity alloy-type electrode materials in practical LIBs.

SUBMITTER: Liang J

PROVIDER: S-EPMC6726882 | biostudies-literature | 2019 Sep

REPOSITORIES: biostudies-literature

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Ultra-high Areal Capacity Realized in Three-Dimensional Holey Graphene/SnO2 Composite Anodes.

Liang Junfei J Sun Hongtao H Zhao Zipeng Z Wang Yiliu Y Feng Zhiying Z Zhu Jian J Guo Lin L Huang Yu Y Duan Xiangfeng X

iScience 20190820

Nanostructured alloy-type electrode materials and its composites have shown extraordinary promise for lithium-ion batteries (LIBs) with exceptional gravimetric capacity. However, studies to date are usually limited to laboratory cells with too low mass loading (and thus too low areal capacity) to exert significant practical impact. Herein, by impregnating micrometer-sized SnO2/graphene composites into 3D holey graphene frameworks (HGF), we show that a well-designed 3D-HGF/SnO2</s ...[more]

PMID: 31476619

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Project description:Li-S batteries (LSBs) require a minimum 6 mAh cm-2 areal capacity to compete with the state-of-the-art lithium ion batteries (LIBs). However, this areal capacity is difficult to achieve due to a major technical issue-the shuttle effect. Nonpolar carbon materials limit the shuttle effect through physical confinement. However, the polar polysulfides (PSs) only provide weak intermolecular interactions (0.1-0.7 eV) with these nonpolar carbon materials. The physically encapsulated PSs inside the nonpolar carbon scaffold eventually diffuses out and starts shuttling. Chemically interactive hosts are more effective at interacting with the PSs due to high binding energies. Herein, a multifunctional separator coating of nitrogen-doped multilayer graphene (NGN) and -SO3 - containing Nafion (N-NGN) is used to mitigate PS shuttling and to produce a high areal capacity LSB. The Nafion is used as a binder instead of PVDF to provide an additional advantage of -SO3 - to chemically bind the PS. The motive of this research is to investigate the effect of highly electronegative N and -SO3 - (N-NGN) in comparison with the -OH, -COOH, and -SO3 - groups from a hydroxyl graphene and Nafion composite (N-OHGN) to mitigate PS shuttling in LSBs. The highly conductive doped graphene architecture (N-NGN) provides efficient pathways for both electrons and ions, which accelerates the electrochemical conversion at high sulfur loading. Moreover, the electron-rich pyridine N and -SO3 - show strong chemical affinity with the PS through polar-polar interactions, which is proven by the superior electrochemical performance and density functional theory calculations. Further, the N-NGN (5 h) produces a maximum areal capacity of 12.0 and 11.0 mAh cm-2, respectively, at 15 and 12 mg cm-2 sulfur loading. This areal capacity limit is significantly higher than the required areal capacity of LSBs for commercial application, which shows the significant strength of N-NGN as an excellent separator coating for LSBs.

Dataset Information

Ultra-high Areal Capacity Realized in Three-Dimensional Holey Graphene/SnO2 Composite Anodes.

Publications

Ultra-high Areal Capacity Realized in Three-Dimensional Holey Graphene/SnO<sub>2</sub> Composite Anodes.

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