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Thickness-independent scalable high-performance Li-S batteries with high areal sulfur loading via electron-enriched carbon framework.

ABSTRACT: Increasing the energy density of lithium-sulfur batteries necessitates the maximization of their areal capacity, calling for thick electrodes with high sulfur loading and content. However, traditional thick electrodes often lead to sluggish ion transfer kinetics as well as decreased electronic conductivity and mechanical stability, leading to their thickness-dependent electrochemical performance. Here, free-standing and low-tortuosity N, O co-doped wood-like carbon frameworks decorated with carbon nanotubes forest (WLC-CNTs) are synthesized and used as host for enabling scalable high-performance Li-sulfur batteries. EIS-symmetric cell examinations demonstrate that the ionic resistance and charge-transfer resistance per unit electro-active surface area of S@WLC-CNTs do not change with the variation of thickness, allowing the thickness-independent electrochemical performance of Li-S batteries. With a thickness of up to 1200 µm and sulfur loading of 52.4 mg cm^-2, the electrode displays a capacity of 692 mAh g^-1 after 100 cycles at 0.1 C with a low E/S ratio of 6. Moreover, the WLC-CNTs framework can also be used as a host for lithium to suppress dendrite growth. With these specific lithiophilic and sulfiphilic features, Li-S full cells were assembled and exhibited long cycling stability.

SUBMITTER: Wang N

PROVIDER: S-EPMC8313709 | biostudies-literature |

REPOSITORIES: biostudies-literature

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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.

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Thickness-independent scalable high-performance Li-S batteries with high areal sulfur loading via electron-enriched carbon framework.

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