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Engineering Catalytic CoSe-ZnSe Heterojunctions Anchored on Graphene Aerogels for Bidirectional Sulfur Conversion Reactions.

ABSTRACT: Sluggish sulfur reduction and lithium sulfide (Li₂ S) oxidation prevent the widespread use of lithium-sulfur (Li-S) batteries, which are attractive alternatives to Li-ion batteries. The authors propose that a transition metal selenide heterojunction (CoSe-ZnSe) catalytically accelerates bidirectional sulfur conversion reactions. A combination of synchrotron X-ray absorption spectroscopy and density functional theory calculations show that a highly active heterointerface with charge redistribution and structure distortion effectively immobilizes sulfur species, facilitates Li ion diffusion, and decreases the sulfur reduction and Li₂ S oxidation energy barriers. The CoSe-ZnSe catalytic cathode exhibits high areal capacities, good rate capability, and superior cycling stability with capacity fading rate of 0.027% per cycle over 1700 cycles. Furthermore, CoSe-ZnSe heterojunctions anchored on graphene aerogels (CoSe-ZnSe@G) enhance ionic transport and catalytic activity under high sulfur loading and lean electrolyte conditions. A high areal capacity of 8.0 mAh cm^-2 is achieved at an electrolyte/sulfur ratio of 3 µL mg^-1 . This study demonstrates the importance of bidirectional catalytic heterojunctions and structure engineering in boosting Li-S battery performances.

SUBMITTER: Ye Z

PROVIDER: S-EPMC8728854 | 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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Engineering Catalytic CoSe-ZnSe Heterojunctions Anchored on Graphene Aerogels for Bidirectional Sulfur Conversion Reactions.

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