Fundamental mechanistic insights into the catalytic reactions of Li-S redox by Co single-atom electrocatalysts via operando methods

Xu, Weixuan; Lang, Shuangyan; Wang, Kaiyang; Zeng, Rui; Li, Huiqi; Feng, Xinran; Krumov, Mihail R.; Bak, Seong-Min; Pollock, Christopher J.; Yeo, Jingjie; Du, Yonghua; Abruña, Héctor D.

doi:10.1126/sciadv.adi5108

Fundamental mechanistic insights into the catalytic reactions of Li-S redox by Co single-atom electrocatalysts via operando methods

Journal Article · Wed Aug 16 00:00:00 EDT 2023 · Science Advances

DOI:https://doi.org/10.1126/sciadv.adi5108· OSTI ID:2204608

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Cornell University, Ithaca, NY (United States)
Yonsei University, Seoul (Korea, Republic of)
Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)

Lithium-sulfur batteries represent an attractive option for energy storage applications. A deeper understanding of the multistep lithium-sulfur reactions and the electrocatalytic mechanisms are required to develop advanced, high-performance batteries. We have systematically investigated the lithium-sulfur redox processes catalyzed by a cobalt single-atom electrocatalyst (Co-SAs/NC) via operando confocal Raman microscopy and x-ray absorption spectroscopy (XAS). The real-time observations, based on potentiostatic measurements, indicate that Co-SAs/NC efficiently accelerates the lithium-sulfur reduction/oxidation reactions, which display zero-order kinetics. Under galvanostatic discharge conditions, the typical stepwise mechanism of long-chain and intermediate-chain polysulfides is transformed to a concurrent pathway under electrocatalysis. In addition, operando cobalt K-edge XAS studies elucidate the potential-dependent evolution of cobalt’s oxidation state and the formation of cobalt-sulfur bonds. Our work provides fundamental insights into the mechanisms of catalyzed lithium-sulfur reactions via operando methods, enabling a deeper understanding of electrocatalysis and interfacial dynamics in electrical energy storage systems.

View Accepted Manuscript (DOE)

Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Organization:: National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)

Grant/Contract Number:: SC0012704

OSTI ID:: 2204608

Report Number(s):: BNL--224956-2023-JAAM

Journal Information:: Science Advances, Journal Name: Science Advances Journal Issue: 33 Vol. 9; ISSN 2375-2548

Publisher:: AAASCopyright Statement

Country of Publication:: United States

Language:: English

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