Phosphate-functionalized Zirconium Metal-Organic Frameworks for Enhancing Lithium-Sulfur Battery Cycling.

Autor: Liu B; Department of Chemistry, Johns Hopkins University, Baltimore, MD 21218, United States., Baumann AE; Department of Chemistry, Johns Hopkins University, Baltimore, MD 21218, United States.; National Institute of Standards and Technology, Gaithersburg, MD 20899, USA., Butala MM; National Institute of Standards and Technology, Gaithersburg, MD 20899, USA.; Department of Materials Science and Engineering, University of Florida, Gainesville, FL 32611, USA., Thoi VS; Department of Chemistry, Johns Hopkins University, Baltimore, MD 21218, United States.; Department of Materials Science and Engineering, Johns Hopkins University, Baltimore, MD 21218, United States.
Jazyk: angličtina
Zdroj: Chemistry (Weinheim an der Bergstrasse, Germany) [Chemistry] 2023 Jul 14; Vol. 29 (40), pp. e202300821. Date of Electronic Publication: 2023 May 30.
DOI: 10.1002/chem.202300821
Abstrakt: Lithium-sulfur batteries are promising candidates for next-generation energy storage devices due to their outstanding theoretical energy density. However, they suffer from low sulfur utilization and poor cyclability, greatly limiting their practical implementation. Herein, we adopted a phosphate-functionalized zirconium metal-organic framework (Zr-MOF) as a sulfur host. With their porous structure, remarkable electrochemical stability, and synthetic versatility, Zr-MOFs present great potential in preventing soluble polysulfides from leaching. Phosphate groups were introduced to the framework post-synthetically since they have shown a strong affinity towards lithium polysulfides and an ability to facilitate Li ion transport. The successful incorporation of phosphate in MOF-808 was demonstrated by a series of techniques including infrared spectroscopy, solid-state nuclear magnetic resonance spectroscopy, and X-ray pair distribution function analysis. When employed in batteries, phosphate-functionalized Zr-MOF (MOF-808-PO4) exhibits significantly enhanced sulfur utilization and ion diffusion compared to the parent framework, leading to higher capacity and rate capability. The improved capacity retention and inhibited self-discharge rate also demonstrate effective polysulfide encapsulation utilizing MOF-808-PO4. Furthermore, we explored their potential towards high-density batteries by examining the cycling performance at various sulfur loadings. Our approach to correlate structure with function using hybrid inorganic-organic materials offers new chemical design strategies for advancing battery materials.
(© 2023 The Authors. Chemistry - A European Journal published by Wiley-VCH GmbH.)
Databáze: MEDLINE
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