Li<SUP>+</SUP> Dynamics of Liquid Electrolytes Nanoconfined in Metal-Organic Frameworks



Farina, Marco, Duff, Benjamin B ORCID: 0000-0002-7398-5002, Tealdi, Cristina, Pugliese, Andrea, Blanc, Frederic ORCID: 0000-0001-9171-1454 and Quartarone, Eliana
(2021) Li<SUP>+</SUP> Dynamics of Liquid Electrolytes Nanoconfined in Metal-Organic Frameworks. ACS APPLIED MATERIALS & INTERFACES, 13 (45). pp. 53986-53995.

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Abstract

Metal-organic frameworks (MOFs) are excellent platforms to design hybrid electrolytes for Li batteries with liquid-like transport and stability against lithium dendrites. We report on Li<sup>+</sup> dynamics in quasi-solid electrolytes consisting in Mg-MOF-74 soaked with LiClO<sub>4</sub>-propylene carbonate (PC) and LiClO<sub>4</sub>-ethylene carbonate (EC)/dimethyl carbonate (DMC) solutions by combining studies of ion conductivity, nuclear magnetic resonance (NMR) characterization, and spin relaxometry. We investigate nanoconfinement of liquid inside MOFs to characterize the adsorption/solvation mechanism at the basis of Li<sup>+</sup> migration in these materials. NMR supports that the liquid is nanoconfined in framework micropores, strongly interacting with their walls and that the nature of the solvent affects Li<sup>+</sup> migration in MOFs. Contrary to the "free'' liquid electrolytes, faster ion dynamics and higher Li<sup>+</sup> mobility take place in LiClO<sub>4</sub>-PC electrolytes when nanoconfined in MOFs demonstrating superionic conductor behavior (conductivity σ<sub>rt</sub> > 0.1 mS cm<sup>-1</sup>, transport number <i>t</i><sub>Li<sup>+</sup></sub> > 0.7). Such properties, including a more stable Li electrodeposition, make MOF-hybrid electrolytes promising for high-power and safer lithium-ion batteries.

Item Type: Article
Uncontrolled Keywords: nanoconfinement, lithium-ion batteries, metal-organic frameworks, dendrites, quasi-solid electrolytes
Divisions: Faculty of Science and Engineering > School of Physical Sciences
Depositing User: Symplectic Admin
Date Deposited: 09 Nov 2021 15:50
Last Modified: 19 Oct 2023 08:42
DOI: 10.1021/acsami.1c16214
Related URLs:
URI: https://livrepository.liverpool.ac.uk/id/eprint/3142968