Ion Conducting Polymer Interfaces for Lithium Metal Anodes: Impact on the Electrodeposition Kinetics

Choudhury, Snehashis; Huang, Zhuojun; Amanchukwu, Chibueze V.; Rudnicki, Paul E.; Chen, Yuelang; Boyle, David Thomas; Qin, Jian; Cui, Yi; Bao, Zhenan

doi:10.1002/aenm.202301899

Ion Conducting Polymer Interfaces for Lithium Metal Anodes: Impact on the Electrodeposition Kinetics

Journal Article · Fri Jul 28 00:00:00 EDT 2023 · Advanced Energy Materials

DOI:https://doi.org/10.1002/aenm.202301899· OSTI ID:1998185

Choudhury, Snehashis ^[1]; Huang, Zhuojun ^[2]; Amanchukwu, Chibueze V. ^[2]; ^[2]; Chen, Yuelang ^[2]; Boyle, David Thomas ^[3]; Qin, Jian ^[2]; Cui, Yi ^[4]; ^[2]

Stanford Univ., CA (United States); SLAC
Stanford Univ., CA (United States)
Department of Chemistry Stanford University Stanford CA 94305 USA
Stanford Univ., CA (United States); SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States). Stanford Institute for Materials and Energy Science (SIMES)

Electrochemical cells that utilize metals (e.g., lithium, sodium, zinc) as anodes are under intense investigation as they are projected to replace the current lithium-ion batteries to serve as a more energy-dense option for commercial applications. In addition, metal electrodes provide opportunities for fundamental research of different phenomena, such as ion transport and electrochemical kinetics, in the complex environment of reactive metal-electrodeposition. In this work, computationally and experimentally the competing effects related to transport and kinetics during the metal electrodeposition process are examined. Using Brownian dynamics simulations, it is shown that slower deposition kinetics results in a more compact and uniform Li morphology. This finding is experimentally implemented by designing ion-containing polymeric coatings on the electrodes that simultaneously provide pathways for lithium-ion transport, while impeding the charge transfer (Li⁺ + e^- → Li) at heterogeneous surfaces. It is further shown that these ionic polymer interfaces can significantly extend the cell-lifetime of a lithium metal battery in both ether-based and carbonate-based electrolytes. Through theoretical and experimental investigations, it is found that a low kinetic to transport rate ratio is a major factor in influencing the Li plating morphology. The plating morphology can be further fine-tuned by increasing ionic conductivity.

View Accepted Manuscript (DOE)

Research Organization:: SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)

Sponsoring Organization:: USDOE; USDOE Office of Energy Efficiency and Renewable Energy (EERE)

Grant/Contract Number:: AC02-76SF00515

OSTI ID:: 1998185

Alternate ID(s):: OSTI ID: 1995920

Journal Information:: Advanced Energy Materials, Journal Name: Advanced Energy Materials Journal Issue: 35 Vol. 13; ISSN 1614-6832

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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