High-efficiency, anode-free lithium–metal batteries with a close-packed homogeneous lithium morphology

Su, Laisuo; Charalambous, Harry; Cui, Zehao; Manthiram, Arumugam

doi:10.1039/d1ee03103a

High-efficiency, anode-free lithium–metal batteries with a close-packed homogeneous lithium morphology

Journal Article · Wed Jan 05 23:00:00 EST 2022 · Energy & Environmental Science

DOI:https://doi.org/10.1039/d1ee03103a· OSTI ID:2217435

Su, Laisuo ^[1]; Charalambous, Harry ^[2]; Cui, Zehao ^[3]; ^[3]

Univ. of Texas, Austin, TX (United States); University of Texas at Austin
Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
Univ. of Texas, Austin, TX (United States)

Anode-free lithium–metal batteries (LMBs) are ideal candidates for high-capacity energy storage as they eliminate the need for a conventional graphite electrode or excess lithium–metal anode. Current anode-free LMBs suffer from low Coulombic efficiency (CE) due to poor lithium stripping efficiency. Advanced electrolyte development is a promising route to maximize lithium plating and stripping CE and minimize capacity fade. However, a poor understanding of the mechanisms by which advanced electrolytes improve performance hampers progress in the practical development of anode-free LMBs. Here, we use synchrotron techniques and other tools to analyze the influence of three commercially available electrolytes on the composition, heterogeneity, kinetics, morphology, and electrochemistry of anode-free LMBs. Advanced electrolytes improve the electrochemical performance of anode-free LMBs by forming much denser and better-packed Li morphologies on a Cu current collector than on the conventional electrolyte. Li plates uniformly over the electrode area with the advanced electrolytes rather than in a few active sites. Inactive crystalline Li with heterogeneous distribution dominates the capacity degradation of anode-free cells, especially with the conventional electrolyte, indicating that reducing the amount of “dead” crystalline Li will significantly improve the cycling stability of anode-free cells. Finally, the understanding of the Li plating and stripping process obtained from this work will accelerate the development of anode-free LMBs with high efficiency.

View Accepted Manuscript (DOE)

Research Organization:: Univ. of Texas, Austin, TX (United States); Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE), Office of Sustainable Transportation. Vehicle Technologies Office (VTO); USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: EE0007762; AC02-06CH11357

OSTI ID:: 2217435

Alternate ID(s):: OSTI ID: 1841293

Journal Information:: Energy & Environmental Science, Journal Name: Energy & Environmental Science Journal Issue: 2 Vol. 15; ISSN 1754-5692

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

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