Operando characterization and regulation of metal dissolution and redeposition dynamics near battery electrode surface

Zhang, Yuxin; Hu, Anyang; Xia, Dawei; Hwang, Sooyeon; Sainio, Sami; Nordlund, Dennis; Michel, F. Marc; Moore, Robert B.; Li, Luxi; Lin, Feng

doi:10.1038/s41565-023-01367-6

Operando characterization and regulation of metal dissolution and redeposition dynamics near battery electrode surface

Journal Article · Thu Apr 20 00:00:00 EDT 2023 · Nature Nanotechnology

DOI:https://doi.org/10.1038/s41565-023-01367-6· OSTI ID:1974182

Zhang, Yuxin ^[1]; ^[1]; Xia, Dawei ^[1]; ^[2]; Sainio, Sami ^[3]; Nordlund, Dennis ^[3]; ^[1]; ^[1]; ^[4]; ^[1]

Virginia Polytechnic Institute and State University (Virginia Tech), Blacksburg, VA (United States)
Brookhaven National Laboratory (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN)
SLAC National Accelerator Laboratory, Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL)
Argonne National Laboratory (ANL), Lemont, IL (United States). Advanced Photon Source (APS)

Mn dissolution has been a longstanding, ubiquitous issue that negatively impacts the performance of Mn-based battery materials. Mn dissolution involves complex chemical and structural transformations at the electrode-electrolyte interface. The continuously evolving electrodeelectrolyte interface has posed great challenges for characterizing the dynamic interfacial process and quantitatively establishing the correlation with battery performance. In this study, we visualize and quantify the temporally and spatially resolved Mn dissolution/redeposition (D/R) dynamics of electrochemically operating Mn-containing cathodes. The particle-level and electrode-level analyses reveal that the D/R dynamics is associated with distinct interfacial degradation mechanisms at different states of charge. Our results statistically differentiate the contributions of surface reconstruction and Jahn-Teller distortion to the Mn dissolution at different operating voltages. Introducing sulfonated polymers (Nafion) into composite electrodes can modulate the D/R dynamics through trapping the dissolved Mn species and rapidly establishing the local Mn D/R equilibrium. This work represents an inaugural effort to pinpoint the chemical and structural transformations responsible for Mn dissolution via an operando synchrotron study and develops an effective method to regulate Mn interfacial dynamics for improving battery performance.

View Accepted Manuscript (DOE)

Research Organization:: Argonne National Laboratory (ANL), Lemont, IL (United States); Brookhaven National Laboratory (BNL), Upton, NY (United States); SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)

Sponsoring Organization:: National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-06CH11357; AC02-76SF00515; SC0012704

OSTI ID:: 1974182

Alternate ID(s):: OSTI ID: 2229844

Report Number(s):: BNL--224405-2023-JAAM

Journal Information:: Nature Nanotechnology, Journal Name: Nature Nanotechnology Vol. 18; ISSN 1748-3387

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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