Mapping Competitive Reduction upon Charging in LiNi0.8Co0.15Al0.05O2 Primary Particles

Wolfman, Mark; Yu, Young-Sang; May, Brian M.; Lebens-Higgins, Zachary W.; Sallis, Shawn; Faenza, Nicholas V.; Pereira, Nathalie; Shirato, Nozomi; Rose, Volker; Shapiro, David A.; Amatucci, Glenn G.; Piper, Louis F. J.; Cabana, Jordi

doi:10.1021/acs.chemmater.0c01986

Mapping Competitive Reduction upon Charging in LiNi_0.8Co_0.15Al_0.05O₂ Primary Particles

Journal Article · Fri Jun 19 00:00:00 UTC 2020 · Chemistry of Materials

DOI:https://doi.org/10.1021/acs.chemmater.0c01986· OSTI ID:1660267

Wolfman, Mark ^[1]; Yu, Young-Sang ^[2]; May, Brian M. ^[3]; Lebens-Higgins, Zachary W. ^[4]; Sallis, Shawn ^[5]; ^[6]; Pereira, Nathalie ^[6]; Shirato, Nozomi ^[7]; Rose, Volker ^[8]; Shapiro, David A. ^[2]; ^[6]; ^[4]; ^[3]

Univ. of Illinois, Chicago, IL (United States); Argonne National Lab. (ANL), Lemont IL (United States). Advanced Photon Source (APS)
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)
Univ. of Illinois, Chicago, IL (United States)
Binghamton Univ., NY (United States)
Binghamton Univ., NY (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)
Rutgers Univ., New Brunswick, NJ (United States)
Argonne National Lab. (ANL), Lemont, IL (United States). Center for Nanoscale Materials
Argonne National Lab. (ANL), Lemont, IL (United States). Advanced Photon Source (APS)

Side reactions involving surface reduction play a critical role in the failure of LiNi_0.8Co_0.15Al_0.05O₂ to reach its theoretical capacity as a cathode material for Li-ion batteries. While macroscopic consequences are known, the underlying nanoscopic mechanisms are not fully elucidated. By coupling X-ray spectroscopy with several X-ray microscopy modalities, we have spatially resolved the extent of Ni oxidation at several states of charge and uncovered heterogeneity that is hidden when considering ensemble measurements alone. The use of morphologically controlled particles enabled high-resolution imaging of these materials, uncovering gradients of Ni oxidation states within individual primary particles. At high states of charge, these gradients revealed regions of possible oxygen deficiency extending deeper into the particle than previously observed. Surface-sensitive X-ray coupled scanning tunneling microscopy allows oxidation states to be measured at the material's surface, showing predominantly Ni^II in the first atomic layer and mixtures of Ni^II with Ni^III/Ni^IV already appearing 1.5 nm into the particle. These results reveal the subtle interplay between irreversible surface transformations and the bulk reactions that ultimately define function, which will refine strategies of surface passivation that are key to overcoming current performance limitations.

View Accepted Manuscript (DOE)

Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS) and Center for Nanoscale Materials (CNM); Binghamton Univ., NY (United States); Energy Frontier Research Centers (EFRC) (United States). NorthEast Center for Chemical Energy Storage (NECCES); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-05CH11231; AC02-06CH11357; SC0012583

OSTI ID:: 1660267

Journal Information:: Chemistry of Materials, Journal Name: Chemistry of Materials Journal Issue: 14 Vol. 32; ISSN 0897-4756

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Mapping Competitive Reduction upon Charging in LiNi0.8Co0.15Al0.05O2 Primary Particles

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Mapping Competitive Reduction upon Charging in LiNi_0.8Co_0.15Al_0.05O₂ Primary Particles