Resolving Chemical and Spatial Heterogeneities at Complex Electrochemical Interfaces in Li-Ion Batteries
Abstract
The high specific capacities of Ni-rich transition metal oxides have garnered immense interest for improving the energy density of Li-ion batteries (LIBs). Despite the potential of these materials, Ni-rich cathodes suffer from interfacial instabilities that lead to crystallographic rearrangement of the active material surface as well as the formation of a cathode electrolyte interphase (CEI) layer on the composite during electrochemical cycling. While changes in crystallographic structure can be detected with diffraction-based methods, probing the chemistry of the disordered, heterogeneous CEI layer is challenging. In this work, we use a combination of ex situ solid-state nuclear magnetic resonance (SSNMR) spectroscopy and X-ray photoemission electron microscopy (XPEEM) to provide chemical and spatial information, on the nanometer length scale, on the CEI deposited on LiNi0.8Mn0.1Co0.1O2 (NMC811) composite cathode films. XPEEM elemental maps offer insight into the lateral arrangement of the electrolyte decomposition products that comprise the CEI and paramagnetic interactions (assessed with electron paramagnetic resonance (EPR) and relaxation measurements) in 13C SSNMR provide information on the radial arrangement of the CEI from the NMC811 particles outward. Using this approach, here we find that LiF, Li2CO3, and carboxy-containing structures are directly appended to NMC811 active particles, whereas soluble species detected during in situmore »
- Authors:
-
[2];
[1]
- Columbia Univ., New York, NY (United States)
- Brookhaven National Lab. (BNL), Upton, NY (United States)
- Publication Date:
- Research Org.:
- Brookhaven National Lab. (BNL), Upton, NY (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)
- OSTI Identifier:
- 1841112
- Report Number(s):
- BNL-222610-2022-JAAM
Journal ID: ISSN 0897-4756
- Grant/Contract Number:
- SC0012704; CBET-2045262; 2021278071
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Chemistry of Materials
- Additional Journal Information:
- Journal Volume: 34; Journal Issue: 1; Journal ID: ISSN 0897-4756
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; Composites; Electrodes; Electron paramagnetic resonance spectroscopy; Nuclear magnetic resonance spectroscopy; Electrolytes
Citation Formats
Hestenes, Julia C., May, Richard, Sadowski, Jerzy T., Munich, Naiara, and Marbella, Lauren E. Resolving Chemical and Spatial Heterogeneities at Complex Electrochemical Interfaces in Li-Ion Batteries. United States: N. p., 2021.
Web. doi:10.1021/acs.chemmater.1c03185.
Hestenes, Julia C., May, Richard, Sadowski, Jerzy T., Munich, Naiara, & Marbella, Lauren E. Resolving Chemical and Spatial Heterogeneities at Complex Electrochemical Interfaces in Li-Ion Batteries. United States. https://doi.org/10.1021/acs.chemmater.1c03185
Hestenes, Julia C., May, Richard, Sadowski, Jerzy T., Munich, Naiara, and Marbella, Lauren E. Tue .
"Resolving Chemical and Spatial Heterogeneities at Complex Electrochemical Interfaces in Li-Ion Batteries". United States. https://doi.org/10.1021/acs.chemmater.1c03185. https://www.osti.gov/servlets/purl/1841112.
@article{osti_1841112,
title = {Resolving Chemical and Spatial Heterogeneities at Complex Electrochemical Interfaces in Li-Ion Batteries},
author = {Hestenes, Julia C. and May, Richard and Sadowski, Jerzy T. and Munich, Naiara and Marbella, Lauren E.},
abstractNote = {The high specific capacities of Ni-rich transition metal oxides have garnered immense interest for improving the energy density of Li-ion batteries (LIBs). Despite the potential of these materials, Ni-rich cathodes suffer from interfacial instabilities that lead to crystallographic rearrangement of the active material surface as well as the formation of a cathode electrolyte interphase (CEI) layer on the composite during electrochemical cycling. While changes in crystallographic structure can be detected with diffraction-based methods, probing the chemistry of the disordered, heterogeneous CEI layer is challenging. In this work, we use a combination of ex situ solid-state nuclear magnetic resonance (SSNMR) spectroscopy and X-ray photoemission electron microscopy (XPEEM) to provide chemical and spatial information, on the nanometer length scale, on the CEI deposited on LiNi0.8Mn0.1Co0.1O2 (NMC811) composite cathode films. XPEEM elemental maps offer insight into the lateral arrangement of the electrolyte decomposition products that comprise the CEI and paramagnetic interactions (assessed with electron paramagnetic resonance (EPR) and relaxation measurements) in 13C SSNMR provide information on the radial arrangement of the CEI from the NMC811 particles outward. Using this approach, here we find that LiF, Li2CO3, and carboxy-containing structures are directly appended to NMC811 active particles, whereas soluble species detected during in situ 1H and 19F solution NMR experiments (e.g., alkyl carbonates, HF, and vinyl compounds) are randomly deposited on the composite surface. We show that the combined approach of ex situ SSNMR and XPEEM, in conjunction with in situ solution NMR, allows spatially-resolved, molecular-level characterization of paramagnetic surfaces and new insights into electrolyte oxidation mechanisms in porous electrode films.},
doi = {10.1021/acs.chemmater.1c03185},
journal = {Chemistry of Materials},
number = 1,
volume = 34,
place = {United States},
year = {Tue Dec 28 00:00:00 EST 2021},
month = {Tue Dec 28 00:00:00 EST 2021}
}
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