Decoding Oxygen K-edge Fingerprints of NCM-811 Degradation via Ab Initio Many-Body Theory and High-Throughput Screening of Crystal Proxies
Abstract
The degradation of LiNi0.8Co0.1Mn0.1O2 (NCM-811) in Li-ion batteries produces complex transition-metal oxides and binary phases that fundamentally limit cathode performance. While identifying these degradation products via X-ray absorption spectroscopy (XAS) is essential for mitigating electrochemical performance loss, interpretation remains challenging due to the structural complexity of real-world samples. In this work, we present an integrated theoretical-experimental framework combining high-resolution oxygen K-edge XAS with \textit{ab initio} simulations based on many-body perturbation theory and high-throughput screening from density functional theory. We first evaluate the spectroscopic fingerprints of eight layered, spinel, and nominal rock-salt reference oxides, identifying discrepancies between the idealized single-crystal bulk phase and experimental spectra. Using high-throughput screening to analyze the oxygen p-projected density of states of 38 distinct polymorphs of NiO, CoO, and MnO, we propose that the spectral differences can emerge, among other factors, from local structural variations represented here by simplified structural proxies. Our work establishes a viable and rigorous computational pathway to interpret the complex landscape of degraded battery materials.
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BibTeX
@misc{duarteruiz2026decoding,
title = {{Decoding Oxygen K-edge Fingerprints of NCM-811 Degradation via Ab Initio Many-Body Theory and High-Throughput Screening of Crystal Proxies}},
author = {Daniel Duarte-Ruiz and Timo Reents and Elmar Kataev and Raul Garcia-Diez and Regan G. Wilks and Marcus Baer and Caterina Cocchi},
howpublished = {arXiv},
year = {2026},
month = oct,
doi = {10.48550/arxiv.2609.02206},
eprint = {2609.02206},
archivePrefix = {arXiv},
url = {https://arxiv.org/abs/2609.02206},
}
RIS
TY - UNPB
TI - Decoding Oxygen K-edge Fingerprints of NCM-811 Degradation via Ab Initio Many-Body Theory and High-Throughput Screening of Crystal Proxies
AU - Daniel Duarte-Ruiz
AU - Timo Reents
AU - Elmar Kataev
AU - Raul Garcia-Diez
AU - Regan G. Wilks
AU - Marcus Baer
AU - Caterina Cocchi
PY - 2026
DA - 2026/10/27
PB - arXiv
DO - 10.48550/arxiv.2609.02206
UR - https://arxiv.org/abs/2609.02206
AB - The degradation of LiNi_0.8Co_0.1Mn_0.1O_2 (NCM-811) in Li-ion batteries produces complex transition-metal oxides and binary phases that fundamentally limit cathode performance. While identifying these degradation products via X-ray absorption spectroscopy (XAS) is essential for mitigating electrochemical performance loss, interpretation remains challenging due to the structural complexity of real-world samples. In this work, we present an integrated theoretical-experimental framework combining high-resolution oxygen K-edge XAS with \textit{ab initio} simulations based on many-body perturbation theory and high-throughput screening from density functional theory. We first evaluate the spectroscopic fingerprints of eight layered, spinel, and nominal rock-salt reference oxides, identifying discrepancies between the idealized single-crystal bulk phase and experimental spectra. Using high-throughput screening to analyze the oxygen p-projected density of states of 38 distinct polymorphs of NiO, CoO, and MnO, we propose that the spectral differences can emerge, among other factors, from local structural variations represented here by simplified structural proxies. Our work establishes a viable and rigorous computational pathway to interpret the complex landscape of degraded battery materials.
ER -