Identifying Redox Orbitals and Defects in Lithium-Ion Cathodes with Compton Scattering and Positron Annihilation Spectroscopies

Identifying Redox Orbitals and Defects in Lithium-Ion Cathodes with Compton Scattering and Positron Annihilation Spectroscopies: A Review

Nokelainen, Johannes (LUT University; Northeastern University)
Barbiellini, Bernardo (LUT University; Northeastern University)
Kuriplach, Jan (Charles University)
Eijt, S.W.H. (TU Delft RST/Fundamental Aspects of Materials and Energy)
Ferragut, Rafael (Politecnico di Milano)
Li, Xin (LUT University; Politecnico di Milano)
Kothalawala, Veenavee (LUT University)
Suzuki, Kosuke (Gunma University)
Hafiz, Hasnain (Carnegie Mellon University)
Bansil, Arun (Northeastern University)

2022

Reduction-oxidation (redox) reactions that transfer conduction electrons from the anode to the cathode are the fundamental processes responsible for generating power in Li-ion batteries. Electronic and microstructural features of the cathode material are controlled by the nature of the redox orbitals and how they respond to Li intercalation. Thus, redox orbitals play a key role in performance of the battery and its degradation with cycling. We unravel spectroscopic descriptors that can be used to gain an atomic-scale handle on the redox mechanisms underlying Li-ion batteries. Our focus is on X-ray Compton Scattering and Positron Annihilation spectroscopies and the related computational approaches for the purpose of identifying orbitals involved in electrochemical transformations in the cathode. This review provides insight into the workings of lithium-ion batteries and opens a pathway for rational design of next-generation battery materials.

cathode materials
density functional theory
first principles calculations
Li-ion battery
positron annihilation spectroscopy
redox orbitals
X-ray compton scattering

http://resolver.tudelft.nl/uuid:7cac8dec-92e0-4476-ad32-3874bb227c09

https://doi.org/10.3390/condmat7030047

Condensed Matter, 7 (3)

Institutional Repository

review

© 2022 Johannes Nokelainen, Bernardo Barbiellini, Jan Kuriplach, S.W.H. Eijt, Rafael Ferragut, Xin Li, Veenavee Kothalawala, Kosuke Suzuki, Hasnain Hafiz, Arun Bansil, More Authors