Rational Design of Battery Materials Through Spectroscopic Characterization and Computational Modeling of Redox Orbitals

Abstract

Reduction-oxidation (redox) reactions are the key electrochemical processes at play in lithium-ion batteries (LIBs). Redox reactions are responsible for generating currents in external circuits by transferring electrons from an anode to a cathode. However, observation of redox orbitals to gain an atomic-level understanding of how they evolve under lithiation and delithiation processes has proven very challenging. In this connection, we have shown that high-energy synchrotron X-ray Compton scattering experiments combined with accurate first-principles modeling of electronic and magnetic structures of battery materials can provide atomic-scale visualization of redox orbitals in working batteries. Our analysis reveals robust spectroscopic descriptors that allow a handle on the reversibility and stability of battery materials and a new paradigm for the rational design of these materials.