Visualizing redox orbitals and their potentials in advanced lithium-ion battery materials using high-resolution x-ray Compton scattering.
Hasnain HafizKosuke SuzukiBernardo BarbielliniYuki OrikasaVincent CallewaertStaszek KaprzykMasayoshi ItouKentaro YamamotoRyota YamadaYoshiharu UchimotoYoshiharu SakuraiHiroshi SakuraiArun BansilPublished in: Science advances (2017)
Reduction-oxidation (redox) reactions are the key processes that underlie the batteries powering smartphones, laptops, and electric cars. A redox process involves transfer of electrons between two species. For example, in a lithium-ion battery, current is generated when conduction electrons from the lithium anode are transferred to the redox orbitals of the cathode material. The ability to visualize or image the redox orbitals and how these orbitals evolve under lithiation and delithiation processes is thus of great fundamental and practical interest for understanding the workings of battery materials. We show that inelastic scattering spectroscopy using high-energy x-ray photons (Compton scattering) can yield faithful momentum space images of the redox orbitals by considering lithium iron phosphate (LiFePO4 or LFP) as an exemplar cathode battery material. Our analysis reveals a new link between voltage and the localization of transition metal 3d orbitals and provides insight into the puzzling mechanism of potential shift and how it is connected to the modification of the bond between the transition metal and oxygen atoms. Our study thus opens a novel spectroscopic pathway for improving the performance of battery materials.
Keyphrases
- solid state
- density functional theory
- transition metal
- high resolution
- electron transfer
- molecular dynamics
- deep learning
- ion batteries
- reduced graphene oxide
- mass spectrometry
- molecular docking
- magnetic resonance
- nitric oxide
- optical coherence tomography
- molecular dynamics simulations
- genetic diversity
- climate change