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Title: Visualizing redox orbitals and their potentials in advanced lithium-ion battery materials using high-resolution x-ray Compton scattering

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. In this study, 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 (LiFePO 4 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.
Authors:
 [1] ; ORCiD logo [2] ;  [1] ; ORCiD logo [3] ; ORCiD logo [4] ;  [5] ;  [6] ;  [7] ; ORCiD logo [2] ; ORCiD logo [7] ;  [6] ; ORCiD logo [2] ;  [1]
  1. Northeastern Univ., Boston, MA (United States). Dept. of Physics
  2. Gunma Univ. (Japan). Faculty of Science and Technology
  3. Ritsumeikan Univ., Shiga (Japan). Dept. of Applied Chemisty
  4. Univ. of Antwerp (Belgium). Dept. of Physics
  5. Northeastern Univ., Boston, MA (United States). Dept. of Physics; AGH - Univ. of Science and Technology, Krakow (Poland). Faculty of Physics and Applied Computer Science
  6. Japan Synchrotron Radiation Research Inst. (SPring-8), Hyogo (Japan)
  7. Kyoto Univ. (Japan). Graduate School of Human and Environmental Studies
Publication Date:
Grant/Contract Number:
FG02-07ER46352; AC02-05CH11231; 24750065; 15K17873
Type:
Accepted Manuscript
Journal Name:
Science Advances
Additional Journal Information:
Journal Volume: 3; Journal Issue: 8; Journal ID: ISSN 2375-2548
Publisher:
AAAS
Research Org:
Northeastern Univ., Boston, MA (United States); Energy Frontier Research Centers (EFRC) (United States). Center for the Computational Design of Functional Layered Materials (CCDM)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC); Japan Science and Technology Agency (JST), Saitama (Japan); Ministry of Education, Culture, Sports, Science and Technology (MEXT) (Japan); Research Foundation-Flanders, Brussels (Belgium)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 25 ENERGY STORAGE; 36 MATERIALS SCIENCE
OSTI Identifier:
1423571