Cation reordering instead of phase transitions: Origins and implications of contrasting lithiation mechanisms in 1D ζ- and 2D α-V 2 O 5

Abstract

The function of cathode materials is determined by factors transcending decades of length scales, spanning the range from the crystal structure and composition of the compound to the dimensions and morphologies of the particles, their connectivity with other particles and with the conductive matrix, and their spatial location relative to the electrolyte–electrode interface. Mitigating the constraints and degradation mechanisms that limit cathode materials from realizing their full potential requires careful consideration of the electrode structure spanning multiple length scales. In this work, we explore an intriguing concept: For the same exact composition (V 2 O 5 ), can the atomic connectivity be altered to stabilize a metastable polymorph that provides access to an entirely distinctive cation insertion and diffusion mechanism?

Document Details

Document Type
Pub Defense Publication
Publication Date
Jan 21, 2022
Source ID
10.1073/pnas.2115072119

Entities

People

  • Andrey Yakovenko
  • Bai-Xiang Xu
  • Brian J. Schultz
  • David A. Santos
  • Harry Charalambous
  • Joseph V. Handy
  • Kamila M. Wiaderek
  • Leonardo Gobbato
  • Luis Rodolfo García Carrillo
  • Matt Pharr
  • Max Pupucevski
  • Sarbajit Banerjee
  • Shahed Rezaei
  • Yuting Luo
  • Yuwei Zhang

Organizations

  • Argonne National Laboratory
  • Technical University of Darmstadt
  • Yusuf Hamied Department of Chemistry

Tags

Readers

  • Plasma Physics.
  • Quantum Chemistry
  • Systems Analysis and Design