Formation and impact of nanoscopic oriented phase domains in electrochemical crystalline electrodes

Wenxiang Chen, Xun Zhan, Renliang Yuan, Saran Pidaparthy, Adrian Xiao Bin Yong, Hyosung An, Zhichu Tang, Kaijun Yin, Arghya Patra, Heonjae Jeong, Cheng Zhang, Kim Ta, Zachary W. Riedel, Ryan M. Stephens, Daniel P. Shoemaker, Hong Yang, Andrew A. Gewirth, Paul V. Braun, Elif Ertekin, Jian Min ZuoQian Chen

Research output: Contribution to journalArticlepeer-review


Electrochemical phase transformation in ion-insertion crystalline electrodes is accompanied by compositional and structural changes, including the microstructural development of oriented phase domains. Previous studies have identified prevailingly transformation heterogeneities associated with diffusion- or reaction-limited mechanisms. In comparison, transformation-induced domains and their microstructure resulting from the loss of symmetry elements remain unexplored, despite their general importance in alloys and ceramics. Here, we map the formation of oriented phase domains and the development of strain gradient quantitatively during the electrochemical ion-insertion process. A collocated four-dimensional scanning transmission electron microscopy and electron energy loss spectroscopy approach, coupled with data mining, enables the study. Results show that in our model system of cubic spinel MnO2 nanoparticles their phase transformation upon Mg2+ insertion leads to the formation of domains of similar chemical identity but different orientations at nanometre length scale, following the nucleation, growth and coalescence process. Electrolytes have a substantial impact on the transformation microstructure (‘island’ versus ‘archipelago’). Further, large strain gradients build up from the development of phase domains across their boundaries with high impact on the chemical diffusion coefficient by a factor of ten or more. Our findings thus provide critical insights into the microstructure formation mechanism and its impact on the ion-insertion process, suggesting new rules of transformation structure control for energy storage materials.

Original languageEnglish (US)
Pages (from-to)92-99
Number of pages8
JournalNature Materials
Issue number1
StatePublished - Jan 2023

ASJC Scopus subject areas

  • General Chemistry
  • General Materials Science
  • Condensed Matter Physics
  • Mechanics of Materials
  • Mechanical Engineering


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