<p>Self-assembled metal nanoparticles exsolved from host oxides have gained prominence in catalysis and electrochemistry owing to their exceptional activity and stability. Understanding the relation between dopant transport and exsolution is important, as the transport mechanism of dopants toward the surface of the host oxide directly influences exsolution sites, density, and dispersion, ultimately determining catalytic functionality. However, the pathways for dopant transport and their interactions with internal defects during exsolution remain unclear due to the complexity of defects hidden in the bulk. Here, we reveal the exsolution pathway mediated by dislocation evolution within a host oxide perovskite. By employing in situ Bragg coherent X-ray diffraction imaging and transmission electron microscopy, we show that dislocations nucleate in the bulk interior and propagate to the surface during the reduction of Ru-doped BaCe<sub>0.85</sub>Y<sub>0.1</sub>Ru<sub>0.05</sub>O<sub>3-δ</sub>. Moreover, we verify that the Ru dopant is specifically correlated with the formation of mixed dislocations, which act as mobile vehicles that dynamically carry Ru defects to the surface in tandem with dislocation propagation. These findings advance our understanding of dislocation dynamics and support the development of exsolved metal nanoparticles for next-generation catalysts.</p>

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Dynamics of dislocation formations and their impacts on exsolution in Ru-doped perovskite oxide

  • Sungwook Choi,
  • Younghwan Lim,
  • Puspendu Guha,
  • Hayoung Kim,
  • Jaeseung Kim,
  • Sungwon Kim,
  • Ross Harder,
  • Wonsuk Cha,
  • Hoyoung Suh,
  • Jinseok Ryu,
  • Sungeun Yang,
  • Ho-Il Ji,
  • Deok-Hwang Kwon,
  • Hyunjung Kim

摘要

Self-assembled metal nanoparticles exsolved from host oxides have gained prominence in catalysis and electrochemistry owing to their exceptional activity and stability. Understanding the relation between dopant transport and exsolution is important, as the transport mechanism of dopants toward the surface of the host oxide directly influences exsolution sites, density, and dispersion, ultimately determining catalytic functionality. However, the pathways for dopant transport and their interactions with internal defects during exsolution remain unclear due to the complexity of defects hidden in the bulk. Here, we reveal the exsolution pathway mediated by dislocation evolution within a host oxide perovskite. By employing in situ Bragg coherent X-ray diffraction imaging and transmission electron microscopy, we show that dislocations nucleate in the bulk interior and propagate to the surface during the reduction of Ru-doped BaCe0.85Y0.1Ru0.05O3-δ. Moreover, we verify that the Ru dopant is specifically correlated with the formation of mixed dislocations, which act as mobile vehicles that dynamically carry Ru defects to the surface in tandem with dislocation propagation. These findings advance our understanding of dislocation dynamics and support the development of exsolved metal nanoparticles for next-generation catalysts.