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An environmentally adaptive gold single-atom catalyst with variable valence states.

Meiliang Ma1, Wen Liu1, Xiaojuan Hu1

  • 1Center of Electron Microscopy, School of Materials Science and Engineering, Zhejiang University, Hangzhou, 310027, China. xiaojuanhu@zju.edu.cn.

Physical Chemistry Chemical Physics : PCCP
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Summary

Environmentally adaptive gold single-atom catalysts on CeO2 surfaces can switch oxidation states, enhancing stability and activity for CO oxidation. This adaptability is key to their high performance in sustainable catalysis.

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Area of Science:

  • Catalysis
  • Materials Science
  • Surface Chemistry

Background:

  • Single-atom catalysts (SACs) offer high atomic efficiency and selectivity but their underlying mechanisms remain unclear.
  • Understanding SACs is crucial for advancing sustainable chemical processes.

Purpose of the Study:

  • To investigate the environmental adaptability and catalytic mechanisms of gold single-atom catalysts on CeO2(111).
  • To elucidate how valence state changes influence catalyst stability and activity.

Main Methods:

  • First-principles calculations were employed to model the behavior of gold single atoms on a CeO2(111) surface.
  • Simulations analyzed catalyst interactions under different gas atmospheres (CO, O2) and reaction conditions.

Main Results:

  • Gold single atoms on CeO2(111) exhibit environmentally adaptive valence states.
  • In CO, gold forms negative oxidation states due to oxygen vacancies, leading to deactivation.
  • In O2, gold oxidizes to positive states, reactivating the catalyst for CO oxidation.

Conclusions:

  • The dynamic oscillation between oxidation states is crucial for the high activity and stability of gold single-atom catalysts.
  • This study provides fundamental insights into SACs' unique properties and performance.
  • Findings pave the way for designing more efficient and robust single-atom catalysts.