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Simultaneous Ni Doping at Atom Scale in Ceria and Assembling into Well-Defined Lotuslike Structure for Enhanced Catalytic Performance

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Authors

  • Qingqing Li
  • Zhen Huang
  • Pengfei Guan
  • Rui Su
  • Qi Cao
  • Yimin Chao
  • Wei Shen
  • Junjie Guo
  • Hualong Xu
  • Renchao Che

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Abstract

Oxide materials with redox capability have attracted worldwide attentions in many applications. Introducing defects into crystal lattice is an effective method to modify and optimize redox capability of oxides as well as their catalytic performance. However, the relationship between intrinsic characteristics of defects and properties of oxides has been rarely reported. Herein, we report a facile strategy to introduce defects by doping a small amount of Ni atoms (∼1.8 at. %) into ceria lattice at atomic level through the effect of microstructure of crystal on the redox property of ceria. Amazingly, a small amount of single Ni atom-doped ceria has formed a homogeneous solid solution with uniform lotuslike morphology. It performs an outstanding catalytic performance of a reduced T50 of CO oxidation at 230 °C, which is 135 °C lower than that of pure CeO2 (365 °C). This is largely attributed to defects such as lattice distortion, crystal defects and elastic strain induced by Ni dopants. The DFT calculation has revealed that the electron density distribution of oxygen ions near Ni dopant, the reduced formation energy of oxygen vacancy originated from local chemical effect caused by local distortion after Ni doping. These differences have a great effect on increasing the concentration of oxygen vacancies and enhancing the migration of lattice oxygen from bulk to a surface which is closely related to optimized redox properties. As a result, oxygen storage capacity and the associated catalytic reactivity has been largely increased. We have clearly demonstrated the change of crystal lattice and the charge distribution effectively modify its chemical and physical properties at the atomic scale.

Details

Original languageEnglish
Pages (from-to)16243-16251
JournalACS Applied Materials & Interfaces
Volume9
Issue number19
Early online date26 Apr 2017
DOIs
Publication statusPublished - 17 May 2017
Peer-reviewedYes

Keywords

    Research areas

  • atomic level doping, cerium oxide, CO oxidation, oxygen vacancy, solid solution

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