<p>Activation of surface lattice oxygen and chemisorbed oxygen on catalyst surfaces constitutes a pivotal step in heterogeneous oxidative catalysis. Herein, we report a strategy for enhancing oxygen activation by rational design of catalysts with single-atom promoters. Single-site Zr species in CeO<sub>2</sub> (Zr<sub>1</sub>-CeO<sub>2</sub>) are synthesized using the atom-trapping method. The Zr<sub>1</sub>-CeO<sub>2</sub>-supported Pt catalyst exhibits enhanced catalytic performance over the CeO<sub>2</sub>-supported Pt catalyst in the oxidation of CO, C<sub>3</sub>H<sub>8</sub>, and C<sub>3</sub>H<sub>6</sub>, achieving significantly lower T<sub>50</sub> values (temperature required to reach 50% conversion). This enhanced catalytic activity is attributed to the formation of an asymmetric Zr<sub>1</sub>-O-Pt<sub>1</sub> structure, which favors the activation of the adjacent surface lattice oxygen and chemisorbed molecular oxygen. This work exemplifies that incorporating single-site atoms into oxide support facilitates oxygen activation, providing new insights into the role of atomically dispersed promoters in heterogeneous catalysis.</p>

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Single-atom Zr promoter boosts oxygen activation on ceria-supported Pt catalysts

  • Weixin Huang,
  • Hao Xu,
  • Yang Deng,
  • Shih-Wei Lin,
  • Hien N. Pham,
  • Rui Zhang,
  • Dong Jiang,
  • Zihao Zhang,
  • Andrew DeLaRiva,
  • Shuxuan Feng,
  • Yixiao Li,
  • Xinrui Zhang,
  • Abhaya K. Datye,
  • Chih-Jung Chen,
  • Yong Wang

摘要

Activation of surface lattice oxygen and chemisorbed oxygen on catalyst surfaces constitutes a pivotal step in heterogeneous oxidative catalysis. Herein, we report a strategy for enhancing oxygen activation by rational design of catalysts with single-atom promoters. Single-site Zr species in CeO2 (Zr1-CeO2) are synthesized using the atom-trapping method. The Zr1-CeO2-supported Pt catalyst exhibits enhanced catalytic performance over the CeO2-supported Pt catalyst in the oxidation of CO, C3H8, and C3H6, achieving significantly lower T50 values (temperature required to reach 50% conversion). This enhanced catalytic activity is attributed to the formation of an asymmetric Zr1-O-Pt1 structure, which favors the activation of the adjacent surface lattice oxygen and chemisorbed molecular oxygen. This work exemplifies that incorporating single-site atoms into oxide support facilitates oxygen activation, providing new insights into the role of atomically dispersed promoters in heterogeneous catalysis.