Stretched Pd-CoOx Interfaces-Induced Oxygen Vacancy Consecutive Activation Realizes Light Alkane Efficacious Destruction

  • Lianghui Xia
  • , Yujie Liu
  • , Kang Hui Lim
  • , Qiyuan Liu
  • , Meizan Jing*
  • , Yanfei Jian
  • , Jingjing Wang
  • , He Xu
  • , Mudi Ma*
  • , Shouning Chai
  • , Reem Albilali
  • , Chi He*
  • *Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

1 Scopus citations

Abstract

The introduction of oxygen vacancies (Ov) into catalyst structures has proven to be an effective strategy for enhancing their activity. To maintain their catalytic performance, however, the efficacious replenishing of the continuously depleted Ov during reactions is pivotal and still a great challenge. To address this, a Pd-CoOx/CeO2 catalyst (Pd-Ens) with highly exposed Pd-CoOx interfaces was rationally crafted, over which remarkable propane degradation activity, stability, and SO2 resistance can be obtained owing to high Pd2+ ratio and significant Ov content. The exposed Pd-CoOx interfaces stretched the lattice of Pd-Ens catalyst, which boosts the redox capacity and charge transfer ability, facilitating the activation of lattice oxygen (Olat) for Ov generation and subsequently stabilizing the Pd species. Continuous Olat activation and abundant Ov promote the adsorption and activation of propane and oxygen over Pd-Ens, accelerating the formation of the acetone intermediate while expediting subsequent deep oxidation. Moreover, the adsorption of SO2 impurity is well limited over Pd-Ens surface attributing to the existence of Pd-CoOx interfaces. In comparison, the Pd-Sup2 counterpart with internal PdO/Co3O4 interfaces exhibits inferior propane catalytic performance and SO2 resistance due to the irreversible Ov depletion, extensive Pd species oxidation, and strong SO2 adsorption. Besides, the weak mineralization ability makes Pd-Sup2 yield more harmful byproducts. These findings offer crucial guidance for developing efficient and practicable catalysts for light alkane degradation as well as other heterogeneous oxidation reactions.

Original languageEnglish
Pages (from-to)1226-1241
Number of pages16
JournalACS ES and T Engineering
Volume5
Issue number5
DOIs
StatePublished - 9 May 2025

Keywords

  • activation mechanism
  • exposed Pd-CoO interfaces
  • lattice oxygen activation
  • light alkane oxidation
  • oxygen vacancy generation

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