TY - JOUR
T1 - Stretched Pd-CoOx Interfaces-Induced Oxygen Vacancy Consecutive Activation Realizes Light Alkane Efficacious Destruction
AU - Xia, Lianghui
AU - Liu, Yujie
AU - Lim, Kang Hui
AU - Liu, Qiyuan
AU - Jing, Meizan
AU - Jian, Yanfei
AU - Wang, Jingjing
AU - Xu, He
AU - Ma, Mudi
AU - Chai, Shouning
AU - Albilali, Reem
AU - He, Chi
N1 - Publisher Copyright:
© 2025 American Chemical Society.
PY - 2025/5/9
Y1 - 2025/5/9
N2 - 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.
AB - 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.
KW - activation mechanism
KW - exposed Pd-CoO interfaces
KW - lattice oxygen activation
KW - light alkane oxidation
KW - oxygen vacancy generation
UR - https://www.scopus.com/pages/publications/85217576483
U2 - 10.1021/acsestengg.4c00861
DO - 10.1021/acsestengg.4c00861
M3 - Article
AN - SCOPUS:85217576483
SN - 2690-0645
VL - 5
SP - 1226
EP - 1241
JO - ACS ES and T Engineering
JF - ACS ES and T Engineering
IS - 5
ER -