TY - JOUR
T1 - Construction of Electron-Enriched Ptδ+ with Reactive Oxygen Species for Enhanced Propane Catalytic Combustion
AU - Yu, Zhixin
AU - Fang, Yarong
AU - Pan, Chuanqi
AU - Ma, Shiqi
AU - Zeng, Yiqing
AU - Yang, Ji
AU - Wan, Shipeng
AU - Zhong, Zhaoxiang
N1 - Publisher Copyright:
© 2025 American Chemical Society.
PY - 2025/4/9
Y1 - 2025/4/9
N2 - The complete catalytic oxidation of propane (C3H8) at low temperatures remains challenging due to the competitive adsorption between the oxidation of the O2 and C3H8 molecules. In this study, we propose an innovative approach to enhance C3H8 oxidation by strategically designing active Ptδ+ sites with modulated electronic structures on F-doped TiO2-supported Pt catalyst (Pt/F-TiO2), which exhibits 50 and 90% of propane conversion at 200 and 320 °C. Our mechanistic study reveals that the electron coupling between Pt 5d and F 2p alters the d orbital electron property, which leads to generation of abundant efficient electron-enriched Ptδ+ species. These new Ptδ+ sites facilitate the adsorption of C3H8 and promote the activation of chemisorbed O2 into superoxide species, in the form of bridge Pt-(O−O)ad-Ti, which synergistically facilitates the methyl C−H cleavage in C3H8. This study presents the strategy for electronic structure engineering of active sites in Pt-based catalysts, paving the way for the development of high-performance catalysts for propane oxidation.
AB - The complete catalytic oxidation of propane (C3H8) at low temperatures remains challenging due to the competitive adsorption between the oxidation of the O2 and C3H8 molecules. In this study, we propose an innovative approach to enhance C3H8 oxidation by strategically designing active Ptδ+ sites with modulated electronic structures on F-doped TiO2-supported Pt catalyst (Pt/F-TiO2), which exhibits 50 and 90% of propane conversion at 200 and 320 °C. Our mechanistic study reveals that the electron coupling between Pt 5d and F 2p alters the d orbital electron property, which leads to generation of abundant efficient electron-enriched Ptδ+ species. These new Ptδ+ sites facilitate the adsorption of C3H8 and promote the activation of chemisorbed O2 into superoxide species, in the form of bridge Pt-(O−O)ad-Ti, which synergistically facilitates the methyl C−H cleavage in C3H8. This study presents the strategy for electronic structure engineering of active sites in Pt-based catalysts, paving the way for the development of high-performance catalysts for propane oxidation.
KW - competitive adsorption
KW - electron-enriched Pt
KW - methyl C−H cleavage
KW - propane catalytic oxidation
KW - reactive superoxide species
UR - http://www.scopus.com/inward/record.url?scp=105003039419&partnerID=8YFLogxK
U2 - 10.1021/acsami.5c00598
DO - 10.1021/acsami.5c00598
M3 - 文章
C2 - 40133807
AN - SCOPUS:105003039419
SN - 1944-8244
VL - 17
SP - 21246
EP - 21256
JO - ACS Applied Materials and Interfaces
JF - ACS Applied Materials and Interfaces
IS - 14
ER -