Regulating Mono-/Binuclear Fe Species in Framework Al-Rich Zeolites for Efficient Low-Temperature Alkane Oxidation

Open AccessCCS ChemistryRESEARCH ARTICLES11 Apr 2024Regulating Mono/Binuclear Fe Species in Framework Al-Rich Zeolites for Efficient Low-Temperature Alkane Oxidation Qiang Zhang, Jialiang Li, Guangyuan He, Junyan Li, Ziyi Chen, Qing Zhang, Chunyu Wang, Guodong Qi, Qiang Wang, Peng Zhang, Jun Xu, Osamu Terasaki, Donghai Mei, Zhongmin Liu and Jihong Yu Qiang Zhang , Jialiang Li , Guangyuan He , Junyan Li , Ziyi Chen , Qing Zhang , Chunyu Wang , Guodong Qi , Qiang Wang , Peng Zhang , Jun Xu , Osamu Terasaki , Donghai Mei , Zhongmin Liu and Jihong Yu https://doi.org/10.31635/ccschem.024.202404123 SectionsSupplemental MaterialAboutPDF ToolsAdd to favoritesDownload CitationsTrack Citations ShareFacebookTwitterLinked InEmail Zeolite-encapsulated extra-framework mono/binuclear Fe3+ species present higher catalytic activities compared to clusters and nanoparticles for direct low-temperature alkane oxidation. However, the fine control of mono/binuclear Fe3+ in zeolites is challenging and the reaction mechanism of low-temperature alkane oxidation remains not clearly identified. Different from previous impregnation and ion-exchange methods generally generating clusters/nanoparticles, here we developed an efficient amino acid-assisted one-pot hydrothermal synthesis strategy for in situ incorporating mono/binuclear Fe3= species into framework Al-rich ZSM-5 zeolites. The high framework Al content (Si/Al=9) provided sufficient negatively-charged sites to anchor mono/binuclear Fe3+ (Fe loading=0.44~0.90 wt%). The as-prepared 0.44Fe@Z-L0.3H6-9 catalyst exhibited superior catalytic properties for selective oxidation of both methane and ethane in the H2O2 solution at 50 °C, presenting a top-level catalytic performance among various heterogeneous/homogeneous catalysts. Combining advanced characterizations and density functional theory calculations, the complex reaction networks for methane and ethane conversions into C1/C2 oxygenates over mononuclear and binuclear Fe3+, for the first time, were mapped out. The mononuclear Fe3+ was found more active than binuclear Fe3+ for both methane and ethane conversions. This work not only provides a whole picture on low-temperature alkane oxidation mechanisms but also guides the rational design of high-performance catalysts for C−H bond activation and beyond. Download figure Download PowerPoint Previous articleNext article FiguresReferencesRelatedDetails Issue AssignmentNot Yet AssignedSupporting Information Copyright & Permissions© 2024 Chinese Chemical Society Downloaded 0 times PDF downloadLoading ...