TY - JOUR
T1 - Solvent-Free Synthesis Enables Encapsulation of Subnanometric FeOx Clusters in Pure Siliceous Zeolites for Efficient Catalytic Oxidation Reactions
AU - Ye, Jiajie
AU - Tang, Xuan
AU - Cheng, Lu
AU - Zhang, Shoujie
AU - Zhan, Wangcheng
AU - Guo, Yanglong
AU - Wang, Li
AU - Cao, Xiao Ming
AU - Wang, Kuan Wen
AU - Dai, Sheng
AU - Guo, Yun
N1 - Publisher Copyright:
© 2024 American Chemical Society. All rights reserved.
PY - 2024/5/15
Y1 - 2024/5/15
N2 - Metal/metal oxide clusters possess a higher count of unsaturated coordination sites than nanoparticles, providing multiatomic sites that single atoms do not. Encapsulating metal/ metal oxide clusters within zeolites is a promising approach for synthesizing and stabilizing these clusters. The unique feature endows the metal clusters with an exceptional catalytic performance in a broad range of catalytic reactions. However, the encapsulation of stable FeOx clusters in zeolite is still challenging, which limits the application of zeolite-encapsulated FeOx clusters in catalysis. Herein, we design a modified solvent-free method to encapsulate FeOx clusters in pure siliceous MFI zeolites (Fe@MFI). It is revealed that the 0.3−0.4 nm subnanometric FeOx clusters are stably encapsulated in the 5/6-membered rings intersectional voids of the pure siliceous MFI zeolites. The encapsulated Fe@MFI catalyst with a Fe loading of 1.4 wt % demonstrates remarkable catalytic activity and recycle stability in the direct oxidation of methane, while also promoting the direct oxidation of cyclohexane, surpassing the performance of conventional zeolite-supported Fe catalysts.
AB - Metal/metal oxide clusters possess a higher count of unsaturated coordination sites than nanoparticles, providing multiatomic sites that single atoms do not. Encapsulating metal/ metal oxide clusters within zeolites is a promising approach for synthesizing and stabilizing these clusters. The unique feature endows the metal clusters with an exceptional catalytic performance in a broad range of catalytic reactions. However, the encapsulation of stable FeOx clusters in zeolite is still challenging, which limits the application of zeolite-encapsulated FeOx clusters in catalysis. Herein, we design a modified solvent-free method to encapsulate FeOx clusters in pure siliceous MFI zeolites (Fe@MFI). It is revealed that the 0.3−0.4 nm subnanometric FeOx clusters are stably encapsulated in the 5/6-membered rings intersectional voids of the pure siliceous MFI zeolites. The encapsulated Fe@MFI catalyst with a Fe loading of 1.4 wt % demonstrates remarkable catalytic activity and recycle stability in the direct oxidation of methane, while also promoting the direct oxidation of cyclohexane, surpassing the performance of conventional zeolite-supported Fe catalysts.
KW - FeO cluster
KW - confinement synthesis
KW - direct oxidation of methane
KW - pure siliceous zeolite
KW - solvent-free synthesis
UR - http://www.scopus.com/inward/record.url?scp=85192231420&partnerID=8YFLogxK
U2 - 10.1021/acsami.4c03083
DO - 10.1021/acsami.4c03083
M3 - Article
AN - SCOPUS:85192231420
SN - 1944-8244
VL - 16
SP - 24691
EP - 24702
JO - ACS Applied Materials and Interfaces
JF - ACS Applied Materials and Interfaces
IS - 19
ER -