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Rhodium Encapsulated within Silicalite‐1 Zeolite as Highly Efficient Catalyst for Nitrous Oxide Decomposition: From Single Atoms to Nanoclusters and Nanoparticles
Author(s) -
Wang Shiwei,
Yan Bo,
Chai Juan,
Li Tianhao,
Yu Hongbo,
Li Tong,
Cao Peng,
Yang Fan,
Yuan Xuemin,
Yin Hongfeng
Publication year - 2021
Publication title -
european journal of inorganic chemistry
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 0.667
H-Index - 136
eISSN - 1099-0682
pISSN - 1434-1948
DOI - 10.1002/ejic.202100106
Subject(s) - catalysis , chemistry , nanoclusters , rhodium , decomposition , nanoparticle , zeolite , inorganic chemistry , adsorption , metal , oxide , x ray photoelectron spectroscopy , desorption , chemical engineering , organic chemistry , engineering
The size of metal species plays a pivotal role in governing catalytic performance of supported metal catalysts. In this work, a series of Rh encapsulated within silicalite‐1 catalysts with different sizes were prepared by one‐pot hydrothermal method and employed to catalyze the decomposition of N 2 O. Detailed structure determinations by HAADF‐STEM, XPS and CO‐DRIFTS demonstrate that subtle modulation of the encapsulated Rh species were achieved easily from single‐atom to nanoclusters and nanoparticles by controlling the loading and reduction conditions of Rh. The turnover frequency (TOF) of N 2 O decomposition showed a typical volcano‐type dependence on Rh size. Kinetic studies revealed that this structure‐sensitive catalysis was related to the difference in N 2 O and O 2 adsorption/desorption for various Rh species. Furthermore, a Rh@S‐1 catalyst with a proper Rh size (ca. 1.6 nm) was identified as the best‐performing catalyst with a maximum TOF (ca. 95 h −1 ), showing much superior activity than other reported Rh‐based catalysts.