Rhodium Encapsulated within Silicalite‐1 Zeolite as Highly Efficient Catalyst for Nitrous Oxide Decomposition: From Single Atoms to Nanoclusters and Nanoparticles
Shiwei Wang, Bo Yan, Juan Chai, Tianhao Li, Hongbo Yu, Tong Li, Peng Cao, Fan Yang, Xuemin Yuan, Hongfeng Yin
Abstract
Abstract 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.