| Autor: |
Zhao, An, Liu, Qing-Yu, Li, Zi-Yu, Li, Xiao-Na, He, Sheng-Gui |
| Předmět: |
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| Zdroj: |
Dalton Transactions: An International Journal of Inorganic Chemistry; 5/21/2024, Vol. 53 Issue 19, p8347-8355, 9p |
| Abstrakt: |
A fundamental understanding of the exact structural characteristics and reaction mechanisms of interface active sites is vital to engineering an energetic metal–support boundary in heterogeneous catalysis. Herein, benefiting from a newly developed high-temperature ion trap reactor, the reverse water–gas shift (RWGS) (CO2 + H2 → CO + H2O) catalyzed by a series of compositionally and structurally well-defined RhnVO3,4− (n = 3–7) clusters were identified under variable temperatures (298–773 K). It is discovered that the Rh5–7VO3,4− clusters can function more effectively to drive RWGS at relatively low temperatures. The experimentally observed size-dependent catalytic behavior was rationalized by quantum-chemical calculations; the framework of RhnVO3,4− is constructed by depositing the Rhn clusters on the VO3,4 "support", and a sandwiched base–acid–base [Rhout−–Rhin+–VO3,4−; Rhout and Rhin represent the outer and inner Rh atoms, respectively] feature in Rh5–7VO3,4− governs the adsorption and activation of reactants as well as the facile desorption of the products. In contrast, isolated Rh5–7− clusters without the electronic modification of the VO3,4 "support" can only catalyze RWGS under relatively high-temperature conditions. [ABSTRACT FROM AUTHOR] |
| Databáze: |
Complementary Index |
| Externí odkaz: |
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