Reverse water-gas shift catalyzed by RhnVO3,4 (n = 3-7) cluster anions under variable temperatures

An Zhao, Qing Yu Liu, Zi Yu Li, Xiao Na Li*, Sheng Gui He*

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

Abstract

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.

Original languageEnglish
JournalDalton Transactions
DOIs
Publication statusAccepted/In press - 2024

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