In situ spectroscopy-guided engineering of rhodium single-atom catalysts for CO oxidation.

ABSTRACT: Single-atom catalysts have recently been applied in many applications such as CO oxidation. Experimental in situ investigations into this reaction, however, are limited. Hereby, we present a suite of operando/in situ spectroscopic experiments for structurally well-defined atomically dispersed Rh on phosphotungstic acid during CO oxidation. The identification of several key intermediates and the steady-state catalyst structure indicate that the reactions follow an unconventional Mars-van Krevelen mechanism and that the activation of O₂ is rate-limiting. In situ XPS confirms the contribution of the heteropoly acid support while in situ DRIFT spectroscopy consolidates the oxidation state and CO adsorption of Rh. As such, direct observation of three key components, i.e., metal cente

SUBMITTER: Hulsey MJ 

PROVIDER: S-EPMC6430772 | biostudies-literature | 2019 Mar

REPOSITORIES: biostudies-literature