Single-Phase Formation of Rh2 O3 Nanoparticles on h-BN Support for Highly Controlled Methane Partial Oxidation to Syngas

Angew Chem Int Ed Engl. 2021 Nov 22;60(48):25411-25418. doi: 10.1002/anie.202110292. Epub 2021 Oct 21.

Abstract

Single-phase formation of active metal oxides on supports has been vigorously pursued in many catalytic applications to suppress undesired reactions and to determine direct structure-property relationships. However, this is difficult to achieve in nanoscale range because the effect of non-uniform metal-support interfaces becomes dominant in the overall catalyst growth, leading to the nucleation of various metastable oxides. Herein, we develop a supported single-phase corundum-Rh2 O3 (I) nanocatalyst by utilizing controlled interaction between metal oxide and h-BN support. Atomic-resolution electron microscopy and first-principle calculation reveal that single-phase formation occurs via uniform and preferential attachment of Rh2 O3 (I) (110) seed planes on well-defined h-BN surface after decomposition of rhodium precursor. By utilizing the Rh/h-BN catalyst in methane partial oxidation, syngas is successfully produced solely following the direct route with keeping a H2 /CO ratio of 2, which makes it ideal for most downstream chemical processes.

Keywords: heterogeneous catalysis; hexagonal boron nitride; methane; rhodium oxide; syngas.