LAUSR

Abstract Heterogeneous catalysts are often complex materials containing different compounds. While this can lead to highly beneficial interfaces, it is difficult to identify the role of single components. In methanol steam reforming (MSR), the interplay between intermetallic compounds, supporting oxides and redox reactions leads to highly active and CO2‐selective materials. Herein, the intrinsic catalytic properties of unsupported In3Pt2, In2Pt, and In7Pt3 as model systems for Pt/In2O3‐based catalytic materials in MSR are addressed. In2Pt was identified as the essential compound responsible for the reported excellent CO2‐selectivity of 99.5 % at 300 °C in supported systems, showing a CO2‐selectivity above 99 % even at 400 °C. Additionally, the partial oxidation of In7Pt3 revealed that too much In2O3 is detrimental for the catalytic properties. The study highlights the crucial role of intermetallic In−Pt compounds in Pt/In2O3 materials with excellent CO2‐selectivity.