Hydrogen storage
in the form of small molecules and subsequent
release are foreseen to play a fundamental role in future energy systems
or carbon cycles. Methanol is an ideal hydrogen carrier due to the
high H/C ratio, the lack of C–C bonds, and being liquid under
ambient conditions. Methanol steam reforming is an advantageous reaction
for the release of the chemically bound hydrogen. Pd- or Pt-based
intermetallic compounds have shown to be CO2-selective
and long-term stable catalytic materials. However, an intrinsic understanding
of the underlying processes is still lacking. In this study, we show
that the redox activity in the In–Pt system can be steered
by gas-phase changes and leads to highly active catalytic materials
at 300 °C [1500 mol (H2)/(mol (Pt) × h)] with
an excellent CO2 selectivity of 99.5%, thus clearly outperforming
previous materials. Reactive transformations between In2Pt, In3Pt2, and In2O3 have been identified to cause the high selectivity. Redox activity
of intermetallic compounds as part of the catalytic cycle was previously
unknown and adds an understanding to the concept of different adsorption
sites.