Visualizing Formation of Intermetallic PdZn in a Palladium/Zinc Oxide Catalyst: Interfacial Fertilization by PdHx

Abstract Controllable synthesis of well‐defined supported intermetallic catalysts is desirable because of their unique properties in physical chemistry. To accurately pinpoint the evolution of such materials at an atomic‐scale, especially clarification of the initial state under a particular chemical environment, will facilitate rational design and optimal synthesis of such catalysts. The dynamic formation of a ZnO‐supported PdZn catalyst is presented, whereby detailed analyses of in situ transmission electron microscopy, electron energy‐loss spectroscopy, and in situ X‐ray diffraction are combined to form a nanoscale understanding of PdZn phase transitions under realistic catalytic conditions. Remarkably, introduction of atoms (H and Zn in sequence) into the Pd matrix was initially observed. The resultant PdH x is an intermediate phase in the intermetallic formation process. The evolution of PdH x in the PdZn catalyst initializes at the PdH x /ZnO interfaces, and proceeds along the PdH x ⟨111⟩ direction.