Visualizing Formation of Intermetallic PdZn in a Palladium/Zinc Oxide Catalyst: Interfacial Fertilization by PdH_<i>x</i>

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.