Jan Höcker, Tevfik Onur Mentes, Alessandro Sala, Andrea Locatelli, Thomas Schmidt, Jens Falta, Sanjaya D. Senanayake and Jan Ingo Flege.
Advanced Materials Interfaces (2015) 2, 1500314.
The interaction of molecular hydrogen with ceria is of important relevance for heterogeneous catalysis related to green chemistry and renewable energy. Here, the complex structural transformations of a well-defined cerium oxide model catalyst are followed in situ and in real time when exposed to a reactive H2 environment. By using electron spectromicroscopy and diffraction with chemical and structural sensitivities, it is demonstrated that the transition from CeO2 to crystalline Ce2O3 occurs through a mixture of transient, coexisting phases on the nanoscale. The findings establish a clear relationship between structure and functionality for hydrogen dissociation over ceria(111), bearing profound implications on the nature of the reduction (Ce4+ → Ce3+) and mechanism for H2 scission.