Single-Site vs. Cluster Catalysis in High Temperature Oxidations

This is the peer reviewed version of the following article "Single-Site vs. Cluster Catalysis in High Temperature Oxidations, which has been published in final form at https://doir.org/10.1002/anie.202102339. This article may be used for non-commercial purposes in accordance with Wiley Terms and Conditions for Self-Archiving."[EN] The behavior of single Pt atoms and small Pt clusters was investigated for high-temperature oxidations. The high stability of these molecular sites in CHA is a key to intrinsic structure-performance descriptions of elemental steps such as O-2 dissociation, and subsequent oxidation catalysis. Subtle changes in the atomic structure of Pt are responsible for drastic changes in performance driven by specific gas/metal/support interactions. Whereas single Pt atoms and Pt clusters (> ca. 1 nm) are unable to activate, scramble, and desorb two O-2 molecules at moderate T (200 degrees C), clusters