Abstract
<h2>Summary</h2> Formulating knowledge of structure-function relationships in heterogeneous catalysis is central to the design of efficient catalysts; yet, the elucidation of dominant reaction sites has remained as a challenge. Here, we present a methodology that can be used to visualize metal-gas and metal-oxide-gas interfaces in three dimensions and to quantify their catalytic activity levels. As a case study, CH<sub>4</sub> oxidation occurring in a Pt/CeO<sub>2</sub> system is chosen. By employing thermally robust Pt@CeO<sub>2</sub> model catalysts with size-tunable and monodisperse cores, and gas-permeable shells, we reconstruct a series of structures in 3D via electron tomography and match the information to activity data and theoretical calculations. This strategy reveals that two different interfaces catalyze the CH<sub>4</sub> oxidation and that their contribution to the overall rate changes with the Pt size, temperature, and gas atmosphere. Our results provide an analytic platform on which to explore reaction pathways and mechanisms applicable to multiple reactions and materials.
Highlights
The interplay between oxide supports and supported metal nanoparticles is of high significance in the field of heterogeneous catalysis [1,2,3,4,5]
Formulating knowledge of structure-function relationships in heterogeneous catalysis is central to the rational design of highly efficient catalysts, yet the elucidation of dominant reaction sites has remained as a grand challenge for researchers
While the role of oxides was oversimplified in the past, evidence suggests that the use of redox-active oxides as a support material can dramatically reshape the landscape of multiple high-value catalytic processes [6,7,8,9,10,11,12,13,14]
Summary
The interplay between oxide supports and supported metal nanoparticles is of high significance in the field of heterogeneous catalysis [1,2,3,4,5]. By employing thermally robust Pt@CeO2 model catalysts with size-tunable and monodisperse cores, and gas-permeable shells, we reconstruct a series of heterogeneous structures in 3D via electron tomography and match the information precisely to catalytic activity data and theoretical calculations.
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