Supported Catalyst Deactivation by Decomposition into Single Atoms Is Suppressed by Increasing Metal Loading.

Abstract

In the high-temperature environments needed to perform catalytic processes, supported precious metal catalysts severely lose their activity over time. Even brief exposure to high temperatures can lead to significant losses in activity, which forces manufacturers to use large amounts of noble metals to ensure effective catalyst function for a required lifetime. Generally, loss of catalytic activity is attributed to nanoparticle sintering, or processes by which larger particles grow at the expense of smaller ones. Here, by independently controlling particle size and particle loading using colloidal nanocrystals, we reveal the opposite process as a novel deactivation mechanism: nanoparticles rapidly lose activity by high-temperature nanoparticle decomposition into inactive single atoms. This deactivation route is remarkably fast, leading to severe loss of activity in as little as ten minutes. Importantly, this deactivation pathway is strongly dependent on particle density and concentration of support defect sites. A quantitative statistical model explains how for certain reactions, higher particle densities can lead to more stable catalysts.