Simultaneous 2D Projection and 3D Topographic Imaging of Gas-Dependent Dynamics of Catalytic Nanoparticles.

ABSTRACT

Catalyst deactivation through pathways such as sintering of nanoparticles and degradation of the support is a critical factor when designing high-performance catalysts. Here, structural changes of supported nanoparticle catalysts are investigated in controlled gas environments (O2, H2O, and H2) at different temperatures by imaging simultaneously the nanoparticle structures in 2D projection and the 3D surface-sensitive topography. Platinum nanoparticles on carbon support as a model system are imaged in an environmental transmission electron microscope (ETEM), with concurrent acquisition of high-angle annular dark field scanning TEM (HAADF-STEM) and secondary electron (SE) images. Particle migration and coalescence occurs and shows gas-dependent kinetics, with nanoparticles moving across and through the support during and after coalescence. The temperature required for motion is lower in O2 than in H2O and H2, explained through the nature of the gas/nanoparticle interactions. In O2 and H2, the carbon support degrades by trench formation along migration pathways, and the particles move continuously, indicating a chemical reaction between gas and support. In H2O gas, motion is more discontinuous and oriented particle attachment occurs, as expected from theoretical predictions. These results suggest that multimodal imaging in ETEM that combines HAADF-STEM and SE data provides comprehensive information regarding catalyst dynamics and degradation mechanisms.