(81b) First Principles Studies of Supported Heterogeneous Catalysts: Water-Gas Shift Reactivity at Metal/Oxide Interfaces

Advances in the theoretical understanding of interfacial catalysis have, over the past decade, enabled use periodic Density Functional Theory studies for screening of a surprisingly large ensemble of heterogeneous catalytic reactions. A significant challenge that has recently emerged in the field, however, is to extend these analyses to more structurally and mechanistically complex catalytic structures that cannot be described by traditional, idealized surface models. Successfully addressing this challenge, in turn, will require both developing realistic structural models for next-generation catalysts and finding strategies to analyze these structures in an efficient, high-throughput manner.

In this talk, I will discuss how we have applied strategies from computational and experimental heterogeneous catalysis to develop reactivity models for the water-gas shift (WGS) reaction at the interface between metal nanoparticles and oxide supports. I will describe the development of a detailed microkinetic model for WGS at Au/oxide interfaces from a tight feedback between theoretical and experimental analyses, and I will then discuss how this model may be generalized to other metals and other oxide supports. I will close by showing how both experimental and computational databases of reactivity data may be analyzed to efficiently identify descriptors for this complex interfacial chemistry, and I will suggest some strategies for exploiting these descriptors for future catalyst screening studies.