Advances in density functional theory have transformed catalyst design from an Edisonian endeavor into one guided by descriptor-based design principles. Recent successes notwithstanding, prevailing catalyst screening workflows are limited by two key aspects. First, precisely determining both the structural features of active site motifs under reaction conditions, and the stability of these active site motifs remains an enduring challenge. Second, while descriptor-based screening is routinely used for mono-functional catalysts, e.g. transition metals; these screening approaches remain underdeveloped for bi-functional catalysts, e.g. metal/oxide interfaces, in comparison. We address these knowledge gaps by introducing two new concepts that are built using model studies on catalysts that activate light hydrocarbons. First, we present an alloy-stability model that predicts both reactivity-descriptors (e.g. binding energies, rates) and stability-descriptors (e.g. nanoparticle cohesive energies, surface energies) for bimetallic nanoparticles having diverse shapes, sizes, and compositions. We then deploy the alloy stability model in conjunction with kinetic and spectroscopic measurements to uncover the catalytic active site ensemble for propene combustion. Insights from this combined theory and experimental study across a library of PtPd nanocrystals reveal that propene combustion is catalyzed by seven-coordinated step edges which dynamically form in the presence of co-fed water. We also demonstrate the utility of the alloy-stability model for designing catalysts with atomic-level specificity using a microkinetic model for NO dissociation. The property ⇒ structure relationships that form the core of our alloy-stability model enables us to reverse-engineer the structure of active sites which are both active and stable under reaction conditions. In the second part, we derive a new class of catalyst design principles for bi-functional metal/oxide interfaces using Au/doped-MgO as a model system. The electrostatic origin of these design principles transcends ubiquitous constraints related to bond-order conservation, thereby enhancing the flexibility in materials space for designing bi-functional interfaces as compared to mono-functional catalysts. We then integrate the alloy-stability model, design principles specific to bi-functional interfaces, and experimental studies, to engineer active sites of supported bimetallic catalysts for methanol synthesis from CO2.

Supported bimetallic catalysts for activating light hydrocarbons: Engineering active site ensembles with atomic-level specificity

Macromolecular Chemistry: The Second Century

[Author Benefits](https://scimeetings.acs.org/?utm_source=pubs_content_marketing&utm_medium=website&utm_campaign=0320_MCF_NPI_Launch_Spring_Homepage&ref=pubs_content_marketing)

[How to use SciMeetings](https://storage.googleapis.com/dl.morressier.com/acs/SciMeetings-ACSSpring2020-HowToGuide_M3020-Final.pdf)

[Frequently Asked Questions](https://storage.googleapis.com/dl.morressier.com/acs/SciMtng_ACSNMSp2020_FAQ_M3120_Final.pdf)

ACS Spring 2020 National Meeting & Expo

The official archive and repository for all ACS Meetings & Expositions abstracts and select posters or presentations.