The rise of global CO2 levels along with a significant imbalance in the nitrogen cycle has created an urgent need to move towards renewable and carbon neutral energy technologies. Electrochemically driven and atomically precise multi-functional catalytic technologies are critical components to move towards a sustainable energy future. However, unlike traditional catalytic systems, these technologies are not fundamentally understood, which forms a major bottleneck for their commercialization. An effective way to overcome this bottleneck is by elucidating the factors that dictate the stability of the underlying solid-liquid and solid-solid multifunctional interfaces present in these technologies under operating conditions. Ab-initio Density Functional Theory (DFT) is a widely used tool to investigate such factors at an atomic scale. Its application has led to successful modeling of many catalytic systems of varying degrees of complexity. However, efforts are still needed to capture a range of phenomena, such as: (i) high adsorbate coverages, (ii) multidentate adsorbates, (iii) explicit solvent effects, (iv) multi-elemental alloys, (v) multi-phasic interactions and (vi) defected catalyst morphologies. Taken together, these complexities result in (i) a large number of possible atomic configurations (O>105), creating a need for the development of efficient algorithmic workflows to sample large phase spaces, and (ii) a need to develop systematic approaches to understand the complex physics governing these phenomena.

In this talk, I will describe a generalized workflow to systematically account for these phenomena. An in-house python-based graph theory algorithm is developed to systematically sample and identify relevant catalytic models. The models are used to study (i) the underlying reaction mechanism at the electrochemical interfaces under an explicit solvent environment, and (ii) physics governing the formation of multifunctional inverse metal oxide catalysts on defected metal surface. The results highlight novel insights into the governing interactions that drive the: (i) activity and selectivity of key nitrogen and oxygen based electro-catalytic reactions, and (ii) stability of industrially relevant metal oxides on defected transition metal catalysts. Such analyses provide pathways to engineer active, selective, and stable catalytic interfaces, crucial to realize a sustainable and carbon neutral energy economy.