Rapid Prediction of Multimetallic Electrocatalysts for CO2 Reduction from First-principles

With dwindling fossil fuels and rising concern about their impact on climate, renewable energies have attracted a considerable amount of attention since last decade. It is urgent to develop cost effective energy storage technologies that can store and release excess power to fill in the gaps when the sun is not shining or the wind is not blowing. Electrochemical reduction of CO2, if coupled with hydrogen (H2) from photocatalytic water splitting, provides a promising solution for the utilization of the abundant greenhouse gas in the Earth’s atmosphere and the intermittent electrical energy from solar panels and wind turbines for fuels and chemicals that are traditionally derived from petroleum. Unfortunately, there are currently no catalysts capable of carrying out this chemistry with both high activity and selectivity. Copper (Cu) is, arguably, the only known metal that produces appreciable amounts of hydrocarbons and oxygenates, although at high overpotentials (~1.0 V). Cu is, by no means, optimal. It is a really exciting field to find improved catalysts for electrochemical reduction of CO2, ideally to hydrocarbons or oxygenates. Tailoring the local chemical reactivity of Cu sites by alloying with other metal atoms could potentially reduce the energy loss for CO2 reduction and enhance the Faraday efficiency to liquid fuels (e.g., ethanol). While the traditional trial-and-error method for catalyst development usually relies on chemical intuition and is time consuming, recent emergence of a descriptor-based materials design approach has significantly improved this and allows the discovery of more efficient catalysts from first-principles. In this talk, I will discuss our mechanistic studies of CO2 reduction to C2 species and develop a rapid screening approach that explore the wide geometrical and chemical phase space of multimetallic alloys with lower potential loss and higher selectivity to liquid fuels.