The catalytic conversion of CO2 into liquid fuels and industrial chemicals sold to offset carbon management costs has been receiving increased attention in recent literature. Despite a growing body of publications on catalyst development, there is still a scarcity of data on which types of reactors can be used, their scalability, and their performance at realistic process conditions. This talk will detail how the electronic structure of the catalyst and related reaction chemistry dictates both the opportunities and constraints placed on the size and scalability of reactors for this application. The first system discussed is based on atomically precise Au25q clusters (q = -1, 0, +1) where we have manipulated the electronic structure of the cluster to tailor electrocatalytic activity. We will also detail the performance of charged Au25 clusters in a realistic reactor system that utilizes simple photovoltaics and solar-charged battery sources to drive the CO2 conversion reaction. The second system discussed is based on Au-ZnO heterostructures where visible-light plasmonic excitations in Au are used to generate heat and drive chemical reactions on the ZnO substrate. The performance and characteristics of Au-ZnO have been evaluated in simple, continuous flow, fixed- and fluidized-bed, photochemical reactors where product distributions are easily tuned with light intensity. We will conclude by illustrating how the reactor characterization, reaction kinetics, mass and energy balance data determined in our studies provide some of the best possible estimates available for assessing the size, scale, and utility of catalytic CO2 conversion approaches.

Catalyst and reactor engineering for carbon-neutral CO2 conversion

251st National Meeting (2016)

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