Interrelated Photo and Electrocatalytic Processes for the Reduction of CO2: Controlling Multiproton/Multielectron Events

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One important approach to remove undesirable CO2 in the atmosphere is to convert it to useful chemicals. This chemistry can be carried out in an electrochemical cell, but there are also recent advances showing that it is possible to do CO2 conversion with light. Thus, one goal is to react CO2 and water with sunlight to generate chemicals that are important both as fuels and as raw materials. Whether this chemistry is carried out electrochemically or photochemically, the reactions require energy. Practical CO2 conversion processes require that the energy input be as small as possible. To that end, catalysts are needed that minimize this energy input while also providing desirable reaction products. Presently, there is only limited understanding of the chemistry needed to build both electrocatalysts and photocatalysts that achieve such efficiency. The Bocarsly research group is advancing the understanding of the fundamental underlying chemistry necessary to develop practical CO2 catalysts. They are using this knowledge to construct new catalysts with improved chemical activity, product selectivity, and energy consumption. This knowledge-based advancement in catalyst design is critical to produce new routes to CO2 utilization that are environmentally responsible and socially beneficial. Dr. Bocarsly is actively engaging in outreach activities related to his research efforts including the education of next generation chemical researchers and K-12 outreach activities carried out under Princeton's Summer Laboratory Learning Program. His activities include a special program to encourage undergraduates in underrepresented groups to consider graduate education in the sciences.Funding from the National Science Foundation makes possible Dr. Bocarsly's studies at Princeton University on catalysts for electrochemical and photochemical CO2 utilization. Electrocatalytic studies focus on the use of metal alloy systems to address both materials science (i.e. electrode composition) and mechanistic question necessary to understand the reduction of aqueous CO2 to organic oxygenates. Presently, an understanding of the detailed mechanisms that allow the coupling of electron and proton transfer in the reduction of CO2 is being sought. Of particular interest is the reduction of CO2 to form carbon-carbon bonds. Three types of studies are underway: 1) The role of meta-stable surface oxides in the reduction of CO2; 2) The photochemical and electrocatalytic reduction of CO2 to CO using manganese carbonyl complexes as homogeneous catalysts; 3) Mixed metal electrodes as PCET catalysts for the formation of multiple carbon products. Understanding unifying chemical themes that underlie all these systems is transformative in terms of fundamental chemistry and the capability it brings in the areas of new fuel resources and environmental protection. Dr. Bocarsly is heavily involved in the education of next generation electrochemical researchers, who are key to an environmentally sensitive alternate energy future. In addition, Dr. Bocarsly carries out activities in the areas of community outreach and K-12 education through Princeton's Materials Program and Princeton's Summer Laboratory Learning Program. Bocarsly's research program also partners with Princeton's Department of Chemistry Outreach to Underrepresented Minors Program, to bring a diverse selection of the national undergraduate population into Princeton research labs for a 10-week summer research experience.This award reflects NSF's statutory mission and has been deemed worthy of support through evaluation using the Foundation's intellectual merit and broader impacts review criteria.