Nanostructured Materials for Electrochemical CO2 Reduction to Multicarbon Products

Abstract

Electrochemical CO2 reduction technology offers promise as a method of carbon storage and energy storage in a world where anthropogenic CO2 levels in the atmosphere are linked with climatic degradation. The main missing piece of an electrochemical CO2 reduction system is the catalyst. Therefore, there are significant efforts to design effective catalysts to convert CO2 into useful products. Multicarbon products are targeted for their relatively high commercial value. In a review of the relevant literature, we present some of the most successful catalyst design strategies for conversion of CO2 into multicarbon products. Following this, we introduce in detail the catalyst design features implemented in the results portion of this work. Next, the experimental methods used in this thesis are described. These include the synthesis of catalyst materials, the methods for measuring the performance of these catalysts, and finally the characterization techniques used to describe the catalysts. The material characterization provides information used to understand their performance. The fourth chapter comprises a high-level view of the economics of CO2 conversion. This analysis informs the areas of focus for researchers, with the ultimate goal of making CO2 conversion a profitable venture. This is followed by a complete experimental work presenting a novel, high-performance catalyst, entitled "Achieving 94% Faradic Efficiency toward Multicarbon Products in CO2 Electroreduction via Synergy Between AgCu Single-Atom Alloy and Ag Nanoparticles." The material is characterized comprehensively, and the catalytic performance is explained using theoretical calculations from collaborators. The following chapter consists of the initial stages of a second experimental work based on another catalyst material. The catalyst is a high-entropy alloy with potential for CO2 conversion performance. Following synthesis and characterization details, the next steps for this work are detailed. Finally, we summarize conclusions of this work and discuss new directions for this research area.