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Full-Text Articles in Physical Sciences and Mathematics
Advancements Toward Sustainable Solar Fuel Production Utilizing Reductive Homogeneous Electro- And Photocatalysis, Hunter Pratt Shirley
Advancements Toward Sustainable Solar Fuel Production Utilizing Reductive Homogeneous Electro- And Photocatalysis, Hunter Pratt Shirley
Electronic Theses and Dissertations
Molecular CO2 and H+ reductive catalysts, whether they be electro- or photocatalytic, have been shown to be possible routes of harnessing solar energy in a clean, renewable manner. There are few electrocatalysts operating at reasonable overpotentials to prove useful in artificial photosynthetic systems, and there are a number of environmental factors within these systems that have yet to be evaluated. Photo-driven catalysis is rare, difficult to control, and rarely provides high-value CO2 reduction products. I report herein an exceptionally low overpotential H+ reduction catalyst, a method of modulating electrocatalysts in-situ to improve performance, a first-of-its-kind mononuclear proton reduction photocatalyst, a …
Robust Nickel Catalysts Supported By Biaryl-Bridged Pyridyl-N-Heterocyclic Carbenes For Carbon Dioxide Reduction To Value-Added Products, Hunter Allen Dulaney
Robust Nickel Catalysts Supported By Biaryl-Bridged Pyridyl-N-Heterocyclic Carbenes For Carbon Dioxide Reduction To Value-Added Products, Hunter Allen Dulaney
Electronic Theses and Dissertations
Carbon dioxide is a greenhouse gas, but also represents a readily accessible C1 feedstock for conversion to solar fuels and value-added chemicals. However, CO2 is relatively inert and very negative voltages or strong chemical reductants are comfor its conversion. An additional challenge lies in achieving these reactions in water where aqueous protons are utilized selectively for CO2 reduction rather than hydrogen generation. Our strategy for CO2 reduction involves the design of new homogeneous catalysts with tunable geometries and polyaromatic frameworks with increased delocalization to lower overpotentials for catalysis. We report a family of biaryl-bridged pyridyl-N-heterocyclic carbene-based ligands and their corresponding …