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ABSTRACT Recycling CO2 into Sustainable Hydrocarbon Fuels: Electrolysis of CO2 and H2O Christopher Ronald Graves Great quantities of hydrocarbon fuels will be needed for the foreseeable future, even if electricity based energy carriers begin to partially replace liquid hydrocarbons in the transportation sector. Fossil fuels and biomass are the most common feedstocks for production of hydrocarbon fuels. However, using renewable or nuclear energy, carbon dioxide and water can be recycled into sustainable hydrocarbon fuels in non-biological processes which remove oxygen from CO2 and H2O (the reverse of fuel combustion). Capture of CO2 from the atmosphere would enable a closed-loop carbon-neutral fuel cycle. The purpose of this work was to develop critical components of a system that recycles CO2 into liquid hydrocarbon fuels. The concept is examined at several scales, beginning with a broad scope analysis of large-scale sustainable energy systems and ultimately studying electrolysis of CO2 and H2O in high temperature solid oxide cells as the heart of the energy conversion, in the form of three experimental studies. The contributions of these studies include discoveries about electrochemistry and materials that could significantly improve the overall energy use and economics of the CO2-to-fuels system. The broad scale study begins by assessing the sustainability and practicality of the various energy carriers that could replace petroleum-derived hydrocarbon fuels, including other hydrocarbons, hydrogen, and storage of electricity on-board vehicles in batteries, ultracapacitors, and flywheels. Any energy carrier can store the energy of any energy source. This sets the context for CO2 recycling – sustainable energy sources like solar and wind power can be used to provide the most energy-dense, convenient fuels which can be readily used in the existing infrastructure. The many ways to recycle CO2 into hydrocarbons, based on thermolysis, thermochemical loops, electrolysis, and photoelectrolysis of CO2 and/or H2O, are critically reviewed. A process based on high temperature co-electrolysis of CO2 and H2O to produce syngas (CO/H2 mixture) is identified as a promising method. High temperature electrolysis makes very efficient use of electricity and heat (near-100% electricity-to-syngas efficiency), provides high reaction rates, and the syngas produced can be catalytically converted to hydrocarbons in well-known fuel synthesis reactors (e.g. Fischer-Tropsch). The experimental studies of high temperature electrolysis are made at different scales – at the cell level, electrode level, and in materials and microstructure development. The results include cell performance and durability, insight into electrode reaction mechanisms, and newPDF Image | Electrolysis of CO2 and H2O
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