Evaluation and optimization of porous and hierarchically porous materials for applications in energy storage and conversion
2014-09
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Evaluation and optimization of porous and hierarchically porous materials for applications in energy storage and conversion
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2014-09
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Materials with nm- and µm-scale pores are important in the design of efficient, safe, and versatile energy conversion and storage systems. In the research detailed in this thesis, the synthesis and testing of porous materials for lithium-ion battery anodes and for thermochemical fuel production are explored.The preparation, modification, and performance of various carbon and transition metal oxide composite materials for lithium-ion battery electrodes are discussed in the first part of this work. Of particular interest are TiO2/carbon composites that possess a three-dimensionally ordered macroporous (3DOM) structure, and, in some instances, additional mesoporosity. By changing the chelating agent used to stabilize the precursor for TiO2, crystallites of TiO2 can either be localized on the surface of the 3DOM structure or buried within the carbon matrix. This positioning has important ramifications for the electrochemical properties of the materials. In addition, the content of carbon in the composite materials can be altered. For carbon-rich composites, improved Li+ insertion/extraction capacities are attained by changing the voltage window used for cycling. Carbon can also be removed altogether, allowing for the formation 3DOM TiO¬2 with good electrochemical properties Conversion of the 3DOM TiO2 to sodium titanate is demonstrated via the ambient pressure treatment of the 3DOM material in sodium hydroxide. Subsequent ion-exchange with H+ results in the formation of hydrogen titanate materials with extremely high surface areas. A remnant of the 3DOM structure remains in these materials.Cerium oxide, praseodymium oxide and perovskite oxide-based catalysts for the thermochemical conversion of solar energy and abundant feedstocks (H2O and CO2) into useable fuels (H2 and CO) are investigated in the second part of this work. All of these materials possess a 3DOM structure and have moderate surface areas intended to improve reaction kinetics. Mixed oxides containing cerium are investigated with the aim of improving the amount of fuel produced, lowering the operational temperature and increasing thermal stability. Initial forays into the praseodymium oxide and perovskite oxide systems are also described, including evaluation of overall fuel production and fuel production kinetics. Special attention is paid to how structural changes during the high-temperature thermochemical reactions affect fuel productivity and kinetics.
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University of Minnesota Ph.D. dissertation. September 2014. Major: Chemistry. Advisor: Andreas Stein. 1 computer file (PDF); xxvii, 447 pages.
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Petkovich, Nicholas Daniel. (2014). Evaluation and optimization of porous and hierarchically porous materials for applications in energy storage and conversion. Retrieved from the University Digital Conservancy, https://hdl.handle.net/11299/168284.
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