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Perovskite-type Oxides as Electrocatalysts in High Temperature Solid Electrolyte Reactor Applications

Meyer, Katja Elizabeth

Abstract Details

2017, Doctor of Philosophy, Ohio State University, Chemical Engineering.
A current field of interest in high temperature electrochemistry is utilizing solid electrolyte materials as electrochemical reactors. Solid electrolyte materials are dense, oxygen ion-conducting oxides which can be used at high temperatures (500-1000 °C) with electrocatalysts to form an electrochemical cell. This technology, in addition to being the basis for solid oxide fuel cells (SOFCs), may be used in different operating modes, allowing it to be used for a variety of applications. When this hardware is operating as a fuel cell, a chemical reaction causes electrons to flow through an external circuit, so that it becomes a chemical to electrical energy conversion device. However, if an external current is applied, it may be used as an ion pump for O2- ions, as well as an electrolyzer, depending on the direction of the current. If an external current is applied in the same direction as an SOFC, the device operates as an ion pump, and may be used as an air separation device capable of supplying oxygen to a process without the need for cryogenic distillation. This mode is also appropriate for partial oxidation reactions, in which the lack of molecular oxygen provides a selectivity advantage. Oxidative dehydrogenation of ethane (ODH) and oxidative coupling of methane (OCM) are two important partial oxidation reactions which may be performed in this type of solid electrolyte reactor and are capable of producing ethylene, a valuable chemical building block. In electrolyzer mode, a current is supplied in the opposite direction, and is capable of removing oxygen from species in the feed. This mode may be used for production of syngas from CO2 and water, supplying a means of creating a high value product while creating a closed carbon loop to eliminate CO2 emissions to the atmosphere. These applications of solid electrolyte reactors have been studied with a particular emphasis on designing a reactor and synthesizing active and selective perovskite-type oxide electrocatalysts. In each project, different electrocatalysts were used. For the air separation project, state-of-the-art materials were used while the reactor design was optimized. In the partial oxidation reactions studied, more emphasis was placed on the role of the anode catalyst, upon which the oxidation reaction occurs. LaxSr1-xTiO3±d and LaxSr1-xTiO3±dCls catalysts were studied for ODH, while SrCo0.9Nb0.1O3±d and SrCo0.9Nb0.1O3±dCls were synthesized for OCM. Production of syngas from CO2 and water were carried out comparing a widely studied material, Ni-YSZ, with LaxSr1-xTiO3±dCls. Finally, a preliminary experiment was also performed using Sr0.9Ce0.1Co0.2Fe0.8O3-d for CO2 reduction.
Umit Ozkan (Advisor)
Anne Co (Committee Member)
Jeffrey Chalmers (Committee Member)
188 p.

Recommended Citations

Citations

  • Meyer, K. E. (2017). Perovskite-type Oxides as Electrocatalysts in High Temperature Solid Electrolyte Reactor Applications [Doctoral dissertation, Ohio State University]. OhioLINK Electronic Theses and Dissertations Center. http://rave.ohiolink.edu/etdc/view?acc_num=osu1493821638601215

    APA Style (7th edition)

  • Meyer, Katja. Perovskite-type Oxides as Electrocatalysts in High Temperature Solid Electrolyte Reactor Applications. 2017. Ohio State University, Doctoral dissertation. OhioLINK Electronic Theses and Dissertations Center, http://rave.ohiolink.edu/etdc/view?acc_num=osu1493821638601215.

    MLA Style (8th edition)

  • Meyer, Katja. "Perovskite-type Oxides as Electrocatalysts in High Temperature Solid Electrolyte Reactor Applications." Doctoral dissertation, Ohio State University, 2017. http://rave.ohiolink.edu/etdc/view?acc_num=osu1493821638601215

    Chicago Manual of Style (17th edition)