Chemical and Biomolecular Engineering Theses and Dissertations
Permanent URI for this collectionhttp://hdl.handle.net/1903/2751
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Item Ceramic Materials Development for Intermediate Temperature Solid Oxide Fuel Cell (IT-SOFC)(2016) Pan, Ke-Ji; Wachsman, Eric D; Chemical Engineering; Digital Repository at the University of Maryland; University of Maryland (College Park, Md.)Solid oxide fuel cell (SOFC) is an electrochemical device that converts chemical energy into electric power with high efficiency. Traditional SOFC has its disadvantages, such as redox cycling instability and carbon deposition while using hydrocarbon fuels. It is because traditional SOFC uses Ni-cermet as anode. In order to solve these problems, ceramic anode is a good candidate to replace Ni. However, the conductivity of most ceramic anode materials are much lower than Ni metal, and it introduces high ohmic resistance. How to increase the conductivity is a hot topic in this research field. Based on our proposed mechanism, several types of ceramic materials have been developed. Vanadium doped perovskite, Sr1-x/2VxTi1-xO3 (SVT) and Sr0.2Na0.8Nb1-xVxO3 (SNNV), achieved the conductivity as high as 300 S*cm-1 in hydrogen, without any high temperature reduction. GDC electrolyte supported cell was fabricated with Sr0.2Na0.8Nb0.9V0.1O3 and the performance was measured in hydrogen and methane respectively. Due to vanadium’s intrinsic problems, the anode supported cell is not easy. Fe doped double perovskite Sr2CoMoO6 (SFCM) was also developed. By carefully doping Fe, the conductivity was improved over one magnitude, without any vigorous reducing conditions. SFCM anode supported cell was successfully fabricated with GDC as the electrolyte. By impregnating Ni-GDC nano particles into the anode, the cell can be operated at lower temperatures while having higher performance than the traditional Ni-cermet cells. Meanwhile, this SFCM anode supported SOFC has long term stability in the reformate containing methane. During the anode development, cathode improvement caused by a thin Co-GDC layer was observed. By adding this Co-GDC layer between the electrolyte and the cathode, the interfacial resistance decreases due to fast oxygen ion transport. This mechanism was confirmed via isotope exchange. This Co-GDC layer works with multiple kinds of cathodes and the modified cell’s performance is 3 times as the traditional Ni-GDC cell. With this new method, lowering the SOFC operation temperature is feasible.Item Synthesis of Novel Alkaline Polymer Electrolyte for Alkaline Fuel Cell Applicaitons(2012) Luo, Yanting; Wang, Chunsheng; Chemical Engineering; Digital Repository at the University of Maryland; University of Maryland (College Park, Md.)Development of the intrinsically OH- conductive polymeric electrolyte (alkaline polymer electrolyte, APE) is the critical component to enable the wide application of alkaline fuel cell (AFC) technology. Alkaline polymer electrolyte fuel cell (APEFC) based on AFC technology has been revived recently for applications in transportation and portable electronic devices due to its advantages of using non-noble metal catalysts, faster oxygen reduction in alkaline medium, and compact design. The research described in this dissertation aims to synthesize a novel APE, with controlled ionic conductivity and mechanical strength to achieve high fuel cell power density and long durability. Most APEs synthesized up to now use a modification of existing engineering polymer backbones, which are very difficult to balance its mechanical properties with its ionic conductivities. In this research, we copolymerized APE precursor polymers, namely poly (methyl methacrylate-co-butyl acrylate-co vinylbenzyl chloride) (PMBV) from three functional monomers, methyl methacrylate (MMA), butyl acrylate (BA) and vinylbenzyl chloride (VBC), where VBC was the functional group that was attached with trimethylamine (TMA) and was the OH- carrier after ion-exchanging. MMA was used for mechanical support and BA was used to alleviate the brittleness coming from MMA and VBC. We synthesized alkaline polymer electrolytes from bottom-up polymerization of these selected functional monomers using free radical solution and miniemulsion copolymerization techniques. By miniemulsion copolymerization, the properties of the obtained APEs could be precisely controlled by tuning the (1) monomer ratio, (2) glass transition temperature (Tg), (3) molecular weight (MW), and (4) crosslinking the copolymer. The increase in Tg was realized by eliminating BA from monomers, which was a low Tg component. MW was optimized through investigating binary copolymerization kinetics factors (initiator and surfactant). For crosslinking, the newly obtained poly (methyl methacrylate-co-vinylbenzyl chloride) (PMV) was crosslinked as a semi-interpenetrating network (s-IPN) to reduce water uptake and thus enhanced the mechanical strength in a humidified environment for APEFCs. After the optimization, our best quaternized PMBV (QPMBV) series APE membranes could reach a maximum power density of 180 mW/cm2 and the crosslinked QPMV APE could last 420 hours on APEFCs, which was among the best overall performance in APE technologies. In the future, we propose to use fluorinated polymer monomers to redesign the polymer backbone. Another direction in the design of APEs is to reselect the possible functional OH- carrier groups to make APEs more chemically and mechanically stable in a high pH environment. And last but not least, atomic force spectroscopy (AFM) is proposed to observe the APE nanostructure, the ionic conductive path, and the local mechanical strength by applying a small voltage between the tip and stage.