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Browsing by Author "Guo, Junsong"
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Item New Understandings of Ethanol Oxidation Reaction Mechanism on Pd/C and Pd2Ru/C Catalysts in Alkaline Direct Ethanol Fuel Cells(Elsevier, 2018-05) Guo, Junsong; Chen, Rongrong; Zhu, Fu-Chun; Sun, Shi-Gang; Vilullas, Hebe M.; Engineering Technology, School of Engineering and TechnologyEthanol oxidation reaction (EOR) on Pd2Ru/C and Pd/C catalysts in alkaline media is studied comprehensively by cyclic voltammetry, chronoamperometry, in situ FTIR, single fuel cell test and electrochemical impedance spectroscopy measurements. The results show that, as compared to Pd/C, Pd2Ru/C favors acetaldehyde formation and hinders its oxidation. Based on X-ray absorption data, which evidence that Ru promotes a larger electronic vacancy of the Pd 4d band, it is expected that the formation of adsorbed ethoxy is favored on Pd2Ru/C and followed by its oxidation to acetaldehyde facilitated by oxygenated species provided by Ru. In contrast, acetaldehyde oxidation is more difficult on Pd2Ru/C than on Pd/C likely because the adsorption energy of the reactive species is increased. We also show that the performance of Pd2Ru/C anode in alkaline direct ethanol fuel cell (ADEFC) is initially better but degrades much more rapidly than that with Pd/C anode under the same test conditions. The degradation is demonstrated to result from the accumulation of large amounts of acetaldehyde, which in alkaline media forms dimers by the aldol condensation reaction. The dimers tend to be responsible for blocking the active sites for further ethanol oxidation. This comprehensive study provides new understandings of the roles of Ru in Pd2Ru/C for EOR in alkaline media, unveils the causes of the performance degradation of fuel cells with Pd2Ru/C and demonstrates that initial good performances are not necessarily a valid criterion for selecting appropriate anode catalysts for ADEFC applications.Item NOVEL NANOSTRUCTURED HIGH-PERFORMANCE ANION EXCHANGE IONOMERS FOR ANION EXCHANGE MEMBRANE FUEL CELLS(Office of the Vice Chancellor for Research, 2012-04-13) Sun, Lu; Guo, Junsong; Zhou, Jie; Xu, Qingming; Chu, Deryn; Chen, RongrongA novel block copolymer, styrene-ethylene/butylene-styrene (SEBS), was chosen as the starting material to prepare pendant quaternary ammonium-based ionomers with an ion-exchange-capacity (IEC) of 0.66, 1.30, and 1.54 meq g-1, denoted by QSEBS-L, QSEBS-M, and QSEBS-H, respectively. These QSEBS ionomers were demonstrated to have excellent dimensional stability against hydration without significantly sacrificing the ionic conductivity as compared to the widely studied polysulfone (PSf) based ionomers. The water uptake of the QSEBS-based ionomers depended on their functionality; a higher IEC in the ionomer resulted in more water uptake and a higher ionic conductivity. The MEAs fabricated with the QSEBS-M and QSEBS-H ionomers showed the best H2/O2 fuel cell performance with peak power densities reaching 210 mW cm-2 at 50 °C, which was significantly higher than that of the PSf-based ionomers (~30 mW cm-2). Electrochemical impedance spec-troscopy (EIS) analysis indicated that the superior fuel cell performance ob-served with the QSEBS-based ionomers can be attributed to: (1) the low in-ternal cell resistance due to good comparability of the QSEBS-based ionomers with the membranes and (2) the low mass transport and charge transport in both the anode and the cathode due to the excellent dimension-al stability and balanced conductivity-hydrophobicity originated by the unique morphology of the QSEBS-based ionomers. AFM phase imaging measurements of the QSEBS-based ionomers revealed unique nanostruc-tures containing isolated hydrophobic and continuous anion conducting hy-drophilic domains. By further optimizing the chemistry and morphology of the ionomers and the membranes, the resistance of the anode and cathode of the AEMFCs will be further reduced.