Theoretical Investigation of H Oxidation on the SrFeMoO (001) Perovskite Surface under Anodic Solid Oxide Fuel Ceil Conditions.
Periodic density functional theory (DFT) calculations and microkinetic modeling are used to investigate the electrochemical oxidation of H fuel on the (001) surface of SrFeiMoO (SFMO) perovskite under anodic solid oxide fuel cell conditions. Three surface models with different Fe/Mo ratios in the to...
| Publicado en: | Journal of the American Chemical Society Vol. 136; no. 23; pp. 8374 - 8387 |
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| Autores principales: | , , , , , , , |
| Formato: | Artículo |
| Publicado: |
American Chemical Society
6/11/2014
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| Materias: | |
| Acceso en línea: | Ver este registro en EBSCOhost |
| fields | @attributes: recordID: 1 pdfLink: plink: https://search.ebscohost.com/login.aspx?direct=true&db=hlh&AN=96808178&site=ehost-live header: @attributes: shortDbName: hlh uiTerm: 96808178 longDbName: Humanities International Complete uiTag: AN controlInfo: bkinfo: jinfo: jid: 00027863 ACS jtl: Journal of the American Chemical Society issn: 00027863 maglogo: N pubinfo: dt: 6/11/2014 vid: 136 iid: 23 pid: 997 pub: American Chemical Society artinfo: ui: 96808178 10.1021/ja502629j ppf: 8374 ppct: 13 formats: tig: atl: Theoretical Investigation of H Oxidation on the SrFeMoO (001) Perovskite Surface under Anodic Solid Oxide Fuel Ceil Conditions. aug: au: Suthirakun, Suwit Ammal, Salai Cheettu Muñoz-Garía, Ana B. Xiao, Guoliang Chen, Fanglin Zur Loye, Hans-Conrad Carter, Emily A. Heyden, Andreas affil: Department of Chemical Engineering, University of South Carolina, 301 Main Street, Columbia, South Carolina 29208, United States Department of Chemical Sciences, University of Naples Federico II, Naples 80126, Italy Department of Mechanical and Aerospace Engineering, Program in Applied and Computational Mathematics, and Andlinger Center for Energy and Environment, Princeton University, Princeton, New Jersey 08544, United States Department of Mechanical Engineering, University of South Carolina, 300 Main Street, Columbia, South Carolina 29208, United States Department of Chemistry and Biochemistry, University of South Carolina, 631 Sumter Street, Columbia, South Carolina 29208, United States su: Hydrogen oxidation Density functional theory Perovskite Anodic oxidation of metals Electrolytic oxidation sug: subj: Hydrogen oxidation Density functional theory Perovskite Anodic oxidation of metals Electrolytic oxidation ab: Periodic density functional theory (DFT) calculations and microkinetic modeling are used to investigate the electrochemical oxidation of H fuel on the (001) surface of SrFeiMoO (SFMO) perovskite under anodic solid oxide fuel cell conditions. Three surface models with different Fe/Mo ratios in the topmost layer-identified by ab initio thermodynamic analysis-are used to investigate the H oxidation mechanism. A microkinetic analysis that considers the effects of anode bias potential suggests that a higher Mo concentration in the surface increases the activity of the surface toward H oxidation. At operating voltage and anodic SOFC conditions, the model predicts that water desorption is rate-controlling and that stabilizing the oxygen vacancy structure increases the overall rate for H oxidation. Although we find that Mo plays a crucial role in improving catalytic activity of SFMO, under fuel cell operating conditions, the Mo content in the surface layer tends to be very low. On the basis of these results and in agreement with previous experimental observations, a strategy for improving the overall electrochemical performance of SFMO is increasing the Mo content or adding small amounts of an active transition metal, such as Ni, to the surface to lower the oxygen vacancy formation energy of the SFMO surface. pubtype: Academic Journal doctype: Article src: R language: English refInfo: copyright: @attributes: flag: Y dt: @attributes: year: 2014 holdings: @attributes: islocal: N |
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