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题名: Mechanistic Studies of Water Electrolysis and Hydrogen Electro-Oxidation on High Temperature Ceria-Based Solid Oxide Electrochemical Cells
作者: Zhang, Chunjuan1, 2;  Yu, Yi1, 2;  Grass, Michael E.3;  Dejoie, Catherine3;  Ding, Wuchen4;  Gaskell, Karen1, 2;  Jabeen, Naila3;  Hong, Young Pyo3;  Shayorskiy, Andrey3;  Bluhrn, Hendrik3;  Li, Wei-Xue4;  Jackson, Gregory S.1, 2;  Hussain, Zahid3;  Liu, Zhi3, 5;  Eichhorn, Bryan W.1, 2
刊名: JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
发表日期: 2013-08-07
DOI: 10.1021/ja402604u
卷: 135, 期:31, 页:11572-11579
收录类别: SCI
文章类型: Article
WOS标题词: Science & Technology ;  Physical Sciences
类目[WOS]: Chemistry, Multidisciplinary
研究领域[WOS]: Chemistry
英文摘要: Through the use of ambient pressure X-ray photoelectron spectroscopy (APXPS) and a single-sided solid oxide electrochemical cell (SOC), we have studied the mechanism of electrocatalytic splitting of water (H2O + 2e(-) -> H-2 + O2-) and electro-oxidation of hydrogen (H-2 + O2- -> H2O + 2e(-)) at similar to 700 degrees C in 0.5 Torr of H-2/H2O on ceria (CeO2-x) electrodes. The experiments reveal a transient build-up of surface intermediates (OH- and Ce3+) and show the separation of charge at the gas solid interface exclusively in the electrochemically active region of the SOC. During water electrolysis on ceria, the increase in surface potentials of the adsorbed OH- and incorporated O2- differ by 0.25 eV in the active regions. For hydrogen electro-oxidation on ceria, the surface concentrations of OH- and O2- shift significantly from their equilibrium values. These data suggest that the same charge transfer step (H2O + Ce3+ double left right arrow Ce4+ + OH- + H-center dot) is rate limiting in both the forward (water electrolysis) and reverse (H-2 electrooxidation) reactions. This separation of potentials reflects an induced surface dipole layer on the ceria surface and represents the effective electrochemical double layer at a gas-solid interface. The in situ XPS data and DFT calculations show that the chemical origin of the OH-/O2- potential separation resides in the reduced polarization of the Ce-OH bond due to the increase of Ce3+ on the electrode surface. These results provide a graphical illustration of the electrochemically driven surface charge transfer processes under relevant and nonultrahigh vacuum conditions.
关键词[WOS]: RAY PHOTOELECTRON-SPECTROSCOPY ;  INITIO MOLECULAR-DYNAMICS ;  OXYGEN VACANCIES ;  SURFACE SCIENCE ;  FUEL-CELLS ;  TRANSITION ;  CHEMISTRY ;  METAL ;  OXIDATION ;  PRESSURE
语种: 英语
WOS记录号: WOS:000323019400036
Citation statistics: 
内容类型: 期刊论文
URI标识: http://cas-ir.dicp.ac.cn/handle/321008/137807
Appears in Collections:中国科学院大连化学物理研究所_期刊论文

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作者单位: 1.Univ Maryland, Dept Chem & Biochem, College Pk, MD 20742 USA
2.Univ Maryland, Dept Mech Engn, College Pk, MD 20742 USA
3.Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Berkeley, CA 94720 USA
4.Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Catalysis, Dalian 116023, Peoples R China
5.ShanghaiTech Univ, Sch Phys Sci & Technol, Shanghai 200031, Peoples R China

Recommended Citation:
Zhang, Chunjuan,Yu, Yi,Grass, Michael E.,et al. Mechanistic Studies of Water Electrolysis and Hydrogen Electro-Oxidation on High Temperature Ceria-Based Solid Oxide Electrochemical Cells[J]. JOURNAL OF THE AMERICAN CHEMICAL SOCIETY,2013,135(31):11572-11579.
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