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    题名: Electronically Coupled Uranium and Iron Oxide Heterojunctions as Efficient Water Oxidation Catalysts
    作者: J. Leduc;Y. Gönüllü;T. Ruoko;T. Fischer;L. Mayrhofer;N. V. Tkachenko;C. L. Dong;A. Held;M. Moseler;S. Mathur
    日期: 2019-10-03
    上传时间: 2020-06-01 12:13:20 (UTC+8)
    摘要: The most critical challenge faced in realizing a high efficiency photoelectrochemical water splitting process is the lack of suitable photoanodes enabling the transfer of four electrons involved in the complex oxygen evolution reaction (OER). Uranium oxides are efficient catalysts due to their wide range optical absorption (E g ≈ 1.8–3.2 eV), high photoconductivity, and multiple valence switching among uranium centers that improves the charge propagation kinetics. Herein, thin films of depleted uranium oxide (U3O8) are demonstrated grown via chemical vapor deposition effectively accelerate the OER in conjunction with hematite (α‐Fe2O3) overlayers through a built‐in potential at the interface. Density functional theory simulations demonstrate that the multivalence of U and Fe ions induce the adjustment of the band alignment subject to the concentration of interfacial Fe ions. In general, the equilibrium state depicts a type II band edge as the favored alignment, which improves charge‐transfer processes as observed in transient and X‐ray absorption (TAS and XAS) spectroscopy. The enhanced water splitting photocurrent density of the heterostructures (J = 2.42 mA cm−2) demonstrates the unexplored potential of uranium oxide in artificial photosynthesis.
    關聯: Advanced Functional Materials 29(50), 1905005
    DOI: 10.1002/adfm.201905005
    显示于类别:[物理學系暨研究所] 期刊論文

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