Leduc, Jennifer, Goenuellue, Yakup, Ruoko, Tero-Petri, Fischer, Thomas, Mayrhofer, Leonhard, Tkachenko, Nikolai V., Dong, Chung-Li, Held, Alexander, Moseler, Michael and Mathur, Sanjay ORCID: 0000-0003-2765-2693 (2019). Electronically Coupled Uranium and Iron Oxide Heterojunctions as Efficient Water Oxidation Catalysts. Adv. Funct. Mater., 29 (50). WEINHEIM: WILEY-V C H VERLAG GMBH. ISSN 1616-3028

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Abstract

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 approximate to 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 (alpha-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.

Item Type: Journal Article
Creators:
CreatorsEmailORCIDORCID Put Code
Leduc, JenniferUNSPECIFIEDUNSPECIFIEDUNSPECIFIED
Goenuellue, YakupUNSPECIFIEDUNSPECIFIEDUNSPECIFIED
Ruoko, Tero-PetriUNSPECIFIEDUNSPECIFIEDUNSPECIFIED
Fischer, ThomasUNSPECIFIEDUNSPECIFIEDUNSPECIFIED
Mayrhofer, LeonhardUNSPECIFIEDUNSPECIFIEDUNSPECIFIED
Tkachenko, Nikolai V.UNSPECIFIEDUNSPECIFIEDUNSPECIFIED
Dong, Chung-LiUNSPECIFIEDUNSPECIFIEDUNSPECIFIED
Held, AlexanderUNSPECIFIEDUNSPECIFIEDUNSPECIFIED
Moseler, MichaelUNSPECIFIEDUNSPECIFIEDUNSPECIFIED
Mathur, SanjayUNSPECIFIEDorcid.org/0000-0003-2765-2693UNSPECIFIED
URN: urn:nbn:de:hbz:38-131385
DOI: 10.1002/adfm.201905005
Journal or Publication Title: Adv. Funct. Mater.
Volume: 29
Number: 50
Date: 2019
Publisher: WILEY-V C H VERLAG GMBH
Place of Publication: WEINHEIM
ISSN: 1616-3028
Language: English
Faculty: Faculty of Mathematics and Natural Sciences
Divisions: Faculty of Mathematics and Natural Sciences > Department of Chemistry > Institute of Inorganic Chemistry
Subjects: no entry
Uncontrolled Keywords:
KeywordsLanguage
ULTRATHIN HEMATITE FILMS; LAYER-BY-LAYER; THIN-FILM; TRANSITION-METAL; OXYGEN; STATES; EVOLUTION; SPECTROSCOPY; PERFORMANCE; UNDERLAYERMultiple languages
Chemistry, Multidisciplinary; Chemistry, Physical; Nanoscience & Nanotechnology; Materials Science, Multidisciplinary; Physics, Applied; Physics, Condensed MatterMultiple languages
Refereed: Yes
URI: http://kups.ub.uni-koeln.de/id/eprint/13138

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