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Title: How Should Iron and Titanium be Combined in Oxides to Improve Photoelectrochemical Properties?

We discuss here for the first time how to combine iron and titanium metal ions to achieve a high photo-electrochemical activity for TiO 2-based photo-anodes in water splitting devices. To do so, a wide range of photoelectrode materials with tailored Ti/Fe ratio and element vicinity were synthesized by using the versatility of aqueous sol–gel chemistry in combination with a microwave-assisted crystallization process. At low ferric concentrations, single phase TiO 2 anatase doped with various Fe amounts were prepared. Strikingly, at higher ferric concentrations, we observed the concomitant crystallization of two polymorphs of Fe 2TiO 5. The as-synthesized compounds were tested as photoelectrode and compared with pure nanoparticles of TiO 2, Fe 2TiO 5 and α- or γ-Fe 2O 3 and with corresponding nanocomposites. When TiO 2 is slightly doped by Fe, the performance of this photo-electrode improves particularly in the low-bias region (< 1.0 V vs. reversible hydrogen electrode.) The photoanode exhibits a higher photocurrent than nanocomposite with TiO 2/Fe 2O 3 and FeTi 2O 5, and more cathodic onset potential. The former can be partly explained by a lower bandgap and a hole with a longer lifetime. For the latter, we propose that the nature of the heterojunction impactsmore » charge carrier recombination. Here, the results presented herein not only answer whether iron and titanium should be combined in the same structure or into heterostructured systems, but also on the importance of the arrangement of ions in the structure to improve the performances of the photoanode.« less
Authors:
 [1] ;  [2] ;  [1] ;  [3] ;  [2] ;  [4] ;  [1] ;  [5] ;  [1] ;  [1]
  1. Sorbonne Univ., Paris (France)
  2. Univ. de Lyon, Cedex (France)
  3. Univ. Montpellier II, Cedex (France)
  4. Univ. de Lyon, Cedex (France); Univ. of California, Los Angeles, CA (United States)
  5. Argonne National Lab. (ANL), Argonne, IL (United States)
Publication Date:
Grant/Contract Number:
AC02-06CH11357
Type:
Accepted Manuscript
Journal Name:
Journal of Physical Chemistry. C
Additional Journal Information:
Journal Volume: 120; Journal Issue: 43; Journal ID: ISSN 1932-7447
Publisher:
American Chemical Society
Research Org:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org:
Centre National de la Recherche Scientifique (CNRS); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22), Scientific User Facilities Division
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; "chimie-douce"; heterojunctions; photoanode; pseudo-brookite; water splitting
OSTI Identifier:
1389050

Petit, Sarah, Melissen, Sigismund T. A. G., Duclaux, Loraine, Sougrati, Moulay T., Le Bahers, Tangui, Sautet, Philippe, Dambournet, Damien, Borkiewicz, Olaf, Laberty-Robert, Christel, and Durupthy, Olivier. How Should Iron and Titanium be Combined in Oxides to Improve Photoelectrochemical Properties?. United States: N. p., Web. doi:10.1021/acs.jpcc.6b05794.
Petit, Sarah, Melissen, Sigismund T. A. G., Duclaux, Loraine, Sougrati, Moulay T., Le Bahers, Tangui, Sautet, Philippe, Dambournet, Damien, Borkiewicz, Olaf, Laberty-Robert, Christel, & Durupthy, Olivier. How Should Iron and Titanium be Combined in Oxides to Improve Photoelectrochemical Properties?. United States. doi:10.1021/acs.jpcc.6b05794.
Petit, Sarah, Melissen, Sigismund T. A. G., Duclaux, Loraine, Sougrati, Moulay T., Le Bahers, Tangui, Sautet, Philippe, Dambournet, Damien, Borkiewicz, Olaf, Laberty-Robert, Christel, and Durupthy, Olivier. 2016. "How Should Iron and Titanium be Combined in Oxides to Improve Photoelectrochemical Properties?". United States. doi:10.1021/acs.jpcc.6b05794. https://www.osti.gov/servlets/purl/1389050.
@article{osti_1389050,
title = {How Should Iron and Titanium be Combined in Oxides to Improve Photoelectrochemical Properties?},
author = {Petit, Sarah and Melissen, Sigismund T. A. G. and Duclaux, Loraine and Sougrati, Moulay T. and Le Bahers, Tangui and Sautet, Philippe and Dambournet, Damien and Borkiewicz, Olaf and Laberty-Robert, Christel and Durupthy, Olivier},
abstractNote = {We discuss here for the first time how to combine iron and titanium metal ions to achieve a high photo-electrochemical activity for TiO2-based photo-anodes in water splitting devices. To do so, a wide range of photoelectrode materials with tailored Ti/Fe ratio and element vicinity were synthesized by using the versatility of aqueous sol–gel chemistry in combination with a microwave-assisted crystallization process. At low ferric concentrations, single phase TiO2 anatase doped with various Fe amounts were prepared. Strikingly, at higher ferric concentrations, we observed the concomitant crystallization of two polymorphs of Fe2TiO5. The as-synthesized compounds were tested as photoelectrode and compared with pure nanoparticles of TiO2, Fe2TiO5 and α- or γ-Fe2O3 and with corresponding nanocomposites. When TiO2 is slightly doped by Fe, the performance of this photo-electrode improves particularly in the low-bias region (< 1.0 V vs. reversible hydrogen electrode.) The photoanode exhibits a higher photocurrent than nanocomposite with TiO2/Fe2O3 and FeTi2O5, and more cathodic onset potential. The former can be partly explained by a lower bandgap and a hole with a longer lifetime. For the latter, we propose that the nature of the heterojunction impacts charge carrier recombination. Here, the results presented herein not only answer whether iron and titanium should be combined in the same structure or into heterostructured systems, but also on the importance of the arrangement of ions in the structure to improve the performances of the photoanode.},
doi = {10.1021/acs.jpcc.6b05794},
journal = {Journal of Physical Chemistry. C},
number = 43,
volume = 120,
place = {United States},
year = {2016},
month = {10}
}