Strong O 2p–Fe 3d Hybridization Observed in Solution-Grown Hematite Films by Soft X-ray Spectroscopies
Abstract
Photoelectrochemical (PEC) water splitting holds the potential as a direct route for solar energy conversation and storage. The performance of a PEC device is strongly influenced by the electronic properties of the photonanode surface. It has been shown that the synthesis methods can have a profound impact on the electronic properties and PEC performance of various photoelectrode materials such as hematite. Soft X-ray spectroscopic techniques, including O K-edge XAS and Fe L-edge XAS/XES, have been employed to investigate how the synthesis methods impact the electronic structure of resulting hematite materials. It is found that the hematite samples via solution regrowth methods show dramatically increased 3d-4sp band ratios in O K-edge XAS spectra and decreased relative elastic peak intensities in Fe L-edge RIXS spectra compared with samples synthesized via ALD or solution grown. The difference observed in O-K and Fe-L spectra indicated that solution regrowth strategy alters the O 2p-Fe 3d hybridization and hence the electronic structure of the hematite films, which proves to be beneficial for PEC performance of the hematite photoanode. Our findings provided new insights and potentially useful strategies for enhancing the PEC performance of photoanode materials.
- Authors:
-
[2];
[1];
[2];
[3]
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)
- Boston College, Chestnut Hill, MA (United States)
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS); Univ. of California, Santa Cruz, CA (United States)
- Publication Date:
- Research Org.:
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC)
- OSTI Identifier:
- 1530329
- Grant/Contract Number:
- AC02-05CH11231
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of Physical Chemistry. B, Condensed Matter, Materials, Surfaces, Interfaces and Biophysical Chemistry
- Additional Journal Information:
- Journal Volume: 122; Journal Issue: 2; Journal ID: ISSN 1520-6106
- Publisher:
- American Chemical Society
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Citation Formats
Ye, Yifan, Thorne, James E., Wu, Cheng Hao, Liu, Yi-Sheng, Du, Chun, Jang, Ji-Wook, Liu, Erik, Wang, Dunwei, and Guo, Jinghua. Strong O 2p–Fe 3d Hybridization Observed in Solution-Grown Hematite Films by Soft X-ray Spectroscopies. United States: N. p., 2017.
Web. doi:10.1021/acs.jpcb.7b06989.
Ye, Yifan, Thorne, James E., Wu, Cheng Hao, Liu, Yi-Sheng, Du, Chun, Jang, Ji-Wook, Liu, Erik, Wang, Dunwei, & Guo, Jinghua. Strong O 2p–Fe 3d Hybridization Observed in Solution-Grown Hematite Films by Soft X-ray Spectroscopies. United States. doi:https://doi.org/10.1021/acs.jpcb.7b06989
Ye, Yifan, Thorne, James E., Wu, Cheng Hao, Liu, Yi-Sheng, Du, Chun, Jang, Ji-Wook, Liu, Erik, Wang, Dunwei, and Guo, Jinghua. Wed .
"Strong O 2p–Fe 3d Hybridization Observed in Solution-Grown Hematite Films by Soft X-ray Spectroscopies". United States. doi:https://doi.org/10.1021/acs.jpcb.7b06989. https://www.osti.gov/servlets/purl/1530329.
@article{osti_1530329,
title = {Strong O 2p–Fe 3d Hybridization Observed in Solution-Grown Hematite Films by Soft X-ray Spectroscopies},
author = {Ye, Yifan and Thorne, James E. and Wu, Cheng Hao and Liu, Yi-Sheng and Du, Chun and Jang, Ji-Wook and Liu, Erik and Wang, Dunwei and Guo, Jinghua},
abstractNote = {Photoelectrochemical (PEC) water splitting holds the potential as a direct route for solar energy conversation and storage. The performance of a PEC device is strongly influenced by the electronic properties of the photonanode surface. It has been shown that the synthesis methods can have a profound impact on the electronic properties and PEC performance of various photoelectrode materials such as hematite. Soft X-ray spectroscopic techniques, including O K-edge XAS and Fe L-edge XAS/XES, have been employed to investigate how the synthesis methods impact the electronic structure of resulting hematite materials. It is found that the hematite samples via solution regrowth methods show dramatically increased 3d-4sp band ratios in O K-edge XAS spectra and decreased relative elastic peak intensities in Fe L-edge RIXS spectra compared with samples synthesized via ALD or solution grown. The difference observed in O-K and Fe-L spectra indicated that solution regrowth strategy alters the O 2p-Fe 3d hybridization and hence the electronic structure of the hematite films, which proves to be beneficial for PEC performance of the hematite photoanode. Our findings provided new insights and potentially useful strategies for enhancing the PEC performance of photoanode materials.},
doi = {10.1021/acs.jpcb.7b06989},
journal = {Journal of Physical Chemistry. B, Condensed Matter, Materials, Surfaces, Interfaces and Biophysical Chemistry},
number = 2,
volume = 122,
place = {United States},
year = {2017},
month = {11}
}
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Figures / Tables:
Figure 1: O K-edge XAS signals of Hematite films synthesized by different methods, the peak decomposition has also indicated in the figure. The experimental data is shown with the open circles and the fitted results are shown with the solid line. The substrate signals are included to fit the TFYmore »
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Figures / Tables found in this record: