Ultrathin alumina passivation for improved photoelectrochemical water oxidation catalysis of tin oxide sensitized by a phosphonate-functionalized perylene diimide first without, and then with, CoOy
Abstract
Previously, a photoanode composed of nanostructured SnO2 coated with the perylene diimide dye N,N'-bis(phosphonomethyl)-3,4,9,10-perylenediimide (PMPDI) plus photoelectrochemically deposited cobalt oxide (CoOy) was shown to photoelectrochemically oxidize water at 31 ± 7% faradaic efficiency. A non-ideal part of that prior system is that the addition of the known CoOy water oxidation catalyst (WOC) resulted in a reduction of the total photocurrent rather than the anticipated increase, due to an increase in charge-carrier recombination. Herein, we show deposition of an ultrathin alumina overlayer applied by atomic layer deposition (ALD) on the SnO2/PMPDI photoanode can improve the photoactivity and catalytic activity of the system; the addition a ca. 1 nm-thick AlOx layer deposited on a 4000 nm (i.e., 4 micron) thick mesoporous anode system can and does have a positive, 2.5-fold improvement in the steady-state photocurrent with 29 ± 9% faradaic efficiency vs. the control anode without alumina passivation by reducing charge-carrier recombination. Moreover, ALD-deposited AlOx layer does help support the understanding of the “anti-catalysis” of co-depositing a CoOy WOC on the SnO2/PMPDI DS-PECs—specifically the picture of direct CoOy–SnO2 contact-mediated recombination—but that AlOx layer was unable to improve the photocurrent in a net SnO2/PMPDI/AlOx(/CoOy) system. We attribute the lack of a performance enhancementmore »
- Authors:
-
- Colorado State Univ., Fort Collins, CO (United States)
- Stony Brook Univ., NY (United States)
- Brookhaven National Lab. (BNL), Upton, NY (United States); Stony Brook Univ., NY (United States)
- Publication Date:
- Research Org.:
- Brookhaven National Laboratory (BNL), Upton, NY (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1830200
- Report Number(s):
- BNL-222376-2021-JAAM
Journal ID: ISSN 2398-4902
- Grant/Contract Number:
- SC0012704
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Sustainable Energy & Fuels
- Additional Journal Information:
- Journal Volume: 5; Journal Issue: 20; Journal ID: ISSN 2398-4902
- Publisher:
- Royal Society of Chemistry
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE
Citation Formats
Jewell, Carly F., Subramanian, Ashwanth, Nam, Chang-Yong, and Finke, Richard G. Ultrathin alumina passivation for improved photoelectrochemical water oxidation catalysis of tin oxide sensitized by a phosphonate-functionalized perylene diimide first without, and then with, CoOy. United States: N. p., 2021.
Web. doi:10.1039/d1se00908g.
Jewell, Carly F., Subramanian, Ashwanth, Nam, Chang-Yong, & Finke, Richard G. Ultrathin alumina passivation for improved photoelectrochemical water oxidation catalysis of tin oxide sensitized by a phosphonate-functionalized perylene diimide first without, and then with, CoOy. United States. https://doi.org/10.1039/d1se00908g
Jewell, Carly F., Subramanian, Ashwanth, Nam, Chang-Yong, and Finke, Richard G. Wed .
"Ultrathin alumina passivation for improved photoelectrochemical water oxidation catalysis of tin oxide sensitized by a phosphonate-functionalized perylene diimide first without, and then with, CoOy". United States. https://doi.org/10.1039/d1se00908g. https://www.osti.gov/servlets/purl/1830200.
@article{osti_1830200,
title = {Ultrathin alumina passivation for improved photoelectrochemical water oxidation catalysis of tin oxide sensitized by a phosphonate-functionalized perylene diimide first without, and then with, CoOy},
author = {Jewell, Carly F. and Subramanian, Ashwanth and Nam, Chang-Yong and Finke, Richard G.},
abstractNote = {Previously, a photoanode composed of nanostructured SnO2 coated with the perylene diimide dye N,N'-bis(phosphonomethyl)-3,4,9,10-perylenediimide (PMPDI) plus photoelectrochemically deposited cobalt oxide (CoOy) was shown to photoelectrochemically oxidize water at 31 ± 7% faradaic efficiency. A non-ideal part of that prior system is that the addition of the known CoOy water oxidation catalyst (WOC) resulted in a reduction of the total photocurrent rather than the anticipated increase, due to an increase in charge-carrier recombination. Herein, we show deposition of an ultrathin alumina overlayer applied by atomic layer deposition (ALD) on the SnO2/PMPDI photoanode can improve the photoactivity and catalytic activity of the system; the addition a ca. 1 nm-thick AlOx layer deposited on a 4000 nm (i.e., 4 micron) thick mesoporous anode system can and does have a positive, 2.5-fold improvement in the steady-state photocurrent with 29 ± 9% faradaic efficiency vs. the control anode without alumina passivation by reducing charge-carrier recombination. Moreover, ALD-deposited AlOx layer does help support the understanding of the “anti-catalysis” of co-depositing a CoOy WOC on the SnO2/PMPDI DS-PECs—specifically the picture of direct CoOy–SnO2 contact-mediated recombination—but that AlOx layer was unable to improve the photocurrent in a net SnO2/PMPDI/AlOx(/CoOy) system. We attribute the lack of a performance enhancement by CoOy WOC to incomplete coverage of each SnO2 nanoparticle by the AlOx. Overall, we find the addition of an optimized ultrathin AlOx layer (0.6 nm thick; deposited at 85 °C) improves the SnO2/PMPDI/AlOx system's photoactivity by a factor of up to ca. 3-fold with reduced recombination. These results document that metal-oxide passivation by low-temperature ALD can be an effective strategy for improving the water oxidation performance of even nanostructured dye sensitized-photoelectrochemical cell.},
doi = {10.1039/d1se00908g},
journal = {Sustainable Energy & Fuels},
number = 20,
volume = 5,
place = {United States},
year = {Wed Sep 22 00:00:00 EDT 2021},
month = {Wed Sep 22 00:00:00 EDT 2021}
}
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