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Predictive Removal of Interfacial Defect-Induced Trap States between Titanium Dioxide Nanoparticles via Sub-Monolayer Zirconium Coating
[Image: see text] First principles modeling of anatase TiO(2) surfaces and their interfacial contacts shows that defect-induced trap states within the band gap arise from intrinsic structural distortions, and these can be corrected by modification with Zr(IV) ions. Experimental testing of these pred...
Autores principales: | , , , , , , , |
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Formato: | Online Artículo Texto |
Lenguaje: | English |
Publicado: |
American Chemical Society
2022
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Acceso en línea: | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9841567/ https://www.ncbi.nlm.nih.gov/pubmed/36660098 http://dx.doi.org/10.1021/acs.jpcc.2c06927 |
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author | Debgupta, Joyashish Lari, Leonardo Isaacs, Mark Carey, John McKenna, Keith P. Lazarov, Vlado K. Chechik, Victor Douthwaite, Richard E. |
author_facet | Debgupta, Joyashish Lari, Leonardo Isaacs, Mark Carey, John McKenna, Keith P. Lazarov, Vlado K. Chechik, Victor Douthwaite, Richard E. |
author_sort | Debgupta, Joyashish |
collection | PubMed |
description | [Image: see text] First principles modeling of anatase TiO(2) surfaces and their interfacial contacts shows that defect-induced trap states within the band gap arise from intrinsic structural distortions, and these can be corrected by modification with Zr(IV) ions. Experimental testing of these predictions has been undertaken using anatase nanocrystals modified with a range of Zr precursors and characterized using structural and spectroscopic methods. Continuous-wave electron paramagnetic resonance (EPR) spectroscopy revealed that under illumination, nanoparticle–nanoparticle interfacial hole trap states dominate, which are significantly reduced after optimizing the Zr doping. Fabrication of nanoporous films of these materials and charge injection using electrochemical methods shows that Zr doping also leads to improved electron conductivity and mobility in these nanocrystalline systems. The simple methodology described here to reduce the concentration of interfacial defects may have wider application to improving the efficiency of systems incorporating metal oxide powders and films including photocatalysts, photovoltaics, fuel cells, and related energy applications. |
format | Online Article Text |
id | pubmed-9841567 |
institution | National Center for Biotechnology Information |
language | English |
publishDate | 2022 |
publisher | American Chemical Society |
record_format | MEDLINE/PubMed |
spelling | pubmed-98415672023-01-17 Predictive Removal of Interfacial Defect-Induced Trap States between Titanium Dioxide Nanoparticles via Sub-Monolayer Zirconium Coating Debgupta, Joyashish Lari, Leonardo Isaacs, Mark Carey, John McKenna, Keith P. Lazarov, Vlado K. Chechik, Victor Douthwaite, Richard E. J Phys Chem C Nanomater Interfaces [Image: see text] First principles modeling of anatase TiO(2) surfaces and their interfacial contacts shows that defect-induced trap states within the band gap arise from intrinsic structural distortions, and these can be corrected by modification with Zr(IV) ions. Experimental testing of these predictions has been undertaken using anatase nanocrystals modified with a range of Zr precursors and characterized using structural and spectroscopic methods. Continuous-wave electron paramagnetic resonance (EPR) spectroscopy revealed that under illumination, nanoparticle–nanoparticle interfacial hole trap states dominate, which are significantly reduced after optimizing the Zr doping. Fabrication of nanoporous films of these materials and charge injection using electrochemical methods shows that Zr doping also leads to improved electron conductivity and mobility in these nanocrystalline systems. The simple methodology described here to reduce the concentration of interfacial defects may have wider application to improving the efficiency of systems incorporating metal oxide powders and films including photocatalysts, photovoltaics, fuel cells, and related energy applications. American Chemical Society 2022-12-23 /pmc/articles/PMC9841567/ /pubmed/36660098 http://dx.doi.org/10.1021/acs.jpcc.2c06927 Text en © 2022 The Authors. Published by American Chemical Society https://creativecommons.org/licenses/by/4.0/Permits the broadest form of re-use including for commercial purposes, provided that author attribution and integrity are maintained (https://creativecommons.org/licenses/by/4.0/). |
spellingShingle | Debgupta, Joyashish Lari, Leonardo Isaacs, Mark Carey, John McKenna, Keith P. Lazarov, Vlado K. Chechik, Victor Douthwaite, Richard E. Predictive Removal of Interfacial Defect-Induced Trap States between Titanium Dioxide Nanoparticles via Sub-Monolayer Zirconium Coating |
title | Predictive Removal
of Interfacial Defect-Induced Trap
States between Titanium Dioxide Nanoparticles via Sub-Monolayer Zirconium
Coating |
title_full | Predictive Removal
of Interfacial Defect-Induced Trap
States between Titanium Dioxide Nanoparticles via Sub-Monolayer Zirconium
Coating |
title_fullStr | Predictive Removal
of Interfacial Defect-Induced Trap
States between Titanium Dioxide Nanoparticles via Sub-Monolayer Zirconium
Coating |
title_full_unstemmed | Predictive Removal
of Interfacial Defect-Induced Trap
States between Titanium Dioxide Nanoparticles via Sub-Monolayer Zirconium
Coating |
title_short | Predictive Removal
of Interfacial Defect-Induced Trap
States between Titanium Dioxide Nanoparticles via Sub-Monolayer Zirconium
Coating |
title_sort | predictive removal
of interfacial defect-induced trap
states between titanium dioxide nanoparticles via sub-monolayer zirconium
coating |
url | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9841567/ https://www.ncbi.nlm.nih.gov/pubmed/36660098 http://dx.doi.org/10.1021/acs.jpcc.2c06927 |
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