Origin of photocatalytic activity enhancement in Pd/Pt-deposited anatase N-TiO2- experimental insights and DFT study of the (001) surface
Autor(a) principal: | |
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Data de Publicação: | 2020 |
Outros Autores: | , , , , , |
Tipo de documento: | Artigo |
Idioma: | eng |
Título da fonte: | Repositório Científico de Acesso Aberto de Portugal (Repositórios Cientìficos) |
Texto Completo: | http://hdl.handle.net/10400.9/3321 |
Resumo: | ABSTRACT: In pursuit of the ideal photocatalyst, cheap and stable semiconductor TiO(2)is considered to be a good choice if one is able to reduce its band gap and decrease the recombination rate of charge carriers. The approach that offers such improvements for energy conversion applications is the modification of TiO(2)with nitrogen and noble metals. However, the origin of these improvements and possibilities for further design of single-atom catalysts are not always straightforward. To shed light on the atomic-scale picture, we modeled the nitrogen-doped (001) anatase TiO(2)surface as a support for palladium and platinum single-atom deposition. The thermodynamics of various synthesis routes for Pd/Pt deposition and nitrogen doping is considered based on density functional theory (DFT)-calculated energies, highlighting the effect of nitrogen doping on metal dimer formation and metal-support interaction. XPS analysis of the valence band of the modified TiO(2)nanocrystals, and the calculated charge transfer and electronic structure of single-atom catalysts supported on the (001) anatase TiO(2)surface provide an insight into modifications occurring in the valence zone of TiO(2)due to nitrogen doping and Pd/Pt deposition at the surface. DFT results also show that substitutional nitrogen doping significantly increases metal-support interaction, while interstitial nitrogen doping promotes only Pt-support interaction. |
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Origin of photocatalytic activity enhancement in Pd/Pt-deposited anatase N-TiO2- experimental insights and DFT study of the (001) surfaceHydrogen productionTitanium dioxideNitrogen oxidesNanoparticlesABSTRACT: In pursuit of the ideal photocatalyst, cheap and stable semiconductor TiO(2)is considered to be a good choice if one is able to reduce its band gap and decrease the recombination rate of charge carriers. The approach that offers such improvements for energy conversion applications is the modification of TiO(2)with nitrogen and noble metals. However, the origin of these improvements and possibilities for further design of single-atom catalysts are not always straightforward. To shed light on the atomic-scale picture, we modeled the nitrogen-doped (001) anatase TiO(2)surface as a support for palladium and platinum single-atom deposition. The thermodynamics of various synthesis routes for Pd/Pt deposition and nitrogen doping is considered based on density functional theory (DFT)-calculated energies, highlighting the effect of nitrogen doping on metal dimer formation and metal-support interaction. XPS analysis of the valence band of the modified TiO(2)nanocrystals, and the calculated charge transfer and electronic structure of single-atom catalysts supported on the (001) anatase TiO(2)surface provide an insight into modifications occurring in the valence zone of TiO(2)due to nitrogen doping and Pd/Pt deposition at the surface. DFT results also show that substitutional nitrogen doping significantly increases metal-support interaction, while interstitial nitrogen doping promotes only Pt-support interaction.Royal Society of ChemistryRepositório do LNEGBatalovic, K.Radakovic, J.Bundaleski, N.Rakocevic, Z.Pasti, I.Skorodumova, N. V.Rangel, C. M.2020-01-01T00:00:00Z2020-01-01T00:00:00Z2024-12-01T00:00:00Zinfo:eu-repo/semantics/publishedVersioninfo:eu-repo/semantics/articleapplication/pdfhttp://hdl.handle.net/10400.9/3321engBatalovic, K... [et.al.] - Origin of photocatalytic activity enhancement in Pd/Pt-deposited anatase N-TiO2- experimental insights and DFT study of the (001) surface. In: Physical Chemistry Chemical Physics, 2020, Vol. 22 (33), p. 18536-185471463-907610.1039/d0cp03186k1463-9084info:eu-repo/semantics/embargoedAccessreponame:Repositório Científico de Acesso Aberto de Portugal (Repositórios Cientìficos)instname:Agência para a Sociedade do Conhecimento (UMIC) - FCT - Sociedade da Informaçãoinstacron:RCAAP2022-09-06T12:28:49Zoai:repositorio.lneg.pt:10400.9/3321Portal AgregadorONGhttps://www.rcaap.pt/oai/openaireopendoar:71602024-03-19T15:36:33.043348Repositório Científico de Acesso Aberto de Portugal (Repositórios Cientìficos) - Agência para a Sociedade do Conhecimento (UMIC) - FCT - Sociedade da Informaçãofalse |
dc.title.none.fl_str_mv |
Origin of photocatalytic activity enhancement in Pd/Pt-deposited anatase N-TiO2- experimental insights and DFT study of the (001) surface |
title |
Origin of photocatalytic activity enhancement in Pd/Pt-deposited anatase N-TiO2- experimental insights and DFT study of the (001) surface |
spellingShingle |
Origin of photocatalytic activity enhancement in Pd/Pt-deposited anatase N-TiO2- experimental insights and DFT study of the (001) surface Batalovic, K. Hydrogen production Titanium dioxide Nitrogen oxides Nanoparticles |
title_short |
Origin of photocatalytic activity enhancement in Pd/Pt-deposited anatase N-TiO2- experimental insights and DFT study of the (001) surface |
title_full |
Origin of photocatalytic activity enhancement in Pd/Pt-deposited anatase N-TiO2- experimental insights and DFT study of the (001) surface |
title_fullStr |
Origin of photocatalytic activity enhancement in Pd/Pt-deposited anatase N-TiO2- experimental insights and DFT study of the (001) surface |
title_full_unstemmed |
Origin of photocatalytic activity enhancement in Pd/Pt-deposited anatase N-TiO2- experimental insights and DFT study of the (001) surface |
title_sort |
Origin of photocatalytic activity enhancement in Pd/Pt-deposited anatase N-TiO2- experimental insights and DFT study of the (001) surface |
author |
Batalovic, K. |
author_facet |
Batalovic, K. Radakovic, J. Bundaleski, N. Rakocevic, Z. Pasti, I. Skorodumova, N. V. Rangel, C. M. |
author_role |
author |
author2 |
Radakovic, J. Bundaleski, N. Rakocevic, Z. Pasti, I. Skorodumova, N. V. Rangel, C. M. |
author2_role |
author author author author author author |
dc.contributor.none.fl_str_mv |
Repositório do LNEG |
dc.contributor.author.fl_str_mv |
Batalovic, K. Radakovic, J. Bundaleski, N. Rakocevic, Z. Pasti, I. Skorodumova, N. V. Rangel, C. M. |
dc.subject.por.fl_str_mv |
Hydrogen production Titanium dioxide Nitrogen oxides Nanoparticles |
topic |
Hydrogen production Titanium dioxide Nitrogen oxides Nanoparticles |
description |
ABSTRACT: In pursuit of the ideal photocatalyst, cheap and stable semiconductor TiO(2)is considered to be a good choice if one is able to reduce its band gap and decrease the recombination rate of charge carriers. The approach that offers such improvements for energy conversion applications is the modification of TiO(2)with nitrogen and noble metals. However, the origin of these improvements and possibilities for further design of single-atom catalysts are not always straightforward. To shed light on the atomic-scale picture, we modeled the nitrogen-doped (001) anatase TiO(2)surface as a support for palladium and platinum single-atom deposition. The thermodynamics of various synthesis routes for Pd/Pt deposition and nitrogen doping is considered based on density functional theory (DFT)-calculated energies, highlighting the effect of nitrogen doping on metal dimer formation and metal-support interaction. XPS analysis of the valence band of the modified TiO(2)nanocrystals, and the calculated charge transfer and electronic structure of single-atom catalysts supported on the (001) anatase TiO(2)surface provide an insight into modifications occurring in the valence zone of TiO(2)due to nitrogen doping and Pd/Pt deposition at the surface. DFT results also show that substitutional nitrogen doping significantly increases metal-support interaction, while interstitial nitrogen doping promotes only Pt-support interaction. |
publishDate |
2020 |
dc.date.none.fl_str_mv |
2020-01-01T00:00:00Z 2020-01-01T00:00:00Z 2024-12-01T00:00:00Z |
dc.type.status.fl_str_mv |
info:eu-repo/semantics/publishedVersion |
dc.type.driver.fl_str_mv |
info:eu-repo/semantics/article |
format |
article |
status_str |
publishedVersion |
dc.identifier.uri.fl_str_mv |
http://hdl.handle.net/10400.9/3321 |
url |
http://hdl.handle.net/10400.9/3321 |
dc.language.iso.fl_str_mv |
eng |
language |
eng |
dc.relation.none.fl_str_mv |
Batalovic, K... [et.al.] - Origin of photocatalytic activity enhancement in Pd/Pt-deposited anatase N-TiO2- experimental insights and DFT study of the (001) surface. In: Physical Chemistry Chemical Physics, 2020, Vol. 22 (33), p. 18536-18547 1463-9076 10.1039/d0cp03186k 1463-9084 |
dc.rights.driver.fl_str_mv |
info:eu-repo/semantics/embargoedAccess |
eu_rights_str_mv |
embargoedAccess |
dc.format.none.fl_str_mv |
application/pdf |
dc.publisher.none.fl_str_mv |
Royal Society of Chemistry |
publisher.none.fl_str_mv |
Royal Society of Chemistry |
dc.source.none.fl_str_mv |
reponame:Repositório Científico de Acesso Aberto de Portugal (Repositórios Cientìficos) instname:Agência para a Sociedade do Conhecimento (UMIC) - FCT - Sociedade da Informação instacron:RCAAP |
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Agência para a Sociedade do Conhecimento (UMIC) - FCT - Sociedade da Informação |
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RCAAP |
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RCAAP |
reponame_str |
Repositório Científico de Acesso Aberto de Portugal (Repositórios Cientìficos) |
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Repositório Científico de Acesso Aberto de Portugal (Repositórios Cientìficos) |
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Repositório Científico de Acesso Aberto de Portugal (Repositórios Cientìficos) - Agência para a Sociedade do Conhecimento (UMIC) - FCT - Sociedade da Informação |
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1799130231432282112 |