DFT Comparison of N-Nitrosodimethylamine (NDMA) Decomposition Pathways Over Ni and Pd

Autores
Ranea, Victor Alejandro; Strathmann, T. J.; Shapley, J. R.; Schneider, W. F.
Año de publicación
2011
Idioma
inglés
Tipo de recurso
artículo
Estado
versión publicada
Descripción
Recent experimental studies report rapid and efficient reduction of N-nitrosodimethylamine (NDMA) and related aquatic micropollutants mediated by palladium (Pd) and nickel (Ni) surfaces, but differing mechanisms have been reported for the surface reactions. Here, NDMA adsorption and fragmentation on Ni and Pd surfaces has been studied using supercell slab density functional theory (DFT) calculations. NDMA adsorbs in two stable configurations on each surface. Upright binding through the NO fragment is slightly preferred energetically and provides entrance to an exothermic N, O dissociation pathway with moderately high activation barriers. Flat binding through the NNO plane is somewhat less favorable but leads to a facile and exothermic dissociation across the N, N bond. These results suggest that both mechanisms are in competition and may contribute to the observed catalytic reduction of NDMA over these metals in aqueous solution.
Fil: Ranea, Victor Alejandro. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - La Plata. Instituto de Investigaciones Fisicoquímicas Teóricas y Aplicadas. Universidad Nacional de La Plata. Facultad de Ciencias Exactas. Instituto de Investigaciones Fisicoquímicas Teóricas y Aplicadas; Argentina. Universidad Nacional de La Plata; Argentina. University of Notre Dame; Estados Unidos
Fil: Strathmann, T. J.. University of Illinois. Urbana - Champaign; Estados Unidos
Fil: Shapley, J. R.. University of Illinois. Urbana - Champaign; Estados Unidos
Fil: Schneider, W. F.. University of Notre Dame; Estados Unidos. University of Illinois. Urbana - Champaign; Estados Unidos
Materia
CATALYTIC REDUCTION
DENSITY FUNCTIONAL CALCULATIONS
NICKEL
PALLADIUM
WATER POLLUTANTS
Nivel de accesibilidad
acceso abierto
Condiciones de uso
https://creativecommons.org/licenses/by-nc-sa/2.5/ar/
Repositorio
CONICET Digital (CONICET)
Institución
Consejo Nacional de Investigaciones Científicas y Técnicas
OAI Identificador
oai:ri.conicet.gov.ar:11336/219363
Acceder
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network_name_str CONICET Digital (CONICET)
spelling DFT Comparison of N-Nitrosodimethylamine (NDMA) Decomposition Pathways Over Ni and PdRanea, Victor AlejandroStrathmann, T. J.Shapley, J. R.Schneider, W. F.CATALYTIC REDUCTIONDENSITY FUNCTIONAL CALCULATIONSNICKELPALLADIUMWATER POLLUTANTShttps://purl.org/becyt/ford/1.4https://purl.org/becyt/ford/1Recent experimental studies report rapid and efficient reduction of N-nitrosodimethylamine (NDMA) and related aquatic micropollutants mediated by palladium (Pd) and nickel (Ni) surfaces, but differing mechanisms have been reported for the surface reactions. Here, NDMA adsorption and fragmentation on Ni and Pd surfaces has been studied using supercell slab density functional theory (DFT) calculations. NDMA adsorbs in two stable configurations on each surface. Upright binding through the NO fragment is slightly preferred energetically and provides entrance to an exothermic N, O dissociation pathway with moderately high activation barriers. Flat binding through the NNO plane is somewhat less favorable but leads to a facile and exothermic dissociation across the N, N bond. These results suggest that both mechanisms are in competition and may contribute to the observed catalytic reduction of NDMA over these metals in aqueous solution.Fil: Ranea, Victor Alejandro. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - La Plata. Instituto de Investigaciones Fisicoquímicas Teóricas y Aplicadas. Universidad Nacional de La Plata. Facultad de Ciencias Exactas. Instituto de Investigaciones Fisicoquímicas Teóricas y Aplicadas; Argentina. Universidad Nacional de La Plata; Argentina. University of Notre Dame; Estados UnidosFil: Strathmann, T. J.. University of Illinois. Urbana - Champaign; Estados UnidosFil: Shapley, J. R.. University of Illinois. Urbana - Champaign; Estados UnidosFil: Schneider, W. F.. University of Notre Dame; Estados Unidos. University of Illinois. Urbana - Champaign; Estados UnidosWiley VCH Verlag2011-03info:eu-repo/semantics/articleinfo:eu-repo/semantics/publishedVersionhttp://purl.org/coar/resource_type/c_6501info:ar-repo/semantics/articuloapplication/pdfapplication/pdfhttp://hdl.handle.net/11336/219363Ranea, Victor Alejandro; Strathmann, T. J.; Shapley, J. R.; Schneider, W. F.; DFT Comparison of N-Nitrosodimethylamine (NDMA) Decomposition Pathways Over Ni and Pd; Wiley VCH Verlag; Chemcatchem; 3; 5; 3-2011; 898-9031867-3880CONICET DigitalCONICETenginfo:eu-repo/semantics/altIdentifier/doi/10.1002/cctc.201000398info:eu-repo/semantics/altIdentifier/url/https://chemistry-europe.onlinelibrary.wiley.com/doi/10.1002/cctc.201000398info:eu-repo/semantics/openAccesshttps://creativecommons.org/licenses/by-nc-sa/2.5/ar/reponame:CONICET Digital (CONICET)instname:Consejo Nacional de Investigaciones Científicas y Técnicas2025-09-03T09:52:03Zoai:ri.conicet.gov.ar:11336/219363instacron:CONICETInstitucionalhttp://ri.conicet.gov.ar/Organismo científico-tecnológicoNo correspondehttp://ri.conicet.gov.ar/oai/requestdasensio@conicet.gov.ar; lcarlino@conicet.gov.arArgentinaNo correspondeNo correspondeNo correspondeopendoar:34982025-09-03 09:52:03.611CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicasfalse
dc.title.none.fl_str_mv DFT Comparison of N-Nitrosodimethylamine (NDMA) Decomposition Pathways Over Ni and Pd
title DFT Comparison of N-Nitrosodimethylamine (NDMA) Decomposition Pathways Over Ni and Pd
spellingShingle DFT Comparison of N-Nitrosodimethylamine (NDMA) Decomposition Pathways Over Ni and Pd
Ranea, Victor Alejandro
CATALYTIC REDUCTION
DENSITY FUNCTIONAL CALCULATIONS
NICKEL
PALLADIUM
WATER POLLUTANTS
title_short DFT Comparison of N-Nitrosodimethylamine (NDMA) Decomposition Pathways Over Ni and Pd
title_full DFT Comparison of N-Nitrosodimethylamine (NDMA) Decomposition Pathways Over Ni and Pd
title_fullStr DFT Comparison of N-Nitrosodimethylamine (NDMA) Decomposition Pathways Over Ni and Pd
title_full_unstemmed DFT Comparison of N-Nitrosodimethylamine (NDMA) Decomposition Pathways Over Ni and Pd
title_sort DFT Comparison of N-Nitrosodimethylamine (NDMA) Decomposition Pathways Over Ni and Pd
dc.creator.none.fl_str_mv Ranea, Victor Alejandro
Strathmann, T. J.
Shapley, J. R.
Schneider, W. F.
author Ranea, Victor Alejandro
author_facet Ranea, Victor Alejandro
Strathmann, T. J.
Shapley, J. R.
Schneider, W. F.
author_role author
author2 Strathmann, T. J.
Shapley, J. R.
Schneider, W. F.
author2_role author
author
author
dc.subject.none.fl_str_mv CATALYTIC REDUCTION
DENSITY FUNCTIONAL CALCULATIONS
NICKEL
PALLADIUM
WATER POLLUTANTS
topic CATALYTIC REDUCTION
DENSITY FUNCTIONAL CALCULATIONS
NICKEL
PALLADIUM
WATER POLLUTANTS
purl_subject.fl_str_mv https://purl.org/becyt/ford/1.4
https://purl.org/becyt/ford/1
dc.description.none.fl_txt_mv Recent experimental studies report rapid and efficient reduction of N-nitrosodimethylamine (NDMA) and related aquatic micropollutants mediated by palladium (Pd) and nickel (Ni) surfaces, but differing mechanisms have been reported for the surface reactions. Here, NDMA adsorption and fragmentation on Ni and Pd surfaces has been studied using supercell slab density functional theory (DFT) calculations. NDMA adsorbs in two stable configurations on each surface. Upright binding through the NO fragment is slightly preferred energetically and provides entrance to an exothermic N, O dissociation pathway with moderately high activation barriers. Flat binding through the NNO plane is somewhat less favorable but leads to a facile and exothermic dissociation across the N, N bond. These results suggest that both mechanisms are in competition and may contribute to the observed catalytic reduction of NDMA over these metals in aqueous solution.
Fil: Ranea, Victor Alejandro. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - La Plata. Instituto de Investigaciones Fisicoquímicas Teóricas y Aplicadas. Universidad Nacional de La Plata. Facultad de Ciencias Exactas. Instituto de Investigaciones Fisicoquímicas Teóricas y Aplicadas; Argentina. Universidad Nacional de La Plata; Argentina. University of Notre Dame; Estados Unidos
Fil: Strathmann, T. J.. University of Illinois. Urbana - Champaign; Estados Unidos
Fil: Shapley, J. R.. University of Illinois. Urbana - Champaign; Estados Unidos
Fil: Schneider, W. F.. University of Notre Dame; Estados Unidos. University of Illinois. Urbana - Champaign; Estados Unidos
description Recent experimental studies report rapid and efficient reduction of N-nitrosodimethylamine (NDMA) and related aquatic micropollutants mediated by palladium (Pd) and nickel (Ni) surfaces, but differing mechanisms have been reported for the surface reactions. Here, NDMA adsorption and fragmentation on Ni and Pd surfaces has been studied using supercell slab density functional theory (DFT) calculations. NDMA adsorbs in two stable configurations on each surface. Upright binding through the NO fragment is slightly preferred energetically and provides entrance to an exothermic N, O dissociation pathway with moderately high activation barriers. Flat binding through the NNO plane is somewhat less favorable but leads to a facile and exothermic dissociation across the N, N bond. These results suggest that both mechanisms are in competition and may contribute to the observed catalytic reduction of NDMA over these metals in aqueous solution.
publishDate 2011
dc.date.none.fl_str_mv 2011-03
dc.type.none.fl_str_mv info:eu-repo/semantics/article
info:eu-repo/semantics/publishedVersion
http://purl.org/coar/resource_type/c_6501
info:ar-repo/semantics/articulo
format article
status_str publishedVersion
dc.identifier.none.fl_str_mv http://hdl.handle.net/11336/219363
Ranea, Victor Alejandro; Strathmann, T. J.; Shapley, J. R.; Schneider, W. F.; DFT Comparison of N-Nitrosodimethylamine (NDMA) Decomposition Pathways Over Ni and Pd; Wiley VCH Verlag; Chemcatchem; 3; 5; 3-2011; 898-903
1867-3880
CONICET Digital
CONICET
url http://hdl.handle.net/11336/219363
identifier_str_mv Ranea, Victor Alejandro; Strathmann, T. J.; Shapley, J. R.; Schneider, W. F.; DFT Comparison of N-Nitrosodimethylamine (NDMA) Decomposition Pathways Over Ni and Pd; Wiley VCH Verlag; Chemcatchem; 3; 5; 3-2011; 898-903
1867-3880
CONICET Digital
CONICET
dc.language.none.fl_str_mv eng
language eng
dc.relation.none.fl_str_mv info:eu-repo/semantics/altIdentifier/doi/10.1002/cctc.201000398
info:eu-repo/semantics/altIdentifier/url/https://chemistry-europe.onlinelibrary.wiley.com/doi/10.1002/cctc.201000398
dc.rights.none.fl_str_mv info:eu-repo/semantics/openAccess
https://creativecommons.org/licenses/by-nc-sa/2.5/ar/
eu_rights_str_mv openAccess
rights_invalid_str_mv https://creativecommons.org/licenses/by-nc-sa/2.5/ar/
dc.format.none.fl_str_mv application/pdf
application/pdf
dc.publisher.none.fl_str_mv Wiley VCH Verlag
publisher.none.fl_str_mv Wiley VCH Verlag
dc.source.none.fl_str_mv reponame:CONICET Digital (CONICET)
instname:Consejo Nacional de Investigaciones Científicas y Técnicas
reponame_str CONICET Digital (CONICET)
collection CONICET Digital (CONICET)
instname_str Consejo Nacional de Investigaciones Científicas y Técnicas
repository.name.fl_str_mv CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicas
repository.mail.fl_str_mv dasensio@conicet.gov.ar; lcarlino@conicet.gov.ar
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score 13.13397

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