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Adsorption of Nitrate and Bicarbonate on Fe-(Hydr)oxide

dc.creatorAcelas N.Y.spa
dc.creatorHadad C.spa
dc.creatorRestrepo A.spa
dc.creatorIbarguen C.spa
dc.creatorFlórez E.spa
dc.date.accessioned2017-12-19T19:36:44Z
dc.date.available2017-12-19T19:36:44Z
dc.date.created2017
dc.identifier.issn201669
dc.identifier.urihttp://hdl.handle.net/11407/4283
dc.description.abstractIn this work, we used density functional theory calculations to study the resulting complexes of adsorption and of inner- and outer-sphere adsorption-like of bicarbonate and nitrate over Fe-(hydr)oxide surfaces using acidic, neutral, and basic simulated pH conditions. High-spin states that follow the 5N + 1 (N is the number of Fe atoms, each having five unpaired electrons) rule are preferred. Monodentate mononuclear (MM1) surface complexes are shown to lead to the most favorable thermodynamic adsorption for both bicarbonate and nitrate with −63.91 and −28.25 kJ/mol, respectively, under neutral conditions. Our results suggest that four types of regular and charged-assisted hydrogen bonds are involved in the adsorption process; all of them can be classified as closed-shell (long-range or ionic). The formal charges induce unusually short and strong hydrogen bonds. The ability of high multiplicity states of Fe clusters to adsorb oxyanions in solvated environments arises from orbital interactions: the 4s virtual orbitals in Fe have a large affinity for the 2p-type electron pairs of oxygens. © 2017 American Chemical Society.eng
dc.language.isoeng
dc.publisherAmerican Chemical Societyspa
dc.relation.isversionofhttps://www.scopus.com/inward/record.uri?eid=2-s2.0-85018400304&doi=10.1021%2facs.inorgchem.7b00513&partnerID=40&md5=0f0ed31db5796b23540d9095320bb02dspa
dc.sourceScopusspa
dc.titleAdsorption of Nitrate and Bicarbonate on Fe-(Hydr)oxidespa
dc.typeArticleeng
dc.rights.accessrightsinfo:eu-repo/semantics/restrictedAccess
dc.contributor.affiliationAcelas, N.Y., Grupo de Materiales con Impacto, Matandmpac. Facultad de Facultad de Ciencias Básicas, Universidad de Medellín, Medellín, Colombiaspa
dc.contributor.affiliationHadad, C., Instituto de Química, Universidad de Antioquia UdeA, Calle 70 No. 52-21, Medellín, Colombiaspa
dc.contributor.affiliationRestrepo, A., Instituto de Química, Universidad de Antioquia UdeA, Calle 70 No. 52-21, Medellín, Colombiaspa
dc.contributor.affiliationIbarguen, C., Grupo de Materiales con Impacto, Matandmpac. Facultad de Facultad de Ciencias Básicas, Universidad de Medellín, Medellín, Colombia, Instituto de Química, Universidad de Antioquia UdeA, Calle 70 No. 52-21, Medellín, Colombiaspa
dc.contributor.affiliationFlórez, E., Grupo de Materiales con Impacto, Matandmpac. Facultad de Facultad de Ciencias Básicas, Universidad de Medellín, Medellín, Colombiaspa
dc.identifier.doi10.1021/acs.inorgchem.7b00513
dc.publisher.facultyFacultad de Ciencias Básicasspa
dc.abstractIn this work, we used density functional theory calculations to study the resulting complexes of adsorption and of inner- and outer-sphere adsorption-like of bicarbonate and nitrate over Fe-(hydr)oxide surfaces using acidic, neutral, and basic simulated pH conditions. High-spin states that follow the 5N + 1 (N is the number of Fe atoms, each having five unpaired electrons) rule are preferred. Monodentate mononuclear (MM1) surface complexes are shown to lead to the most favorable thermodynamic adsorption for both bicarbonate and nitrate with −63.91 and −28.25 kJ/mol, respectively, under neutral conditions. Our results suggest that four types of regular and charged-assisted hydrogen bonds are involved in the adsorption process; all of them can be classified as closed-shell (long-range or ionic). The formal charges induce unusually short and strong hydrogen bonds. The ability of high multiplicity states of Fe clusters to adsorb oxyanions in solvated environments arises from orbital interactions: the 4s virtual orbitals in Fe have a large affinity for the 2p-type electron pairs of oxygens. © 2017 American Chemical Society.eng
dc.creator.affiliationGrupo de Materiales con Impacto, Matandmpac. Facultad de Facultad de Ciencias Básicas, Universidad de Medellín, Medellín, Colombiaspa
dc.creator.affiliationInstituto de Química, Universidad de Antioquia UdeA, Calle 70 No. 52-21, Medellín, Colombiaspa
dc.relation.ispartofesInorganic Chemistryspa
dc.relation.ispartofesInorganic Chemistry Volume 56, Issue 9, 1 May 2017, Pages 5455-5464spa
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dc.type.versioninfo:eu-repo/semantics/publishedVersion
dc.type.driverinfo:eu-repo/semantics/article
dc.identifier.reponamereponame:Repositorio Institucional Universidad de Medellínspa
dc.identifier.instnameinstname:Universidad de Medellínspa


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