Ammonia Capture in Rhodium(II)-Based Metal–Organic Polyhedra via Synergistic Coordinative and H‑Bonding Interactions [Dataset]

30 pages. Table of Contents: S1. Materials and experimental methods: S1.1 Materials; S1.2 Experimental methods. -- S2. Computational methods. -- S3. Characterization of Rh-MOPs used as adsorbents for NH3. -- S4. NH3 uptake in H-RhMOP. -- S5. Computer simulation of the interaction between H-RhMOP and...

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Autores: Carné-Sánchez, Arnau, Martínez Esaín, Jordi, Rookard, Tanner, Flood, Christopher J., Faraudo, Jordi, Stylianou, Kyriakos C., Maspoch, Daniel
Tipo de recurso: conjunto de datos
Fecha de publicación:2023
País:España
Institución:Consejo Superior de Investigaciones Científicas (CSIC)
Repositorio:DIGITAL.CSIC. Repositorio Institucional del CSIC
OAI Identifier:oai:digital.csic.es:10261/336232
Acceso en línea:http://hdl.handle.net/10261/336232
Access Level:acceso abierto
Palabra clave:Experimental data showed
Developing new technologies
Benzene dicarboxylate
Aliphatic alkoxide chains
Least three cycles
Store ammonia safely
Mops strongly interact
Adsorption experiments revealed
Ammonia uptake performance
Ammonia uptake
Uptake capacity
Ammonia proceeds
Ammonia adsorbents
World
Upon activation
Three rh
Surface functionalization
Poses environmental
Porous hosts
Paddlewheel cluster
Outer surface
One decorated
Low concentrations
Hydroxyl groups
Health risks
First time
First step
Findings demonstrate
Diverse sectors
Bonded clusters
Based mops
Axial site
Acidic water
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oai_identifier_str oai:digital.csic.es:10261/336232
network_acronym_str ES
network_name_str España
repository_id_str
dc.title.none.fl_str_mv Ammonia Capture in Rhodium(II)-Based Metal–Organic Polyhedra via Synergistic Coordinative and H‑Bonding Interactions [Dataset]
title Ammonia Capture in Rhodium(II)-Based Metal–Organic Polyhedra via Synergistic Coordinative and H‑Bonding Interactions [Dataset]
spellingShingle Ammonia Capture in Rhodium(II)-Based Metal–Organic Polyhedra via Synergistic Coordinative and H‑Bonding Interactions [Dataset]
Carné-Sánchez, Arnau
Experimental data showed
Developing new technologies
Benzene dicarboxylate
Benzene dicarboxylate
Aliphatic alkoxide chains
Least three cycles
Store ammonia safely
Mops strongly interact
Adsorption experiments revealed
Ammonia uptake performance
Ammonia uptake
Uptake capacity
Ammonia proceeds
Ammonia adsorbents
World
Upon activation
Three rh
Surface functionalization
Poses environmental
Porous hosts
Paddlewheel cluster
Outer surface
One decorated
Low concentrations
Hydroxyl groups
Health risks
First time
First step
Findings demonstrate
Diverse sectors
Bonded clusters
Based mops
Axial site
Acidic water
title_short Ammonia Capture in Rhodium(II)-Based Metal–Organic Polyhedra via Synergistic Coordinative and H‑Bonding Interactions [Dataset]
title_full Ammonia Capture in Rhodium(II)-Based Metal–Organic Polyhedra via Synergistic Coordinative and H‑Bonding Interactions [Dataset]
title_fullStr Ammonia Capture in Rhodium(II)-Based Metal–Organic Polyhedra via Synergistic Coordinative and H‑Bonding Interactions [Dataset]
title_full_unstemmed Ammonia Capture in Rhodium(II)-Based Metal–Organic Polyhedra via Synergistic Coordinative and H‑Bonding Interactions [Dataset]
title_sort Ammonia Capture in Rhodium(II)-Based Metal–Organic Polyhedra via Synergistic Coordinative and H‑Bonding Interactions [Dataset]
dc.creator.none.fl_str_mv Carné-Sánchez, Arnau
Martínez Esaín, Jordi
Rookard, Tanner
Flood, Christopher J.
Faraudo, Jordi
Stylianou, Kyriakos C.
Maspoch, Daniel
author Carné-Sánchez, Arnau
author_facet Carné-Sánchez, Arnau
Martínez Esaín, Jordi
Rookard, Tanner
Flood, Christopher J.
Faraudo, Jordi
Stylianou, Kyriakos C.
Maspoch, Daniel
author_role author
author2 Martínez Esaín, Jordi
Rookard, Tanner
Flood, Christopher J.
Faraudo, Jordi
Stylianou, Kyriakos C.
Maspoch, Daniel
author2_role author
author
author
author
author
author
dc.contributor.none.fl_str_mv Carné-Sánchez, Arnau [arnau.carne@icn2.cat]
Maspoch, Daniel [daniel.maspoch@icn2.cat]
Consejo Superior de Investigaciones Científicas [https://ror.org/02gfc7t72]
dc.subject.none.fl_str_mv Experimental data showed
Developing new technologies
Benzene dicarboxylate
Benzene dicarboxylate
Aliphatic alkoxide chains
Least three cycles
Store ammonia safely
Mops strongly interact
Adsorption experiments revealed
Ammonia uptake performance
Ammonia uptake
Uptake capacity
Ammonia proceeds
Ammonia adsorbents
World
Upon activation
Three rh
Surface functionalization
Poses environmental
Porous hosts
Paddlewheel cluster
Outer surface
One decorated
Low concentrations
Hydroxyl groups
Health risks
First time
First step
Findings demonstrate
Diverse sectors
Bonded clusters
Based mops
Axial site
Acidic water
topic Experimental data showed
Developing new technologies
Benzene dicarboxylate
Benzene dicarboxylate
Aliphatic alkoxide chains
Least three cycles
Store ammonia safely
Mops strongly interact
Adsorption experiments revealed
Ammonia uptake performance
Ammonia uptake
Uptake capacity
Ammonia proceeds
Ammonia adsorbents
World
Upon activation
Three rh
Surface functionalization
Poses environmental
Porous hosts
Paddlewheel cluster
Outer surface
One decorated
Low concentrations
Hydroxyl groups
Health risks
First time
First step
Findings demonstrate
Diverse sectors
Bonded clusters
Based mops
Axial site
Acidic water
description 30 pages. Table of Contents: S1. Materials and experimental methods: S1.1 Materials; S1.2 Experimental methods. -- S2. Computational methods. -- S3. Characterization of Rh-MOPs used as adsorbents for NH3. -- S4. NH3 uptake in H-RhMOP. -- S5. Computer simulation of the interaction between H-RhMOP and NH3: S5.1. DFT calculations of the interaction between Rh2(Ac)4 and NH3; S5.1.2. DFT calculations of the interaction between Rh2(Ac)4, NH3 and H2O; S5.2. Computer simulation of the interaction between H-RhMMOP and NH3; S5.2.1. Parametrization of the Force Field from DFT calculations; S5.2.2. Molecular dynamic simulations of the interaction between H-RhMOP and NH3. -- S6. FTIR spectroscopy of ammonia-loaded H-RhMOP. -- S7. NH3 uptake in Rh2(Ac)4. -- S8. Digital photographs showing the regeneration of H-RhMOP. -- S9. NH3 uptake in OH-RhMOP and C12-RhMOP. -- S10. Computer simulation of the interaction between functionalized Rh-MOPs and NH3: S10.1 OH-RhMOP and NH3; S10.2 C12-RhMOP and NH3.
publishDate 2023
dc.date.none.fl_str_mv 2023
2023
2023
dc.type.none.fl_str_mv info:eu-repo/semantics/dataset
http://purl.org/coar/resource_type/c_ddb1
format dataset
dc.identifier.none.fl_str_mv http://hdl.handle.net/10261/336232
url http://hdl.handle.net/10261/336232
dc.language.none.fl_str_mv Inglés
language_invalid_str_mv Inglés
dc.relation.none.fl_str_mv Carné-Sánchez, Arnau; Martínez Esaín, Jordi; Rookard, Tanner; Flood, Christopher J.; Faraudo, Jordi; Stylianou, Kyriakos C.; Maspoch, Daniel. Ammonia Capture in Rhodium(II)-Based Metal-Organic Polyhedra via Synergistic Coordinative and H-Bonding Interactions. https://doi.org/10.1021/acsami.2c19206. http://hdl.handle.net/10261/336065
https://doi.org/10.1021/acsami.2c19206.s001
Sí
dc.rights.none.fl_str_mv info:eu-repo/semantics/openAccess
eu_rights_str_mv openAccess
dc.format.none.fl_str_mv application/pdf
dc.publisher.none.fl_str_mv Figshare
publisher.none.fl_str_mv Figshare
dc.source.none.fl_str_mv reponame:DIGITAL.CSIC. Repositorio Institucional del CSIC
instname:Consejo Superior de Investigaciones Científicas (CSIC)
instname_str Consejo Superior de Investigaciones Científicas (CSIC)
reponame_str DIGITAL.CSIC. Repositorio Institucional del CSIC
collection DIGITAL.CSIC. Repositorio Institucional del CSIC
repository.name.fl_str_mv
repository.mail.fl_str_mv
_version_ 1869406404099440640
spelling Ammonia Capture in Rhodium(II)-Based Metal–Organic Polyhedra via Synergistic Coordinative and H‑Bonding Interactions [Dataset]Carné-Sánchez, ArnauMartínez Esaín, JordiRookard, TannerFlood, Christopher J.Faraudo, JordiStylianou, Kyriakos C.Maspoch, DanielExperimental data showedDeveloping new technologiesBenzene dicarboxylateBenzene dicarboxylateAliphatic alkoxide chainsLeast three cyclesStore ammonia safelyMops strongly interactAdsorption experiments revealedAmmonia uptake performanceAmmonia uptakeUptake capacityAmmonia proceedsAmmonia adsorbentsWorldUpon activationThree rhSurface functionalizationPoses environmentalPorous hostsPaddlewheel clusterOuter surfaceOne decoratedLow concentrationsHydroxyl groupsHealth risksFirst timeFirst stepFindings demonstrateDiverse sectorsBonded clustersBased mopsAxial siteAcidic water30 pages. Table of Contents: S1. Materials and experimental methods: S1.1 Materials; S1.2 Experimental methods. -- S2. Computational methods. -- S3. Characterization of Rh-MOPs used as adsorbents for NH3. -- S4. NH3 uptake in H-RhMOP. -- S5. Computer simulation of the interaction between H-RhMOP and NH3: S5.1. DFT calculations of the interaction between Rh2(Ac)4 and NH3; S5.1.2. DFT calculations of the interaction between Rh2(Ac)4, NH3 and H2O; S5.2. Computer simulation of the interaction between H-RhMMOP and NH3; S5.2.1. Parametrization of the Force Field from DFT calculations; S5.2.2. Molecular dynamic simulations of the interaction between H-RhMOP and NH3. -- S6. FTIR spectroscopy of ammonia-loaded H-RhMOP. -- S7. NH3 uptake in Rh2(Ac)4. -- S8. Digital photographs showing the regeneration of H-RhMOP. -- S9. NH3 uptake in OH-RhMOP and C12-RhMOP. -- S10. Computer simulation of the interaction between functionalized Rh-MOPs and NH3: S10.1 OH-RhMOP and NH3; S10.2 C12-RhMOP and NH3.Ammonia (NH3) is among the world’s most widely produced bulk chemicals, given its extensive use in diverse sectors such as agriculture; however, it poses environmental and health risks at low concentrations. Therefore, there is a need for developing new technologies and materials to capture and store ammonia safely. Herein, we report for the first time the use of metal–organic polyhedra (MOPs) as ammonia adsorbents. We evaluated three different rhodium-based MOPs: [Rh2(bdc)2]12 (where bdc is 1,3-benzene dicarboxylate); one functionalized with hydroxyl groups at its outer surface [Rh2(OH-bdc)2]12 (where OH-bdc is 5-hydroxy-1,3-benzene dicarboxylate); and one decorated with aliphatic alkoxide chains at its outer surface [Rh2(C12O-bdc)2]12 (where C12O-bdc is 5-dodecoxybenzene-1,3-benzene dicarboxylate). Ammonia-adsorption experiments revealed that all three Rh-MOPs strongly interact with ammonia, with uptake capacities exceeding 10 mmol/gMOP. Furthermore, computational and experimental data showed that the mechanism of the interaction between Rh-MOPs and ammonia proceeds through a first step of coordination of NH3 to the axial site of the Rh(II) paddlewheel cluster, which triggers the adsorption of additional NH3 molecules through H-bonding interaction. This unique mechanism creates H-bonded clusters of NH3 on each Rh(II) axial site, which accounts for the high NH3 uptake capacity of Rh-MOPs. Rh-MOPs can be regenerated through their immersion in acidic water, and upon activation, their ammonia uptake can be recovered for at least three cycles. Our findings demonstrate that MOPs can be used as porous hosts to capture corrosive molecules like ammonia, and that their surface functionalization can enhance the ammonia uptake performance.Peer reviewedFigshareCarné-Sánchez, Arnau [arnau.carne@icn2.cat]Maspoch, Daniel [daniel.maspoch@icn2.cat]Consejo Superior de Investigaciones Científicas [https://ror.org/02gfc7t72]202320232023info:eu-repo/semantics/datasethttp://purl.org/coar/resource_type/c_ddb1application/pdfhttp://hdl.handle.net/10261/336232reponame:DIGITAL.CSIC. Repositorio Institucional del CSICinstname:Consejo Superior de Investigaciones Científicas (CSIC)InglésCarné-Sánchez, Arnau; Martínez Esaín, Jordi; Rookard, Tanner; Flood, Christopher J.; Faraudo, Jordi; Stylianou, Kyriakos C.; Maspoch, Daniel. Ammonia Capture in Rhodium(II)-Based Metal-Organic Polyhedra via Synergistic Coordinative and H-Bonding Interactions. https://doi.org/10.1021/acsami.2c19206. http://hdl.handle.net/10261/336065https://doi.org/10.1021/acsami.2c19206.s001Síinfo:eu-repo/semantics/openAccessoai:digital.csic.es:10261/3362322026-05-22T06:33:51Z
score 15,811543

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