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Inequivalent Solvation Effects on the N 1s Levels of Self-Associated Melamine Molecules in Aqueous Solution
[Image: see text] This work shows how the N 1s photoemission (PE) spectrum of self-associated melamine molecules in aqueous solution has been successfully rationalized using an integrated computational approach encompassing classical metadynamics simulations and quantum calculations based on density...
Autores principales: | , , , , , , , , , , |
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Formato: | Online Artículo Texto |
Lenguaje: | English |
Publicado: |
American Chemical Society
2023
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Acceso en línea: | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10084451/ https://www.ncbi.nlm.nih.gov/pubmed/36972466 http://dx.doi.org/10.1021/acs.jpcb.3c00327 |
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author | Ponzi, Aurora Rosa, Marta Kladnik, Gregor Unger, Isaak Ciavardini, Alessandra Di Nardi, Lorys Viola, Elisa Nicolas, Christophe Došlić, Nađa Goldoni, Andrea Lanzilotto, Valeria |
author_facet | Ponzi, Aurora Rosa, Marta Kladnik, Gregor Unger, Isaak Ciavardini, Alessandra Di Nardi, Lorys Viola, Elisa Nicolas, Christophe Došlić, Nađa Goldoni, Andrea Lanzilotto, Valeria |
author_sort | Ponzi, Aurora |
collection | PubMed |
description | [Image: see text] This work shows how the N 1s photoemission (PE) spectrum of self-associated melamine molecules in aqueous solution has been successfully rationalized using an integrated computational approach encompassing classical metadynamics simulations and quantum calculations based on density functional theory (DFT). The first approach allowed us to describe interacting melamine molecules in explicit waters and to identify dimeric configurations based on π–π and/or H-bonding interactions. Then, N 1s binding energies (BEs) and PE spectra were computed at the DFT level for all structures both in the gas phase and in an implicit solvent. While pure π-stacked dimers show gas-phase PE spectra almost identical to that of the monomer, those of the H-bonded dimers are sensibly affected by NH···NH or NH···NC interactions. Interestingly, the solvation suppresses all of the non-equivalences due to the H-bonds yielding similar PE spectra for all dimers, matching very well our measurements. |
format | Online Article Text |
id | pubmed-10084451 |
institution | National Center for Biotechnology Information |
language | English |
publishDate | 2023 |
publisher | American Chemical Society |
record_format | MEDLINE/PubMed |
spelling | pubmed-100844512023-04-11 Inequivalent Solvation Effects on the N 1s Levels of Self-Associated Melamine Molecules in Aqueous Solution Ponzi, Aurora Rosa, Marta Kladnik, Gregor Unger, Isaak Ciavardini, Alessandra Di Nardi, Lorys Viola, Elisa Nicolas, Christophe Došlić, Nađa Goldoni, Andrea Lanzilotto, Valeria J Phys Chem B [Image: see text] This work shows how the N 1s photoemission (PE) spectrum of self-associated melamine molecules in aqueous solution has been successfully rationalized using an integrated computational approach encompassing classical metadynamics simulations and quantum calculations based on density functional theory (DFT). The first approach allowed us to describe interacting melamine molecules in explicit waters and to identify dimeric configurations based on π–π and/or H-bonding interactions. Then, N 1s binding energies (BEs) and PE spectra were computed at the DFT level for all structures both in the gas phase and in an implicit solvent. While pure π-stacked dimers show gas-phase PE spectra almost identical to that of the monomer, those of the H-bonded dimers are sensibly affected by NH···NH or NH···NC interactions. Interestingly, the solvation suppresses all of the non-equivalences due to the H-bonds yielding similar PE spectra for all dimers, matching very well our measurements. American Chemical Society 2023-03-27 /pmc/articles/PMC10084451/ /pubmed/36972466 http://dx.doi.org/10.1021/acs.jpcb.3c00327 Text en © 2023 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 | Ponzi, Aurora Rosa, Marta Kladnik, Gregor Unger, Isaak Ciavardini, Alessandra Di Nardi, Lorys Viola, Elisa Nicolas, Christophe Došlić, Nađa Goldoni, Andrea Lanzilotto, Valeria Inequivalent Solvation Effects on the N 1s Levels of Self-Associated Melamine Molecules in Aqueous Solution |
title | Inequivalent Solvation
Effects on the N 1s Levels
of Self-Associated Melamine Molecules in Aqueous Solution |
title_full | Inequivalent Solvation
Effects on the N 1s Levels
of Self-Associated Melamine Molecules in Aqueous Solution |
title_fullStr | Inequivalent Solvation
Effects on the N 1s Levels
of Self-Associated Melamine Molecules in Aqueous Solution |
title_full_unstemmed | Inequivalent Solvation
Effects on the N 1s Levels
of Self-Associated Melamine Molecules in Aqueous Solution |
title_short | Inequivalent Solvation
Effects on the N 1s Levels
of Self-Associated Melamine Molecules in Aqueous Solution |
title_sort | inequivalent solvation
effects on the n 1s levels
of self-associated melamine molecules in aqueous solution |
url | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10084451/ https://www.ncbi.nlm.nih.gov/pubmed/36972466 http://dx.doi.org/10.1021/acs.jpcb.3c00327 |
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