Direct observation of the complex S(IV) equilibria at the liquid-vapor interface.


Journal

Nature communications
ISSN: 2041-1723
Titre abrégé: Nat Commun
Pays: England
ID NLM: 101528555

Informations de publication

Date de publication:
18 Oct 2024
Historique:
received: 07 06 2024
accepted: 04 10 2024
medline: 18 10 2024
pubmed: 18 10 2024
entrez: 17 10 2024
Statut: epublish

Résumé

The multi-phase oxidation of S(IV) plays a crucial role in the atmosphere, leading to the formation of haze and severe pollution episodes. We here contribute to its understanding on a molecular level by reporting experimentally determined pK

Identifiants

pubmed: 39420175
doi: 10.1038/s41467-024-53186-5
pii: 10.1038/s41467-024-53186-5
doi:

Types de publication

Journal Article

Langues

eng

Sous-ensembles de citation

IM

Pagination

8987

Informations de copyright

© 2024. The Author(s).

Références

Seinfeld, J. H. & Pandis, S. N. Atmospheric Chemistry and Physics: From Air Pollution to Climate Change (Wiley & Sons, Inc., John, 2016).
Tilgner, A. et al. Acidity and the multiphase chemistry of atmospheric aqueous particles and clouds. Atmos. Chem. Phys. 21, 13483–13536 (2021).
doi: 10.5194/acp-21-13483-2021
Holleman, A. F., Wiberg, N., Wiberg, E. & Fischer, G. Lehrbuch der Anorganischen Chemie https://doi.org/10.1515/9783110177701 (Walter de Gruyter, 2007).
Hoffmann, E. H., Tilgner, A., Vogelsang, U., Wolke, H. & Herrmann, R. Near-explicit multiphase modeling of halogen chemistry in a mixed urban and maritime coastal area. ACS Earth Space Chem. 3, 2452–2471 (2019).
doi: 10.1021/acsearthspacechem.9b00184
Cheng, Y. et al. Reactive nitrogen chemistry in aerosol water as a source of sulfate during haze events in China. Sci. Adv. 2, e1601530 (2016).
pubmed: 28028539 pmcid: 5176349 doi: 10.1126/sciadv.1601530
Yang, J. et al. Unraveling a New Chemical Mechanism of Missing Sulfate formation in Aerosol Haze: Gaseous NO
Liu, T., Clegg, S. L. & Abbatt, J. P. D. Fast oxidation of sulfur dioxide by hydrogen peroxide in deliquesced aerosol particles. Proc. Natl. Acad. Sci. USA 117, 1354–1359 (2020).
pubmed: 31900361 pmcid: 6983387 doi: 10.1073/pnas.1916401117
Liu, T. & Abbatt, J. P. D. Oxidation of sulfur dioxide by nitrogen dioxide accelerated at the interface of deliquesced aerosol particles. Nat. Chem. 13, 1173–1177 (2021).
doi: 10.1038/s41557-021-00777-0
Gladich, I., Lin, C., Sinopoli, A. & Francisco, J. S. Uptake and hydration of sulfur dioxide on dry and wet hydroxylated silica surfaces: a computational study. Phys. Chem. Chem. Phys. 24, 172–179 (2022).
doi: 10.1039/D1CP04747G
Ammann, M. et al. Evaluated kinetic and photochemical data for atmospheric chemistry: Volume VI—heterogeneous reactions with liquid substrates. Atmos. Chem. Phys. 13, 8045–8228 (2013).
doi: 10.5194/acp-13-8045-2013
Jayne, J. T., Davidovits, P., Worsnop, D. R. & Kolb, C. E. Uptake of sulfur dioxide(g) by aqueous surfaces as a function of pH: the effect of chemical reaction at the interface. J. Phys. Chem. A 94, 6041–6048 (1990).
doi: 10.1021/j100378a076
Boniface, J. et al. Uptake of Gas-phase SO
doi: 10.1021/jp000479h
Donaldson, D. J., Guest, J. A. & Goh, M. C. Evidence for Adsorbed SO
doi: 10.1021/j100023a002
Tarbuck, T. L. & Richmond, G. L. SO
pubmed: 16316225 doi: 10.1021/ja056478q
Tarbuck, T. L. & Richmond, G. L. Adsorption and Reaction of CO
pubmed: 16522107 doi: 10.1021/ja057375a
Group, I. T. Kinetic and Photochemical Data. IUPAC Task Group, https://iupac.aeris-data.fr/en/home-english/ .
Voegele, A. F. et al. About the Stability of Sulfurous Acid (H
pubmed: 12693045 doi: 10.1002/1521-3765(20021216)8:24<5644::AID-CHEM5644>3.0.CO;2-9
Guthrie, J. P. Tautomeric equilibria and pKa values for ’sulfurous acid’ in aqueous solution: a thermodynamic analysis. Can. J. Chem. 57, 454–457 (1979).
doi: 10.1139/v79-074
Horner, D. A. & Connick, R. E. Equilibrium quotient for the isomerization of bisulfite ion from [Formula: see text] to SO
doi: 10.1021/ic00234a026
Eldridge, D. L., Mysen, B. O. & Cody, G. D. Experimental estimation of the bisulfite isomer quotient as a function of temperature: Implications for sulfur isotope fractionations in aqueous sulfite solutions. Geochim. Cosmochim. Acta 220, 309–328 (2018).
doi: 10.1016/j.gca.2017.10.005
Risberg, E. D. et al. Sulfur X-ray Absorption and Vibrational Spectroscopic Study of Sulfur Dioxide, Sulfite, and Sulfonate Solutions and of the Substituted Sulfonate Ions [Formula: see text] (X = H, Cl, F). Inorg. Chem. 46, 8332–8348 (2007).
Prisle, N. L. et al. Surface/bulk partitioning and acid/base speciation of aqueous decanoate: direct observations and atmospheric implications. Atmos. Chem. Phys. 12, 12227–12242 (2012).
doi: 10.5194/acp-12-12227-2012
Wellen, B. A., Lach, E. A. & Allen, H. C. Surface pK
pubmed: 28825425 doi: 10.1039/C7CP04527A
Jungwirth, P. & Tobias, D. J. Specific Ion Effects at the Air/Water Interface. Chem. Rev. 106, 1259–1281 (2006).
pubmed: 16608180 doi: 10.1021/cr0403741
Ghosal, S. et al. Electron Spectroscopy of Aqueous Solution Interfaces Reveals Surface Enhancement of Halides. Science 307, 563–566 (2005).
pubmed: 15681380 doi: 10.1126/science.1106525
Thürmer, S. et al. Accurate vertical ionization energy and work function determinations of liquid water and aqueous solutions. Chem. Sci. 12, 10558–10582 (2021).
pubmed: 34447550 pmcid: 8356740 doi: 10.1039/D1SC01908B
Wilhelm, J., Golze, D., Talirz, L., Hutter, J. & Pignedoli, C. A. Toward GW Calculations on Thousands of Atoms. J. Phys. Chem. Lett. 9, 306–312 (2018).
pubmed: 29280376 doi: 10.1021/acs.jpclett.7b02740
Li, J. Jin, Y., Rinke, P., Yang, W. & Golze, D. Benchmark of GW Methods for Core-level Binding Energies. J. Chem. Theory Comput. 18, 7570–7585 (2022).
pubmed: 36322136 pmcid: 9753590 doi: 10.1021/acs.jctc.2c00617
Shigeta, Y., Ferreira, A. M., Zakrzewski, V. G. & Ortiz, J. V. Electron propagator calculations with Kohn-Sham reference states. Int. J. Quantum Chem. 85, 411–420 (2001).
doi: 10.1002/qua.1543
Martins-Costa, M. T. C., Anglada, J. M., Francisco, J. S. & Ruiz-López, M. F. Photochemistry of SO
pubmed: 30226769 doi: 10.1021/jacs.8b07845
Roy, S., Baer, M. D., Mundy, C. J. & Schenter, G. K. Marcus Theory of Ion-pairing. J. Chem. Theory Comput. 13, 3470–3477 (2017).
pubmed: 28715638 doi: 10.1021/acs.jctc.7b00332
Voegele, A. F., Tautermann, C. S., Rauch, C., Loerting, T. & Klaus, R. L. On the Formation of the Sulfonate Ion from Hydrated Sulfur Dioxide. J. Phys. Chem. A 108, 3859–3864 (2004).
doi: 10.1021/jp0377578
Werner, J. et al. Shifted equilibria of organic acids and bases in the aqueous surface region. Phys. Chem. Chem. Phys. 20, 23281–23293 (2018).
pubmed: 30191936 pmcid: 6146375 doi: 10.1039/C8CP01898G
Bunting, J. W. & Kanter, J. P. Acidity and Tautomerism of ß-keto Esters and Amides in Aqueous Solution. J. Am. Chem. Soc. 115, 11705–11715 (1993).
doi: 10.1021/ja00078a008
Hoffmann, M. R. On the Kinetics and Mechanism of Oxidation of Aquated Sulfur Dioxide by Ozone. Atmos. Environ. 20, 1145–1154 (1986).
doi: 10.1016/0004-6981(86)90147-2
Kahan, T. F., Ardura, D. & Donaldson, D. J. Mechanism of Aqueous-phase Ozonation of S(iv). J. Phys. Chem. A 114, 2164–2170 (2010).
pubmed: 20085262 doi: 10.1021/jp9085156
Viefhaus, J. et al. The Variable Polarization XUV Beamline P04 at PETRA III: Optics, Mechanics and their Performance. Nucl. Instrum. Methods Phys. Res. Sect. A 710, 151–154 (2013).
doi: 10.1016/j.nima.2012.10.110
Malerz, S. et al. A setup for studies of photoelectron circular dichroism from chiral molecules in aqueous solution. Rev. Sci. Instrum. 93, 015101 (2022).
doi: 10.1063/5.0072346
Malerz, S. et al. Low-energy constraints on photoelectron spectra measured from liquid water and aqueous solutions. Phys. Chem. Chem. Phys. 23, 8246–8260 (2021).
pubmed: 33710216 doi: 10.1039/D1CP00430A
Brown, M. A. et al. A new Endstation at the Swiss Light Source for Ultraviolet Photoelectron Spectroscopy, X-ray photoelectron spectroscopy, and X-ray absorption spectroscopy measurements of Liquid Solutions. Rev. Sci. Instrum. 84, 073904 (2013).
Margarella, A. M. et al. Dissociation of Sulfuric Acid in Aqueous Solution: Determination of the Photoelectron Spectral Fingerprints of H
doi: 10.1021/jp308090k
Jämbeck, J. P. M. & Lyubartsev, A. P. Update to the General Amber Force Field for Small Solutes with an Emphasis on Free Energies of Hydration. J. Phys. Chem. B 118, 3793–3804 (2014).
pubmed: 24684585 doi: 10.1021/jp4111234
Jorgensen, W. L., Chandrasekhar, J., Madura, J. D., Impey, R. W. & Klein, M. L. Comparison of simple potential functions for simulating liquid water. J. Chem. Phys. 79, 926–935 (1983).
doi: 10.1063/1.445869
Leontyev, I. & Stuchebrukhov, A. Accounting for electronic polarization in non-polarizable force fields. Phys. Chem. Chem. Phys. 13, 2613–2626 (2011).
pubmed: 21212894 doi: 10.1039/c0cp01971b
Kühne, T. D. et al. CP2K: an electronic structure and molecular dynamics software package—Quickstep: efficient and accurate electronic structure calculations. J. Chem. Phys. 152, 194103 (2020).
pubmed: 33687235 doi: 10.1063/5.0007045
Perdew, J. P., Burke, K. & Ernzerhof, M. Generalized Gradient Approximation made Simple. Phys. Rev. Lett. 77, 3865–3868 (1996).
pubmed: 10062328 doi: 10.1103/PhysRevLett.77.3865
Grimme, S., Antony, J., Ehrlich, S. & Krieg, H. A consistent and accurate ab initio parametrization of density functional dispersion correction (DFT-D) for the 94 elements H-Pu. J. Chem. Phys. 132, 154104 (2010).
doi: 10.1063/1.3382344
Tribello, G. A., Bonomi, M., Branduardi, D., Camilloni, C. & Bussi, G. PLUMED 2: New feathers for an old bird. Comput. Phys. Commun. 185, 604–613 (2014).
doi: 10.1016/j.cpc.2013.09.018
Bussy, A. & Hutter, J. Efficient and low-scaling linear-response time-dependent density functional theory implementation for core-level spectroscopy of large and periodic systems. Phys. Chem. Chem. Phys. 23, 4736–4746 (2021).
pubmed: 33598668 doi: 10.1039/D0CP06164F
Golze, D., Keller, L. & Rinke, P. Accurate absolute and relative core-level binding energies from gw. J. Phys. Chem. Lett. 11, 1840–1847 (2020).
pubmed: 32043890 pmcid: 7735733 doi: 10.1021/acs.jpclett.9b03423
Adamo, C. & Barone, V. Toward reliable density functional methods without adjustable parameters: the PBE0 model. J. Chem. Phys. 110, 6158–6170 (1999).
doi: 10.1063/1.478522
Siggel, M. R. F., Field, C., Sæthre, L. J., Bo/rve, K. J. & Thomas, T. D. High resolution photoelectron spectroscopy of sulfur 2p electrons in the H
doi: 10.1063/1.472761
Yang, H., Gladich, I., Boucly, A., Artiglia, L. & Ammann, M. Orcinol and resorcinol induce local ordering of water molecules near the liquid-vapor interface. Environ. Sci.: Atmos. 2, 1277–1291 (2022).
pubmed: 36561553

Auteurs

Tillmann Buttersack (T)

Fritz Haber Institute of the Max Planck Society, Faradayweg 4-6, 14195, Berlin, Germany. buttersack@fhi.mpg.de.

Ivan Gladich (I)

Qatar Environment and Energy Research Institute, Hamad Bin Khalifa University, P.O. Box 34110, Doha, Qatar. igladich@hbku.edu.qa.

Shirin Gholami (S)

Fritz Haber Institute of the Max Planck Society, Faradayweg 4-6, 14195, Berlin, Germany.

Clemens Richter (C)

Fritz Haber Institute of the Max Planck Society, Faradayweg 4-6, 14195, Berlin, Germany.

Rémi Dupuy (R)

Sorbonne Université, CNRS, Laboratoire de Chimie Physique-Matière et Rayonnement, Paris Cedex 05, F-75005, France.

Christophe Nicolas (C)

Synchrotron SOLEIL, L'Orme des Merisiers, Saint-Aubin-BP 48, 91192, Gif-sur-Yvette, France.

Florian Trinter (F)

Fritz Haber Institute of the Max Planck Society, Faradayweg 4-6, 14195, Berlin, Germany.

Annette Trunschke (A)

Fritz Haber Institute of the Max Planck Society, Faradayweg 4-6, 14195, Berlin, Germany.

Daniel Delgado (D)

Fritz Haber Institute of the Max Planck Society, Faradayweg 4-6, 14195, Berlin, Germany.

Pablo Corral Arroyo (P)

Laboratory of Physical Chemistry, Department of Chemistry and Applied Biosciences, ETH Zürich, Vladimir-Prelog-Weg 2, Zürich, CH-8093, Switzerland.

Evelyne A Parmentier (EA)

Laboratory of Physical Chemistry, Department of Chemistry and Applied Biosciences, ETH Zürich, Vladimir-Prelog-Weg 2, Zürich, CH-8093, Switzerland.

Bernd Winter (B)

Fritz Haber Institute of the Max Planck Society, Faradayweg 4-6, 14195, Berlin, Germany.

Lucia Iezzi (L)

PSI Center for Energy and Environmental Sciences, Paul Scherrer Institute, Villigen PSI, CH-5232, Switzerland.

Antoine Roose (A)

PSI Center for Energy and Environmental Sciences, Paul Scherrer Institute, Villigen PSI, CH-5232, Switzerland.
IMT Nord Europe, Institut Mines-Télécom, University Lille, Lille, F-59000, France.

Anthony Boucly (A)

PSI Center for Energy and Environmental Sciences, Paul Scherrer Institute, Villigen PSI, CH-5232, Switzerland.

Luca Artiglia (L)

PSI Center for Energy and Environmental Sciences, Paul Scherrer Institute, Villigen PSI, CH-5232, Switzerland.

Markus Ammann (M)

PSI Center for Energy and Environmental Sciences, Paul Scherrer Institute, Villigen PSI, CH-5232, Switzerland.

Ruth Signorell (R)

Laboratory of Physical Chemistry, Department of Chemistry and Applied Biosciences, ETH Zürich, Vladimir-Prelog-Weg 2, Zürich, CH-8093, Switzerland.

Hendrik Bluhm (H)

Fritz Haber Institute of the Max Planck Society, Faradayweg 4-6, 14195, Berlin, Germany. bluhm@fhi.mpg.de.

Classifications MeSH