Elucidation of Molecular-level Mechanisms of Oxygen Atom Reactions with Chlorine Ion in NaCl Solutions using Molecular Dynamics Simulations Combined with Density Functional Theory

Kód výsledku v IS VaVaI

<a href="https://www.isvavai.cz/riv?ss=detail&h=RIV%2F61389021%3A_____%2F23%3A00578063" target="_blank" >RIV/61389021:_____/23:00578063 - isvavai.cz</a>

Výsledek na webu

<a href="https://chemistry-europe.onlinelibrary.wiley.com/doi/10.1002/slct.202203937" target="_blank" >https://chemistry-europe.onlinelibrary.wiley.com/doi/10.1002/slct.202203937</a>

DOI - Digital Object Identifier

<a href="http://dx.doi.org/10.1002/slct.202203937" target="_blank" >10.1002/slct.202203937</a>

Jazyk výsledku

angličtina

Název v původním jazyce

Elucidation of Molecular-level Mechanisms of Oxygen Atom Reactions with Chlorine Ion in NaCl Solutions using Molecular Dynamics Simulations Combined with Density Functional Theory

Popis výsledku v původním jazyce

Molecular dynamics simulations combined with density functional theory were performed to investigate the reaction mechanisms for oxygen atom and chlorine ion in NaCl solutions. Considering the ground and first excited states of the oxygen atom, four bulk systems, O(3P)-NaCl-63H2O, O(1D)-NaCl-63H2O, O(3P)-4NaCl-63H2O, and O(1D)-4NaCl-63H2O were studied. The main reaction pathway depended on the concentration of the aqueous electrolyte solution. For a dilute solution with a 1 : 64 ratio of NaCl to H2O, the singlet oxygen atom first attached a water molecule to produce a neutral OH radical, and then the OH radical and chlorine ion approach each other to form an intermediate structure [Cl…OH]−. Synchronously, the intermediate transferred charge to the solvated OH radical by accessing the hydrogen bond network. Finally, neutral HOCl and OH− ions were formed. For a dense solution with a 4 : 64 ratio of NaCl to H2O, a singlet oxygen atom was directly combined with Cl− to produce ClO− via an oxygen transfer reaction. The subsequent ab-initio energy computations indicated the most probable mechanism, where the O atom directly combines with Cl− ion to OCl−. This study provides insights into the fundamental mechanisms of the behavior of dissolved oxygen radicals in aqueous electrolyte solutions.

Název v anglickém jazyce

Elucidation of Molecular-level Mechanisms of Oxygen Atom Reactions with Chlorine Ion in NaCl Solutions using Molecular Dynamics Simulations Combined with Density Functional Theory

Popis výsledku anglicky

Molecular dynamics simulations combined with density functional theory were performed to investigate the reaction mechanisms for oxygen atom and chlorine ion in NaCl solutions. Considering the ground and first excited states of the oxygen atom, four bulk systems, O(3P)-NaCl-63H2O, O(1D)-NaCl-63H2O, O(3P)-4NaCl-63H2O, and O(1D)-4NaCl-63H2O were studied. The main reaction pathway depended on the concentration of the aqueous electrolyte solution. For a dilute solution with a 1 : 64 ratio of NaCl to H2O, the singlet oxygen atom first attached a water molecule to produce a neutral OH radical, and then the OH radical and chlorine ion approach each other to form an intermediate structure [Cl…OH]−. Synchronously, the intermediate transferred charge to the solvated OH radical by accessing the hydrogen bond network. Finally, neutral HOCl and OH− ions were formed. For a dense solution with a 4 : 64 ratio of NaCl to H2O, a singlet oxygen atom was directly combined with Cl− to produce ClO− via an oxygen transfer reaction. The subsequent ab-initio energy computations indicated the most probable mechanism, where the O atom directly combines with Cl− ion to OCl−. This study provides insights into the fundamental mechanisms of the behavior of dissolved oxygen radicals in aqueous electrolyte solutions.

Druh

J_imp - Článek v periodiku v databázi Web of Science

CEP obor

—

OECD FORD obor

10305 - Fluids and plasma physics (including surface physics)

Projekt

<a href="/cs/project/GA19-25026S" target="_blank" >GA19-25026S: Charakterizace chemicky reaktivních kapalin produkovaných nerovnovážným plazmatem</a><br>

Návaznosti

I - Institucionalni podpora na dlouhodoby koncepcni rozvoj vyzkumne organizace

Rok uplatnění

2023

Kód důvěrnosti údajů

S - Úplné a pravdivé údaje o projektu nepodléhají ochraně podle zvláštních právních předpisů

Název periodika

ChemistrySelect

ISSN

2365-6549

e-ISSN

2365-6549

Svazek periodika

8

Číslo periodika v rámci svazku

23

Stát vydavatele periodika

US - Spojené státy americké

Počet stran výsledku

7

Strana od-do

e202203937

Kód UT WoS článku

001005867000001

EID výsledku v databázi Scopus

2-s2.0-85162141445