{"title":"Kinetic-mechanistic studies of ruthenium macrocyclic complexes formation as potential donors and scavengers of nitric oxide and correlated species","authors":"Juliana Guerreiro Cezar, Tamires Mariel Muniz Milhazes, Kleber Queiroz Ferreira","doi":"10.1007/s11243-024-00575-w","DOIUrl":null,"url":null,"abstract":"<div><p>In this paper, the mechanisms of reactions involving complexes with tetraazamacrocyclic (mac) ligands against nitrosyl ligands in an aqueous medium were explored, with emphasis on reactivity to nitric oxide (NO) and analog species, like nitrite ion (NO<sub>2</sub><sup>−</sup>). The reactions between [RuCl(OH<sub>2</sub>)(mac)]<sup>2+</sup> with NO and [RuCl(OH)(mac)]<sup>2+</sup> with NO<sub>2</sub><sup>−</sup> were performed in an aqueous solution within pH 1 or 7, and the rate constants (<i>k</i>) and the thermodynamic parameters (∆<i>H</i><sup>#</sup>, ∆<i>S</i><sup>#</sup>) of activation were determined. The reaction between NO and the complex with cyclen is faster than that with the complex with cyclam. However, the reaction of the cyclen complex with NO<sub>2</sub><sup>−</sup> is slower than NO. This research provides detailed reaction kinetics and thermodynamic activation parameters for these interactions for the first time. In addition, the redox processes of coordinated NO<sup>−</sup> and NO<sub>2</sub><sup>−</sup> ligands to ruthenium were evaluated and the electrochemical release of NO from nitrosyl compounds upon electrochemical potential application. Our findings bring significant contributions in elucidating mechanisms related to NO capture both in vitro and in vivo.</p><h3>Graphical Abstract</h3>\n<div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":1,"journal":{"name":"Accounts of Chemical Research","volume":null,"pages":null},"PeriodicalIF":16.4000,"publicationDate":"2024-03-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Accounts of Chemical Research","FirstCategoryId":"92","ListUrlMain":"https://link.springer.com/article/10.1007/s11243-024-00575-w","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
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Abstract
In this paper, the mechanisms of reactions involving complexes with tetraazamacrocyclic (mac) ligands against nitrosyl ligands in an aqueous medium were explored, with emphasis on reactivity to nitric oxide (NO) and analog species, like nitrite ion (NO2−). The reactions between [RuCl(OH2)(mac)]2+ with NO and [RuCl(OH)(mac)]2+ with NO2− were performed in an aqueous solution within pH 1 or 7, and the rate constants (k) and the thermodynamic parameters (∆H#, ∆S#) of activation were determined. The reaction between NO and the complex with cyclen is faster than that with the complex with cyclam. However, the reaction of the cyclen complex with NO2− is slower than NO. This research provides detailed reaction kinetics and thermodynamic activation parameters for these interactions for the first time. In addition, the redox processes of coordinated NO− and NO2− ligands to ruthenium were evaluated and the electrochemical release of NO from nitrosyl compounds upon electrochemical potential application. Our findings bring significant contributions in elucidating mechanisms related to NO capture both in vitro and in vivo.
期刊介绍：
Accounts of Chemical Research presents short, concise and critical articles offering easy-to-read overviews of basic research and applications in all areas of chemistry and biochemistry. These short reviews focus on research from the author’s own laboratory and are designed to teach the reader about a research project. In addition, Accounts of Chemical Research publishes commentaries that give an informed opinion on a current research problem. Special Issues online are devoted to a single topic of unusual activity and significance.
Accounts of Chemical Research replaces the traditional article abstract with an article "Conspectus." These entries synopsize the research affording the reader a closer look at the content and significance of an article. Through this provision of a more detailed description of the article contents, the Conspectus enhances the article's discoverability by search engines and the exposure for the research.
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