{"title":"Solvent-free CO2 cycloaddition by one- and two-dimensional sodium coordination polymers based on hydrazonic ligands","authors":"","doi":"10.1016/j.jssc.2024.124973","DOIUrl":null,"url":null,"abstract":"<div><p>We successfully synthesized and characterized four new coordination polymers of sodium: sodium 4-hydroxy-3-{[2-(pyridine-4-carbonyl)hydrazinylidene]methyl}benzene-1-sulfonate (<strong>NaL</strong><sup><strong>4-Py</strong></sup>), sodium 3-[(2-benzoylhydrazinylidene)methyl]-4-hydroxybenzene-1-sulfonate (<strong>NaL</strong><sup><strong>Ph</strong></sup>), sodium 3-[(2-acetylhydrazinylidene)methyl]-4-hydroxybenzene-1-sulfonate (<strong>NaL</strong><sup><strong>Me</strong></sup>), and sodium 3-[(2-carbamoylhydrazinylidene)methyl]-4-hydroxybenzene-1-sulfonate (<strong>NaL</strong><sup><strong>NH2</strong></sup>). These polymers were synthesized through a 1:1 condensation reaction of hydrazide derivatives with sodium salicylaldehyde-5-sulfonate monohydrate (NaSalSO<sub>3</sub>) and were thoroughly characterized using various analytical techniques. The compounds <strong>NaL</strong><sup><strong>Me</strong></sup> and <strong>NaL</strong><sup><strong>Ph</strong></sup>, crystallized in the P <span><math><mrow><mover><mn>1</mn><mo>‾</mo></mover></mrow></math></span> and P2<sub>1</sub>/n space groups, respectively, forming one-dimensional polymers. On the other hand, <strong>NaL</strong><sup><strong>NH2</strong></sup> and <strong>NaL</strong><sup><strong>4-Py</strong></sup> crystallized in the <em>Cmca</em> and P <span><math><mrow><mover><mn>1</mn><mo>‾</mo></mover></mrow></math></span> space groups, respectively, forming two-dimensional coordination polymers. The coordination environment of the sodium cation differed among the compounds, with the imine nitrogen atom interfering in <strong>NaL</strong><sup><strong>4-Py</strong></sup> and <strong>NaL</strong><sup><strong>Ph</strong></sup>. The sulfonate group exhibited various coordination modes, resulting in the different dimensionalities of the polymers. Compounds <strong>NaL</strong><sup><strong>4-Py</strong></sup> and <strong>NaL</strong><sup><strong>Ph</strong></sup> acted as heterogeneous Lewis acid catalysts for the solvent-free cycloaddition reaction of epichlorohydrine and CO<sub>2</sub> into valued cyclic carbonate. High selective conversion (68 %) of epichlorohydrin to cyclic carbonate was obtained at mild conditions, 60 °C and 1 bar CO<sub>2</sub>, after 24 h of reaction.</p></div>","PeriodicalId":378,"journal":{"name":"Journal of Solid State Chemistry","volume":null,"pages":null},"PeriodicalIF":3.2000,"publicationDate":"2024-08-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of Solid State Chemistry","FirstCategoryId":"92","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S0022459624004274","RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, INORGANIC & NUCLEAR","Score":null,"Total":0}
引用次数: 0
Abstract
We successfully synthesized and characterized four new coordination polymers of sodium: sodium 4-hydroxy-3-{[2-(pyridine-4-carbonyl)hydrazinylidene]methyl}benzene-1-sulfonate (NaL4-Py), sodium 3-[(2-benzoylhydrazinylidene)methyl]-4-hydroxybenzene-1-sulfonate (NaLPh), sodium 3-[(2-acetylhydrazinylidene)methyl]-4-hydroxybenzene-1-sulfonate (NaLMe), and sodium 3-[(2-carbamoylhydrazinylidene)methyl]-4-hydroxybenzene-1-sulfonate (NaLNH2). These polymers were synthesized through a 1:1 condensation reaction of hydrazide derivatives with sodium salicylaldehyde-5-sulfonate monohydrate (NaSalSO3) and were thoroughly characterized using various analytical techniques. The compounds NaLMe and NaLPh, crystallized in the P and P21/n space groups, respectively, forming one-dimensional polymers. On the other hand, NaLNH2 and NaL4-Py crystallized in the Cmca and P space groups, respectively, forming two-dimensional coordination polymers. The coordination environment of the sodium cation differed among the compounds, with the imine nitrogen atom interfering in NaL4-Py and NaLPh. The sulfonate group exhibited various coordination modes, resulting in the different dimensionalities of the polymers. Compounds NaL4-Py and NaLPh acted as heterogeneous Lewis acid catalysts for the solvent-free cycloaddition reaction of epichlorohydrine and CO2 into valued cyclic carbonate. High selective conversion (68 %) of epichlorohydrin to cyclic carbonate was obtained at mild conditions, 60 °C and 1 bar CO2, after 24 h of reaction.
期刊介绍:
Covering major developments in the field of solid state chemistry and related areas such as ceramics and amorphous materials, the Journal of Solid State Chemistry features studies of chemical, structural, thermodynamic, electronic, magnetic, and optical properties and processes in solids.