Nazir Ud Din Mir, Subhrajyoti Ghosh, Kalimuthu Abirami Sundari, Amarajothi Dhakshinamoorthy and Shyam Biswas*,
{"title":"一个功能化Al(III)金属-有机框架的策略设计,用于环境条件下炔内CO2的化学固定和合成具有重要生物学意义的杂环","authors":"Nazir Ud Din Mir, Subhrajyoti Ghosh, Kalimuthu Abirami Sundari, Amarajothi Dhakshinamoorthy and Shyam Biswas*, ","doi":"10.1021/acs.inorgchem.5c0084110.1021/acs.inorgchem.5c00841","DOIUrl":null,"url":null,"abstract":"<p >The increasing impact of elevated atmospheric CO<sub>2</sub> levels on climate and biological systems underscores the urgent need for effective materials to mitigate these concentrations. Simultaneously, the demand for quinoline derivatives has risen sharply due to their critical role in synthesizing life-saving drugs. Here, we present the synthesis, characterization, and catalytic activity of an aqua-stable Al(III) metal–organic framework (MOF <b>1′</b>) and its postmodified variant doped with Ag(0) nanoparticles (<b>1′</b>-Ag NPs). The native MOF (<b>1′</b>) and its nanoparticle-anchored derivative exhibited remarkable efficacy in two key areas: the quantitative synthesis of quinoline heterocycles and irreversible chemical fixation of CO<sub>2</sub> into various alkynes. Under ambient temperature and atmospheric CO<sub>2</sub> pressure, <b>1′</b>-Ag NPs demonstrated exceptional catalytic performance for the cyclization of propargylic alcohols. Moreover, the catalysts exhibited excellent recyclability across multiple reusability cycles. Detailed control experiments revealed that the outstanding performance of <b>1′</b> and <b>1′</b>-Ag NPs stems from the anchored functional groups within <b>1′</b> and the highly exposed alkalophilic Ag(0) catalytic sites distributed along the surface of <b>1′</b>-Ag NPs. This study highlights the dual utility of <b>1′</b> and <b>1′</b>-Ag NPs, demonstrating their potential in both the selective synthesis of quinoline heterocycles and the environmentally sustainable capture and irreversible chemical conversion of CO<sub>2</sub> under mild conditions.</p>","PeriodicalId":40,"journal":{"name":"Inorganic Chemistry","volume":"64 16","pages":"8386–8396 8386–8396"},"PeriodicalIF":4.7000,"publicationDate":"2025-04-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Strategic Design of a Functionalized Al(III) Metal–Organic Framework for Chemical Fixation of CO2 inside Alkynes under Ambient Conditions and Synthesis of Biologically Important Heterocycles\",\"authors\":\"Nazir Ud Din Mir, Subhrajyoti Ghosh, Kalimuthu Abirami Sundari, Amarajothi Dhakshinamoorthy and Shyam Biswas*, \",\"doi\":\"10.1021/acs.inorgchem.5c0084110.1021/acs.inorgchem.5c00841\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p >The increasing impact of elevated atmospheric CO<sub>2</sub> levels on climate and biological systems underscores the urgent need for effective materials to mitigate these concentrations. Simultaneously, the demand for quinoline derivatives has risen sharply due to their critical role in synthesizing life-saving drugs. Here, we present the synthesis, characterization, and catalytic activity of an aqua-stable Al(III) metal–organic framework (MOF <b>1′</b>) and its postmodified variant doped with Ag(0) nanoparticles (<b>1′</b>-Ag NPs). The native MOF (<b>1′</b>) and its nanoparticle-anchored derivative exhibited remarkable efficacy in two key areas: the quantitative synthesis of quinoline heterocycles and irreversible chemical fixation of CO<sub>2</sub> into various alkynes. Under ambient temperature and atmospheric CO<sub>2</sub> pressure, <b>1′</b>-Ag NPs demonstrated exceptional catalytic performance for the cyclization of propargylic alcohols. Moreover, the catalysts exhibited excellent recyclability across multiple reusability cycles. Detailed control experiments revealed that the outstanding performance of <b>1′</b> and <b>1′</b>-Ag NPs stems from the anchored functional groups within <b>1′</b> and the highly exposed alkalophilic Ag(0) catalytic sites distributed along the surface of <b>1′</b>-Ag NPs. This study highlights the dual utility of <b>1′</b> and <b>1′</b>-Ag NPs, demonstrating their potential in both the selective synthesis of quinoline heterocycles and the environmentally sustainable capture and irreversible chemical conversion of CO<sub>2</sub> under mild conditions.</p>\",\"PeriodicalId\":40,\"journal\":{\"name\":\"Inorganic Chemistry\",\"volume\":\"64 16\",\"pages\":\"8386–8396 8386–8396\"},\"PeriodicalIF\":4.7000,\"publicationDate\":\"2025-04-15\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Inorganic Chemistry\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://pubs.acs.org/doi/10.1021/acs.inorgchem.5c00841\",\"RegionNum\":2,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, INORGANIC & NUCLEAR\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Inorganic Chemistry","FirstCategoryId":"92","ListUrlMain":"https://pubs.acs.org/doi/10.1021/acs.inorgchem.5c00841","RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, INORGANIC & NUCLEAR","Score":null,"Total":0}
Strategic Design of a Functionalized Al(III) Metal–Organic Framework for Chemical Fixation of CO2 inside Alkynes under Ambient Conditions and Synthesis of Biologically Important Heterocycles
The increasing impact of elevated atmospheric CO2 levels on climate and biological systems underscores the urgent need for effective materials to mitigate these concentrations. Simultaneously, the demand for quinoline derivatives has risen sharply due to their critical role in synthesizing life-saving drugs. Here, we present the synthesis, characterization, and catalytic activity of an aqua-stable Al(III) metal–organic framework (MOF 1′) and its postmodified variant doped with Ag(0) nanoparticles (1′-Ag NPs). The native MOF (1′) and its nanoparticle-anchored derivative exhibited remarkable efficacy in two key areas: the quantitative synthesis of quinoline heterocycles and irreversible chemical fixation of CO2 into various alkynes. Under ambient temperature and atmospheric CO2 pressure, 1′-Ag NPs demonstrated exceptional catalytic performance for the cyclization of propargylic alcohols. Moreover, the catalysts exhibited excellent recyclability across multiple reusability cycles. Detailed control experiments revealed that the outstanding performance of 1′ and 1′-Ag NPs stems from the anchored functional groups within 1′ and the highly exposed alkalophilic Ag(0) catalytic sites distributed along the surface of 1′-Ag NPs. This study highlights the dual utility of 1′ and 1′-Ag NPs, demonstrating their potential in both the selective synthesis of quinoline heterocycles and the environmentally sustainable capture and irreversible chemical conversion of CO2 under mild conditions.
期刊介绍:
Inorganic Chemistry publishes fundamental studies in all phases of inorganic chemistry. Coverage includes experimental and theoretical reports on quantitative studies of structure and thermodynamics, kinetics, mechanisms of inorganic reactions, bioinorganic chemistry, and relevant aspects of organometallic chemistry, solid-state phenomena, and chemical bonding theory. Emphasis is placed on the synthesis, structure, thermodynamics, reactivity, spectroscopy, and bonding properties of significant new and known compounds.