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

IF 4.7 2区 化学 Q1 CHEMISTRY, INORGANIC & NUCLEAR Inorganic Chemistry Pub Date : 2025-04-15 DOI:10.1021/acs.inorgchem.5c00841
Nazir Ud Din Mir, Subhrajyoti Ghosh, Kalimuthu Abirami Sundari, Amarajothi Dhakshinamoorthy, Shyam Biswas
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引用次数: 0

摘要

大气中二氧化碳浓度升高对气候和生物系统的影响越来越大,迫切需要有效的材料来减轻这些浓度。同时,对喹啉衍生物的需求急剧上升,因为它们在合成救命药物中起着关键作用。在这里,我们介绍了一种水稳定的Al(III)金属有机骨架(MOF 1’)及其掺杂Ag(0)纳米粒子(1’-Ag NPs)的后修饰变体的合成、表征和催化活性。天然MOF(1’)及其纳米粒子锚定衍生物在喹啉杂环的定量合成和二氧化碳不可逆化学固定成各种炔烃这两个关键领域表现出显著的功效。在环境温度和大气CO2压力下,1′-Ag NPs对丙炔醇的环化反应表现出优异的催化性能。此外,催化剂在多次重复使用循环中表现出优异的可回收性。详细的对照实验表明,1 ‘和1 ’ -Ag NPs的优异性能源于1 ‘内锚定的官能团和沿1 ’ -Ag NPs表面分布的高度暴露的亲碱性Ag(0)催化位点。本研究强调了1 ‘和1 ’ -Ag NPs的双重用途,展示了它们在选择性合成喹啉杂环和环境可持续捕获和不可逆化学转化CO2在温和条件下的潜力。
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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.
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来源期刊
Inorganic Chemistry
Inorganic Chemistry 化学-无机化学与核化学
CiteScore
7.60
自引率
13.00%
发文量
1960
审稿时长
1.9 months
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.
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