{"title":"TEMPO-functionalized porous aromatic framework for efficient and selective electrocatalytic oxidation of cyclooctene","authors":"","doi":"10.1016/j.mcat.2024.114558","DOIUrl":null,"url":null,"abstract":"<div><p>The development of economically viable and environmentally benign oxidation reaction systems with high selectivity and efficiency is a key focus in synthetic chemistry. Utilizing water as an oxygen source, alongside an anodic system for converting water to oxygenated compounds, represents an atom-economical and sustainable strategy for highly selectively synthesizing epoxides. Herein, we synthesized a novel porous aromatic framework with TEMPO radicals uniformly immobilized on the pore surface by a synthetic bottom-up approach (PAF-TEMPO). Strategically grafting TEMPO catalytic sites, which results in a highly dense and uniform dispersion, promotes extensive reactant contact, thereby enhancing catalytic efficiency. The PAF-TEMPO catalyst demonstrated efficient electrocatalytic activity for cyclooctene oxidation to cyclooctene oxide, achieving 89.7 % yield and 90.3 % selectivity with good recyclability. This work will give inspiration for novel electrocatalyst design and development of green and sustainable catalytic systems.</p></div>","PeriodicalId":393,"journal":{"name":"Molecular Catalysis","volume":null,"pages":null},"PeriodicalIF":3.9000,"publicationDate":"2024-09-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Molecular Catalysis","FirstCategoryId":"92","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S2468823124007405","RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
引用次数: 0
Abstract
The development of economically viable and environmentally benign oxidation reaction systems with high selectivity and efficiency is a key focus in synthetic chemistry. Utilizing water as an oxygen source, alongside an anodic system for converting water to oxygenated compounds, represents an atom-economical and sustainable strategy for highly selectively synthesizing epoxides. Herein, we synthesized a novel porous aromatic framework with TEMPO radicals uniformly immobilized on the pore surface by a synthetic bottom-up approach (PAF-TEMPO). Strategically grafting TEMPO catalytic sites, which results in a highly dense and uniform dispersion, promotes extensive reactant contact, thereby enhancing catalytic efficiency. The PAF-TEMPO catalyst demonstrated efficient electrocatalytic activity for cyclooctene oxidation to cyclooctene oxide, achieving 89.7 % yield and 90.3 % selectivity with good recyclability. This work will give inspiration for novel electrocatalyst design and development of green and sustainable catalytic systems.
开发具有高选择性和高效率的经济可行且对环境无害的氧化反应系统是合成化学的一个重点。利用水作为氧源,同时利用阳极系统将水转化为含氧化合物,是一种原子经济、可持续的高选择性合成环氧化物的策略。在此,我们通过一种自下而上的合成方法(PAF-TEMPO)合成了一种新型多孔芳香框架,其孔隙表面均匀固定了 TEMPO 自由基。有策略地接枝 TEMPO 催化位点可形成高度致密和均匀的分散,促进反应物的广泛接触,从而提高催化效率。PAF-TEMPO 催化剂在环辛烯氧化成环辛烯氧化物的过程中表现出高效的电催化活性,产率达 89.7%,选择性达 90.3%,并具有良好的可回收性。这项工作将为新型电催化剂的设计和绿色可持续催化系统的开发提供灵感。
期刊介绍:
Molecular Catalysis publishes full papers that are original, rigorous, and scholarly contributions examining the molecular and atomic aspects of catalytic activation and reaction mechanisms. The fields covered are:
Heterogeneous catalysis including immobilized molecular catalysts
Homogeneous catalysis including organocatalysis, organometallic catalysis and biocatalysis
Photo- and electrochemistry
Theoretical aspects of catalysis analyzed by computational methods