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Metal-free activation of molecular oxygen by covalent triazine frameworks for selective aerobic oxidation
Science Advances ( IF 11.7 ) Pub Date : 2020-04-03 , DOI: 10.1126/sciadv.aaz2310
Sara Abednatanzi 1 , Parviz Gohari Derakhshandeh 1 , Karen Leus 1 , Henk Vrielinck 2 , Freddy Callens 2 , Johannes Schmidt 3 , Aleksandr Savateev 4 , Pascal Van Der Voort 1
Affiliation  

Oxygen activation is a critical step in ubiquitous heterogeneous oxidative processes, most prominently in catalysis, electrolysis, and pharmaceutical applications. We present here our findings on metal-free O2 activation on covalent triazine frameworks (CTFs) as an important class of N-rich materials. The O2 activation process was studied for the formation of aldehydes, ketones and imines. A detailed mechanistic study of O2 activation and the role of nitrogen heteroatoms were comprehensively investigated. The electron paramagnetic resonance (EPR) and control experiments provide strong evidence for the reaction mechanism proving the applicability of the CTFs to activate oxygen into superoxide species. This report highlights the importance of a self-templating procedure to introduce N functionalities for the development of metal-free catalytic materials. The presented findings reveal an important step toward the use of CTFs as inexpensive and high-performance alternatives to metal-based materials not only for catalysis but also for biorelated applications dealing with O2 activation.



中文翻译:


通过共价三嗪骨架无金属活化分子氧以进行选择性有氧氧化



氧活化是普遍存在的多相氧化过程中的关键步骤,尤其是在催化、电解和制药应用中。我们在此介绍我们关于共价三嗪骨架(CTF)作为一类重要的富氮材料的无金属 O 2活化的研究结果。研究了醛、酮和亚胺形成的O 2活化过程。全面研究了O 2活化的详细机制和氮杂原子的作用。电子顺磁共振(EPR)和控制实验为反应机制提供了强有力的证据,证明了CTFs将氧活化成超氧化物物质的适用性。该报告强调了引入氮功能的自模板程序对于开发无金属催化材料的重要性。所提出的研究结果揭示了使用CTF作为金属基材料的廉价且高性能替代品的重要一步,不仅用于催化,而且还用于处理O 2活化的生物相关应用。

更新日期:2020-04-06
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