掺杂 N 的β-酮烯胺共价有机框架(COFs)用于提高光催化氧化活性

IF 3.2 3区 化学 Q2 CHEMISTRY, INORGANIC & NUCLEAR Journal of Solid State Chemistry Pub Date : 2024-09-16 DOI:10.1016/j.jssc.2024.125017
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引用次数: 0

摘要

β-酮烯胺基 COF 具有高稳定性、良好的结晶性和可调的骨架结构,因此受到广泛研究。掺氮是提高 COF 催化活性的有效方法之一。本文通过 1,3,5-二甲基氯代葡萄糖醇(TP)与含有不同数量氮原子的对苯二胺之间的希夫碱缩合反应,成功地构建了掺氮的β-酮烯胺基(0N-TP-COF、1N-TP-COF、2N-TP-COF)COFs。研究表明,随着氮原子数的增加,制备的 COFs 表现出更合适的电子结构和更丰富的电子活性位点。此外,0N-TP-COF(99%,48 小时)< 1N-TP-COF(99%,32 小时)< 2N-TP-COF(99%,16 小时)对 4-甲酰基苯硼酸转化的光催化性能,以及 0N-TP-COF(99%,16 小时)< 1N-TP-COF(99%,3.5 h) <2N-TP-COF(99 %,1.5 h)。值得注意的是,所有掺杂氮的 COF 都具有优异的催化活性和稳定性,其中 2N-TP-COF 的催化活性最高。这项研究表明,掺杂氮原子是提高光催化性能的有效方法。
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N-doping of β-ketoenamine based covalent organic frameworks (COFs) for enhancing photocatalytic oxidation activity

β-ketoenamine-based COFs are widely investigated due to their high stability, good crystallinity and tunable skeleton structures. Nitrogen doping is one of the effective ways to enhance the catalytic activity of COFs. Herein, N-doping of β-ketoenamine-based (0N-TP-COF, 1N-TP-COF, 2N-TP-COF) COFs were successfully constructed by the Schiff base condensation reaction between 1,3,5-tiformylphloroglucinol (TP) and p-phenylenediamine containing different numbers of nitrogen atoms. Studies showed that the as-prepared COFs exhibited more suitable electronic structure and more electron-rich active sites with the increasing of N atoms. Furthermore, the photocatalytic performance of 4-formylphenylboronic acid transformation was 0N-TP-COF (99 %, 48 h) < 1N-TP-COF (99 %, 32 h) < 2N-TP-COF (99 %, 16 h), and the photocatalytic performance of benzylamine coupling was 0N-TP-COF (99 %, 16 h) < 1N-TP-COF (99 %, 3.5 h) <2N-TP-COF (99 %, 1.5 h), respectively. Note that all N-doping COFs have excellent catalytic activity as well as stability, and 2N-TP-COF exhibits the highest catalytic activity. This work demonstrates that doping of nitrogen atoms is an effective way to enhance photocatalytic performance.

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来源期刊
Journal of Solid State Chemistry
Journal of Solid State Chemistry 化学-无机化学与核化学
CiteScore
6.00
自引率
9.10%
发文量
848
审稿时长
25 days
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.
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