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增强光催化活性氧物种监测:利用电化学快速感应香豆素降解过程中形成的羟基自由基。

Enhanced Monitoring of Photocatalytic Reactive Oxygen Species: Using Electrochemistry for Rapid Sensing of Hydroxyl Radicals Formed during the Degradation of Coumarin.

机构信息

The Bryden Centre, Queen's University Belfast, University Road, Belfast BT7 1NN, U.K.

Department of Life and Physical Sciences, Atlantic Technological University, Donegal, Letterkenny F92 FC93, Ireland.

出版信息

J Phys Chem A. 2023 Jun 15;127(23):5039-5047. doi: 10.1021/acs.jpca.3c00741. Epub 2023 May 31.

Abstract

Many recent research studies have reported indirect methods for the detection and quantification of OH radicals generated during photocatalysis. The short lifespan and high reactivity of these radicals make indirect detection using probes such as coumarin a more viable quantification method. Hydroxyl radical production is commonly monitored using fluorescence spectroscopy to determine the concentration of the compound 7-hydroxycoumarin, which is formed from hydroxyl radical attack on coumarin. There are, however, a number of additional hydroxylated coumarins generated during this process, which are less amenable to detection by fluorescence spectroscopy. Consequently, limitations and inaccuracies of this method have previously been reported in the literature. As an alternative approach to those previously reported, this work has developed an electrochemical screening method using coumarin as a OH radical trap, that is capable of in situ monitoring of not only 7-hydroxycoumarin, but all the main mono-hydroxylated products formed. As a result, this technique is a more representative and comprehensive method for the quantification of OH radicals produced by photocatalysts using coumarin as a probe molecule. Moreover, the electroanalytical method provides a portable, rapid, sensitive, and accurate in situ method for the monitoring of OH radical formation without the need for sample preparation.

摘要

许多最近的研究报告都报道了间接方法来检测和量化光催化过程中生成的羟基自由基。这些自由基的短寿命和高反应性使得使用香豆素等探针进行间接检测成为更可行的定量方法。羟基自由基的产生通常通过荧光光谱法进行监测,以确定 7-羟基香豆素的浓度,该化合物是由羟基自由基攻击香豆素形成的。然而,在这个过程中还会生成许多其他的羟基化香豆素,这些香豆素的荧光光谱检测不太容易。因此,该方法在之前的文献中已经被报道存在局限性和不准确性。作为对之前报道方法的一种替代方法,这项工作开发了一种使用香豆素作为 OH 自由基捕获剂的电化学筛选方法,该方法能够原位监测不仅是 7-羟基香豆素,而且是所有主要单羟基化产物的形成。因此,与使用香豆素作为探针分子的其他方法相比,该技术是一种更具代表性和更全面的定量光催化剂产生的 OH 自由基的方法。此外,该电化学分析方法提供了一种便携式、快速、灵敏和准确的原位方法,用于监测 OH 自由基的形成,而无需进行样品制备。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/681a/10278141/19ca834e2054/jp3c00741_0002.jpg

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