液-液接触电催化H2O2生成羟基自由基

IF 7.4 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY
Hai-Mei Li, Airong Xie, Chengzi Hong, Zichen Wang, Xu Chu, Zhong Lin Wang, Yi Liu, Peng Jiang
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引用次数: 0

摘要

接触电催化(CEC)已成为一种很有前途的活性氧(ROS)生成策略,主要通过水氧化反应(WOR)和氧还原反应(ORR),形成了接触电动力治疗(CEDT)的基础。然而,ORR的高能量势垒实质上限制了整体催化效率。在此,我们提出了一种替代的过氧化氢(h2o2)还原途径来取代ORR途径,使羟基自由基(•OH)在没有超声辅助的情况下自发产生。制备了全氟碳纳米乳液,构建了全氟碳-水液-液界面。PFC-水界面的接触通电诱导界面电子转移过程,其中PFC作为介质从氢氧根离子(OH -)中捕获电子,随后将其转移到H2O2中,从而生成•OH。此外,超声波可以通过增加液液接触频率和促进电子从带负电荷的PFC (PFC*)释放到h2o2来促进•OH的产生。重要的是,我们证明了这种基于h2o2的CEC途径代表了以前未被认识的CEDT机制。在H2O2过表达的肿瘤微环境中,这种机制导致ROS生成增强和肿瘤细胞死亡。这项工作揭示了cet框架内隐藏的催化途径,为CEC在肿瘤治疗中的应用提供了新的见解。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
Hydroxyl Radical Generation from H2O2 via Liquid-Liquid Contact-Electro-Catalysis
Contact-electro-catalysis (CEC) has emerged as a promising strategy for reactive oxygen species (ROS) generation, primarily through water oxidation reactions (WOR) and oxygen reduction reactions (ORR), forming the foundation of contact-electrodynamic therapy (CEDT). However, the high energy barrier of the ORR substantially limits the overall catalytic efficiency. Herein, we propose an alternative hydrogen peroxide (H 2 O 2 ) reduction pathway to replace the ORR pathway, enabling the spontaneous generation of hydroxyl radicals (•OH) without ultrasound assistance. Perfluorocarbon (PFC) nanoemulsions were prepared to construct a PFC-water liquidliquid interface. Contact electrification at the PFC-water interface induces interfacial electron-transfer process, wherein the PFC act as mediators by capturing electrons from hydroxide ions (OH -) and subsequently transferring them to H2O2 , thereby generating •OH. Furthermore, ultrasound can enhance •OH production by increasing the frequency of liquid-liquid contact and facilitating electron release from negatively charged PFC (PFC*) to H 2 O 2 . Importantly, we demonstrate that this H 2 O 2 -based CEC pathway represents a previously unrecognized mechanism underlying CEDT. In tumor microenvironments, where H2O2 is overexpressed, this mechanism leads to enhanced ROS production and tumor cell death. This work uncovers a hidden catalytic route within the CEDT framework and provides new insights into the application of CEC for tumor therapy.
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来源期刊
Chemical Science
Chemical Science CHEMISTRY, MULTIDISCIPLINARY-
CiteScore
14.40
自引率
4.80%
发文量
1352
审稿时长
2.1 months
期刊介绍: Chemical Science is a journal that encompasses various disciplines within the chemical sciences. Its scope includes publishing ground-breaking research with significant implications for its respective field, as well as appealing to a wider audience in related areas. To be considered for publication, articles must showcase innovative and original advances in their field of study and be presented in a manner that is understandable to scientists from diverse backgrounds. However, the journal generally does not publish highly specialized research.
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