Improving the onset of oxygen redox reactions by activating surface defects with visible light on a ZnO-based electrode

IF 2.4 3区 化学 Q2 CHEMISTRY, INORGANIC & NUCLEAR
C.K. Zagal Padilla , Sergio A. Gamboa , B. Campillo , Virginia Gomez-Vidales , A. Álvarez Gallegos
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Abstract

This study investigates the influence of photoactivated oxygen vacancies (VO) on the activation of oxygen redox reactions, such as evolution (OER) and reduction (ORR) reactions. The reactions were carried out on the surface of an electrode prepared with ZnO prepared by green synthesis and supported on sterling silver. Structural and surface analyses using X-ray diffraction (XRD), Raman spectroscopy, X-ray photoelectron spectroscopy (XPS), and electron paramagnetic resonance (EPR) confirmed the presence of oxygen vacancies. Electrochemical analysis performed in an alkaline medium showed that Vo exhibited photoactivation under visible light illumination. This photoactivation process facilitated electron transfer, resulting in the formation of superoxide intermediates (O2-). These intermediates contribute to the generation of singlet oxygen (1O2), which enhances OER activity and enables the photoexcitation of adsorbed peroxides and singlet oxygen. This process promotes the formation of triplet oxygen (3O2), which improves the ORR kinetics. The incorporation of Mg into the Zn-O matrix may play an essential role in these processes. These results provide new insights into the design of electrocatalysts using visible-light-activated redox processes for rechargeable batteries and fuel cell applications.

Abstract Image

利用可见光在zno基电极上激活表面缺陷,改善氧氧化还原反应的发生
本研究探讨了光活性氧空位(VO)对氧氧化还原反应如演化(OER)和还原(ORR)反应活化的影响。在绿色合成法制备的ZnO电极表面和纯银载体上进行了反应。利用x射线衍射(XRD)、拉曼光谱(Raman spectroscopy)、x射线光电子能谱(XPS)和电子顺磁共振(EPR)对其结构和表面进行分析,证实了氧空位的存在。在碱性介质中进行的电化学分析表明,Vo在可见光照射下表现出光活化。这种光活化过程促进了电子转移,导致超氧化物中间体(O2-)的形成。这些中间体有助于生成单线态氧(1O2),从而增强OER活性,使吸附的过氧化物和单线态氧能够光激发。这一过程促进了三态氧(3O2)的形成,提高了ORR动力学。Mg在Zn-O基体中的掺入可能在这些过程中起重要作用。这些结果为可充电电池和燃料电池使用可见光激活氧化还原过程设计电催化剂提供了新的见解。
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来源期刊
Polyhedron
Polyhedron 化学-晶体学
CiteScore
4.90
自引率
7.70%
发文量
515
审稿时长
2 months
期刊介绍: Polyhedron publishes original, fundamental, experimental and theoretical work of the highest quality in all the major areas of inorganic chemistry. This includes synthetic chemistry, coordination chemistry, organometallic chemistry, bioinorganic chemistry, and solid-state and materials chemistry. Papers should be significant pieces of work, and all new compounds must be appropriately characterized. The inclusion of single-crystal X-ray structural data is strongly encouraged, but papers reporting only the X-ray structure determination of a single compound will usually not be considered. Papers on solid-state or materials chemistry will be expected to have a significant molecular chemistry component (such as the synthesis and characterization of the molecular precursors and/or a systematic study of the use of different precursors or reaction conditions) or demonstrate a cutting-edge application (for example inorganic materials for energy applications). Papers dealing only with stability constants are not considered.
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