In Situ Raman Studying the Microstructure and Function of FeIV Species in Advanced Oxidation Process

IF 5.8 2区 环境科学与生态学 Q1 CHEMISTRY, MULTIDISCIPLINARY
Chunwan Wang, Shiwei Li, Yun Zhang, Xiaoling Zhang, Wei Ran, Rui Liu
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引用次数: 0

Abstract

Due to the efficient and stable pollutant degradation properties, Fe species from Fe-based single-atom catalysts (Fe-SACs) have garnered significant interest in advanced oxidation processes (AOPs). However, the microstructure and function of Fe species in these processes remain contentious. In this study, we developed Au@SiO2@Fe-SACs and utilized a combination of in situ surface-enhanced Raman spectroscopy, theoretical calculations, and synchrotron radiation techniques to elucidate the structure and functional mechanisms of Fe species during AOPs. Our findings demonstrated that Fe-SACs with a FeN4 structure were loaded on Au@SiO2 to obtain Au@SiO2@Fe-SACs. During PMS oxidation, a Raman peak associated with the Fe-O bonds appeared at 837 cm-1 along with blue-shifts of Fe-N bonds from 183 cm-1 and 322 cm-1 to 191 cm-1 and 335 cm-1, proving the generation of Fe species. Specifically, the elongation of the Fe-O bond displaced the Fe atom from the NC plane, resulting in an extension of the Fe-N bond length from 1.88 Å to 1.93 Å. Furthermore, the FeⅣ species directly oxidized typical pollutant phenol through a direct oxidation transformation pathway (DOTP) within a wide pH range of 3 to 9. They exhibited a significant increase in removal efficiency of phenol than the hydroxyl radicals (·OH) from activated H2O2 and effective reduction of total organic carbon (TOC). This study offers critical insights into the structural and functional attributes of FeⅣ species, providing valuable guidance for the design of more efficient Fe-SACs in AOPs.
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来源期刊
Environmental Science: Nano
Environmental Science: Nano CHEMISTRY, MULTIDISCIPLINARY-ENVIRONMENTAL SCIENCES
CiteScore
12.20
自引率
5.50%
发文量
290
审稿时长
2.1 months
期刊介绍: Environmental Science: Nano serves as a comprehensive and high-impact peer-reviewed source of information on the design and demonstration of engineered nanomaterials for environment-based applications. It also covers the interactions between engineered, natural, and incidental nanomaterials with biological and environmental systems. This scope includes, but is not limited to, the following topic areas: Novel nanomaterial-based applications for water, air, soil, food, and energy sustainability Nanomaterial interactions with biological systems and nanotoxicology Environmental fate, reactivity, and transformations of nanoscale materials Nanoscale processes in the environment Sustainable nanotechnology including rational nanomaterial design, life cycle assessment, risk/benefit analysis
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