☆ 4.7 Article

Novel solar-driven ferrate(VI) activation system for micropollutant degradation: Elucidating the role of Fe(IV) and Fe(V)

JOURNAL OF HAZARDOUS MATERIALS (2022)

Journal

JOURNAL OF HAZARDOUS MATERIALS

Volume 437, Issue -, Pages -

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ELSEVIER

DOI: 10.1016/j.jhazmat.2022.129428

Keywords

Solar; Ferrate(VI); Photochemistry; High-valent iron intermediates

Funding

National Natural Science Foundation of China [52100013]
Natural Science Foundation of Guangdong Province [2022A1515011207]
Guangdong Provincial Department of Education Youth Innovation Talents Project (Natural Science) [2020KQNCX092]
Student Innovation and Entrepreneurship Program of Wuyi University [2020CX12]
Basic and Theoretical Scientific Research Projects of Jiangmen City [2020JC01017]
Research Project of High-level Talents of Wuyi University [2019AL024]

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Abstract

This paper presents a novel process using solar-ferrate(VI) for efficient degradation of micropollutants. The study found that Fe(V) and Fe(IV), rather than reactive oxygen species, played a significant role in the process. The researchers also elucidated the reaction mechanism of Fe(VI) and its degradation of micropollutants. Additionally, the study investigated the effect of pH and various ions on the degradation process. The solar-ferrate(VI) process demonstrated excellent applicability under different irradiation conditions.

This paper presents a novel process of solar-ferrate(VI) [Fe(VI)] for micropollutant degradation. The solar-Fe(VI) process promoted micropollutant degradation compared with Fe(VI) alone and solar. The radical scavenging and probing experiment results suggested that Fe(V) and Fe(IV) but not reactive oxygen species were most likely involved in the solar-Fe(VI) process. Through building a kinetic model, Fe(IV) and Fe(V) were observed to play an equally significant role in the solar-Fe(VI) process. Afterward, the reaction mechanism of the photochemistry of Fe(VI) was elaborated. Fe(IV) formed from Fe(VI) photolysis and then decomposed to Fe(II) which reacted with Fe(VI) to form Fe(V). Furthermore, the effect of pH on carbamazepine (CBZ) degradation was studied and the quantum yields of Fe(VI) were determined, with (1.98 +/- 0.16) x 10(-3) mol.einstein(-1), (5.90 +/- 0.27) x 10-(4) mol.einstein(-1), and (1.66 +/- 0.14) x 10(-4) mol.einstein(-1) at pH 7.0, 8.0, and 9.0, respectively. Inorganic ions, including Cl, HCO3, and Br displayed negligible influence on the CBZ degradation, whereas humic acid inhibited the CBZ degradation. Finally, the solar-Fe(VI) process exhibited good applicability in authentic waters and under different irradiation (natural sunlight, ultraviolet light, and visible light from solar cut-off emission). Overall, this study provides a new routine for efficient micropollutant elimination and reveals the photochemistry of Fe(VI).

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Reactive High-Valent Iron Intermediates in Enhancing Treatment of Water by Ferrate

Virender K. Sharma, Mingbao Feng, Dionysios D. Dionysiou, Hong-Cai Zhou, Chetan Jinadatha, Kyriakos Manoli, Mallory F. Smith, Rafael Luque, Xingmao Ma, Ching-Hua Huang

Summary: Efforts are being made to enhance the reactivity of ferrate by generating highly reactive iron intermediates (Fe-V and Fe-IV) from the tetraoxy anion of iron in the +6 oxidation state. Various strategies, such as addition of acid, metal ions, and reductants, are utilized to produce Fe-V and Fe-IV species for more efficient treatment of polluted water. Kinetic modeling and DFT calculations provide opportunities to distinguish between Fe-IV and Fe-V in order to improve oxidation reactions using ferrate.

ENVIRONMENTAL SCIENCE & TECHNOLOGY (2022)