pH-Driven Efficacy of the Ferrate(VI)–Peracetic Acid System in Swift Sulfonamide Antibiotic Degradation: A Deep Dive into Active Species Evolution and Mechanistic Insights

过氧乙酸 化学 人体净化 污染物 降级(电信) 反应速率常数 激进的 环境化学 过氧化氢 动力学 有机化学 废物管理 工程类 计算机科学 物理 电信 量子力学
作者
Xin‐Jia Chen,Chang‐Wei Bai,Yi-Jiao Sun,Xin-Tong Huang,Binbin Zhang,Yi-Shuo Zhang,Qi Xing Yang,Jing‐Hang Wu,Fei Chen
出处
期刊:Environmental Science & Technology [American Chemical Society]
卷期号:57 (48): 20206-20218 被引量:95
标识
DOI:10.1021/acs.est.3c06370
摘要

In the realm of wastewater treatment, the power of ferrate (Fe(VI)) and peracetic acid (PAA) as oxidants stands out. But their combined might is where the enhancement truly lies. Their collaborative effect intensifies, but the underlying mechanics, especially across varying pH levels and pollutant types, still lurks in obscurity. Our study delved into the sophisticated oxidation interplay among Fe(VI)–PAA, Fe(VI)–H 2 O 2, and standalone Fe(VI) systems. Notably, at a pH of 9.0, boasting a kinetic constant of ∼0.127 M –1 ·s –1, the Fe(VI)–PAA system annihilated the pollutant sulfamethoxazole, outpacing its counterparts by a staggering 48.73-fold when compared to the Fe(VI)–H 2 O 2 system and 105.58-fold when using Fe(VI) individually. The behavior of active species─such as the dynamic •OH radicals and high-valent iron species (Fe(IV)/Fe(V))─shifted with pH variations, leading to distinct degradation pathways. Our detailed exploration pinpoints the behaviors of certain species across pH levels from 3.0 to 9.0. In more acidic environments, the •OH species proved indispensable for the system’s reactivity. Conversely, as the pH inclined, degradation was increasingly steered by high-valent iron species. This intensive probe demystifies Fe(VI) interactions, deepening our understanding of the capabilities of the Fe(VI)-centered system and guiding us toward cleaner water solutions. Importantly, pH value, often underappreciated, holds the reins in organic wastewater decontamination. Embracing this key player is vital as we strategize for more expansive systems in upcoming ventures.
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