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

被引:50
作者
Chen, Xin-Jia [1 ]
Bai, Chang-Wei [1 ]
Sun, Yi-Jiao [1 ]
Huang, Xin-Tong [1 ]
Zhang, Bin-Bin [1 ]
Zhang, Yi-Shuo [1 ]
Yang, Qi [2 ,3 ]
Wu, Jing-Hang [4 ]
Chen, Fei [1 ]
机构
[1] Chongqing Univ, Coll Environm & Ecol, Key Lab Three Gorges Reservoir Reg Ecoenvironm, Minist Educ, Chongqing 400045, Peoples R China
[2] Hunan Univ, Coll Environm Sci & Engn, Changsha 410082, Peoples R China
[3] Hunan Univ, Key Lab Environm Biol & Pollut Control, Minist Educ, Changsha 410082, Peoples R China
[4] Univ Sci & Technol China, Dept Environm Sci & Engn, CAS Key Lab Urban Pollutant Convers, Hefei 230026, Peoples R China
基金
中国国家自然科学基金;
关键词
pH-dependent degradation; Fe(VI)-PAA; sulfonamide antibiotics transformation; active species evolution; mechanism dissection; EMERGING CONTAMINANTS; OXIDATION; PEROXYMONOSULFATE; SULFAMETHOXAZOLE; BIOACCUMULATION; INVOLVEMENT; FERRATE(V); ACTIVATION; REMOVAL; FE(IV);
D O I
10.1021/acs.est.3c06370
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
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)-H2O2, and standalone Fe(VI) systems. Notably, at a pH of 9.0, boasting a kinetic constant of similar to 0.127 M-1<middle dot>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)-H2O2 system and 105.58-fold when using Fe(VI) individually. The behavior of active species & horbar;such as the dynamic center dot OH radicals and high-valent iron species (Fe(IV)/Fe(V))& horbar;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 center dot 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.
引用
收藏
页码:20206 / 20218
页数:13
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