Degradation of dyes by peroxymonosulfate activated by ternary CoFeNi-layered double hydroxide: Catalytic performance, mechanism and kinetic modeling

化学 氢氧化物 动能 催化作用 层状双氢氧化物 三元络合物 三元运算 机制(生物学) 降级(电信) 化学工程 动力学 无机化学 有机化学 工程类 哲学 物理 认识论 程序设计语言 电信 量子力学 计算机科学
作者
Hanxuan Zeng,Weiqiu Zhang,Lin Deng,Jinming Luo,Shiqing Zhou,Xia Liu,Yong Pei,Zhou Shi,John C. Crittenden
出处
期刊:Journal of Colloid and Interface Science [Elsevier BV]
卷期号:515: 92-100 被引量:110
标识
DOI:10.1016/j.jcis.2018.01.016
摘要

Ternary CoFeNi-layered double hydroxide (CoFeNi-LDH) was synthesized and initially applied to activate peroxymonosulfate (PMS) for the degradation of Congo red (CR) and Rhodamine B (RhB). The results show that the CoFeNi-LDH/PMS system can efficiently degrade nearly 100% of 20 mg/L CR or 20 mg/L RhB within 6- and 10-min reaction times, respectively. And the catalyst exhibits higher degradation efficiency on CR than on RhB under identical conditions, which is confirmed by electron clouds of the highest occupied molecular orbital (HOMO) and lowest unoccupied molecular orbital (LUMO) performed by DFT calculations. Quenching tests reveal that SO4- is the dominant active species participating in the degradation process. Mechanism investigation demonstrates that Co(II)-Co(III)-Co(II) cycle is responsible for activating PMS to generate radicals for dyes degradation. A dynamic kinetic model is successfully developed to simulate the concentration profiles of CR and RhB degradation in CoFeNi-LDH/PMS system. The empirical second order rate constants between SO4- and CR (kSO4-/CR), HO and CR (kOH/CR), SO4- and RhB (kSO4-/RhB), HO and RhB (kHO/RhB) are determined to be 2.47 × 107, 3.44 × 106, 8.39 × 106 and 2.62 × 107 M-1s-1, respectively. In addition, toxic assessment using ECOSAR program suggests that the overall toxicity of CR and RhB decreased after treatment with CoFeNi-LDH/PMS system. Repeating tests and application of CoFeNi-LDH in different water sources give us adequate confidence that the as-synthesized CoFeNi-LDH is favorable for the purification of dye-contaminanted waters in practical.
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