School of Environmental & Chemical Engineering, Dalian Jiaotong University, Dalian 116021, China; Key Laboratory of Industrial Ecology and Environmental Engineering (Ministry of Education), School of Environmental Science and Technology, Dalian University of Technology, Dalian 116024, China.
Key Laboratory of Industrial Ecology and Environmental Engineering (Ministry of Education), School of Environmental Science and Technology, Dalian University of Technology, Dalian 116024, China.
J Hazard Mater. 2023 Feb 15;444(Pt A):130394. doi: 10.1016/j.jhazmat.2022.130394. Epub 2022 Nov 15.
As two important components of dissolved organic matter (DOM), dissolved black carbon (DBC) and humic acid (HA) possess different chemical and structural properties, which might influence their activities like metal complexation and mediating electron transfer. In this study, a series of coprecipitates of iron oxides (FeO) and DOM (HA or DBC) having different C/Fe molar ratios (0.2-3.0) was prepared under ambient conditions, which exhibited excellent catalytic efficiencies upon Fenton-like degradation of norfloxacin (NOR). Pseudo-first-order rate constant of NOR oxidation catalyzed by DBC-FeO (C/Fe=3.0, 1.13 h) was 30.5, 4.3-14.2, and 1.3-15.7 folds higher than those mediated by FeO alone, HA-FeO and DBC-FeO coprecipitates having C/Fe molar ratios of 0.2 and 1.6, respectively. Due to the higher concentrations of surface-bound Fe(III)/Fe(II) in the DBC-FeO mediated systems, improved Fe(III)/Fe(II) cycling rates, •OH accumulation and NOR degradation were observed as compared with those of counterpart systems mediated by HA-FeO. Besides functioning in Fe-C complexation to accelerate FeOOH cleavage, carbonyl/carboxyl groups of the coprecipitates also serve as electron shuttles, both of which improved Fe(III)/Fe(II) cycling and •OH production. Our findings emphasized the influence of DOM source and compositions on Fe(III)/Fe(II) cycling and provided a facile approach of preparing Fe-C catalyst for contaminants elimination.
作为溶解态有机物(DOM)的两个重要组成部分,溶解态黑碳(DBC)和腐殖酸(HA)具有不同的化学和结构性质,这可能会影响它们的活性,如金属络合和介导电子转移。在这项研究中,在环境条件下制备了一系列具有不同 C/Fe 摩尔比(0.2-3.0)的氧化铁(FeO)和 DOM(HA 或 DBC)共沉淀物,它们在类芬顿体系下对诺氟沙星(NOR)的降解表现出优异的催化效率。DBC-FeO(C/Fe=3.0)共沉淀物催化 NOR 氧化的准一级速率常数(1.13 h)分别是 FeO 单独、C/Fe 摩尔比为 0.2 和 1.6 的 HA-FeO 和 DBC-FeO 共沉淀物介导的 NOR 氧化的 30.5、4.3-14.2 和 1.3-15.7 倍。由于 DBC-FeO 介导体系中表面结合的 Fe(III)/Fe(II)浓度较高,与 HA-FeO 介导的对应体系相比,观察到 Fe(III)/Fe(II)循环速率提高、•OH 积累和 NOR 降解。除了在 Fe-C 络合中加速 FeOOH 裂解外,共沉淀物中的羰基/羧基基团还作为电子穿梭体,这两者都提高了 Fe(III)/Fe(II)循环和•OH 生成。我们的研究结果强调了 DOM 来源和组成对 Fe(III)/Fe(II)循环的影响,并提供了一种制备用于去除污染物的 Fe-C 催化剂的简便方法。