National and Provincial Joint Engineering Laboratory of Wetland Ecological Conservation, Heilongjiang Academy of Science, Harbin, 150040, China.
State Key Laboratory of Urban Water Resource and Environment, School of Environment, Harbin Institute of Technology, Harbin, 150090, China.
J Hazard Mater. 2019 Mar 5;365:744-750. doi: 10.1016/j.jhazmat.2018.11.031. Epub 2018 Nov 11.
In this study, Fe-modified goethite with low defects (α-Fe(Fe)OOH) was synthesized and characterized. Results revealed that α-Fe(Fe)OOH is a nano magnetic material with goethite (α-FeOOH) -type structures and has fewer Lewis acid of Fe on its surface. Moreover, α-Fe(Fe)OOH was effective in catalytic ozonation of 4-chloronitrobenzene (4-CNB), which is a probe contaminant that cannot be efficiently removed through sole ozonation. The removal of 4-CNB increased with ozone concentration and α-Fe(Fe)OOH dosage, but decreased with the presence of carbonate, sulfate and phosphate. The catalytic activity of α-Fe(Fe)OOH also showed a dependence on solution pH. The presence of humic acid accelerated 4-CNB removal at low concentration but inhibited the removal at high concentration. In comparison with α-FeOOH, α-Fe(Fe)OOH significantly enhanced hydroxyl radicals generation and reduced Fe ions release in this process. The hydroxyl groups of Fe on α-FeOOH and α-Fe(Fe)OOH surface was active site for ozone decomposition into hydroxyl radicals. Introducing Fe significantly increased the density of surface hydroxyl groups relative to α-FeOOH. This enhancement significantly promoted hydroxyl radicals generation and 4-CNB degradation in the solution.
在这项研究中,合成并表征了具有低缺陷(α-Fe(Fe)OOH)的改性针铁矿。结果表明,α-Fe(Fe)OOH 是一种纳米磁性材料,具有针铁矿(α-FeOOH)型结构,表面的 Lewis 酸 Fe 较少。此外,α-Fe(Fe)OOH 对 4-氯硝基苯(4-CNB)的催化臭氧化有效,4-CNB 是一种探针污染物,单独臭氧化无法有效去除。4-CNB 的去除率随臭氧浓度和α-Fe(Fe)OOH 用量的增加而增加,但随碳酸盐、硫酸盐和磷酸盐的存在而降低。α-Fe(Fe)OOH 的催化活性也表现出对溶液 pH 的依赖性。腐殖酸的存在会在低浓度下加速 4-CNB 的去除,但在高浓度下会抑制其去除。与 α-FeOOH 相比,α-Fe(Fe)OOH 显著增强了羟基自由基的生成并减少了铁离子的释放。α-FeOOH 和 α-Fe(Fe)OOH 表面的 Fe 羟基基团是臭氧分解为羟基自由基的活性位点。引入 Fe 会显著增加表面羟基基团的密度,从而显著促进溶液中羟基自由基的生成和 4-CNB 的降解。