College of Environmental Science and Engineering, Nankai University, Tianjin 300350, China.
College of Environmental Science and Engineering, Nankai University, Tianjin 300350, China; Key Laboratory of Pollution Processes and Environmental Criteria (Ministry of Education), Tianjin 300350, China; Tianjin Engineering Center of Environmental Diagnosis and Contamination Remediation, Tianjin 300350, China.
Sci Total Environ. 2021 May 20;770:144680. doi: 10.1016/j.scitotenv.2020.144680. Epub 2021 Jan 17.
Research on the in-situ generation of hydrogen peroxide (HO) using nano zero-valent iron (nZVI) has received more and more attention in recent years. However, the low utilization rate of nZVI, strict production conditions, and high energy consumption limit the application of this technology in actual environmental pollution remediation. In this study, carbon-coated nZVI (Fe@C) was used to synthesize HO in situ and realize the mineralization of nitrobenzene (NB). The results showed that the composite removed 91% of NB through adsorption, reduction, and oxidation within 120 min, of which oxidation accounts for 42.92%. Not only that, the composite material could achieve effective mineralization of NB under the wide pH range of 3-7. Quantitative experiments of hydroxyl radicals (HO) showed that the composite could generate 185.64 μM HO in 120 min without any extra energy consumption. The carbon-coated structure effectively inhibits the formation of the passivation layer on the surface of the nZVI, thereby ensuring the high activity of the Fe. In addition, the carbon coating strengthens the sequential single-electron transfer process by changing the oxygen reduction pathway on the surface of the nZVI, so that the Fe can efficiently generate HO through the superoxide radical (O) pathway under neutral conditions. This study provides a fundamental understanding of the in-situ synthesis of HO to mineralize NB by carbon-coated nZVI.
近年来,利用纳米零价铁(nZVI)原位生成过氧化氢(HO)的研究受到了越来越多的关注。然而,nZVI 的利用率低、生产条件严格、能耗高等限制了该技术在实际环境污染修复中的应用。本研究采用碳包覆纳米零价铁(Fe@C)原位合成 HO 并实现对硝基苯(NB)的矿化。结果表明,该复合材料在 120min 内通过吸附、还原和氧化去除了 91%的 NB,其中氧化占 42.92%。不仅如此,该复合材料在 pH 值为 3-7 的宽范围内能够实现对 NB 的有效矿化。羟基自由基(HO)的定量实验表明,该复合材料在 120min 内无需额外的能量消耗即可生成 185.64μM 的 HO。碳包覆结构有效地抑制了 nZVI 表面钝化层的形成,从而保证了 Fe 的高活性。此外,碳涂层通过改变 nZVI 表面的氧还原途径,增强了顺序单电子转移过程,使得 Fe 能够在中性条件下通过超氧自由基(O)途径有效地生成 HO。本研究为碳包覆 nZVI 原位合成 HO 矿化 NB 提供了基础认识。