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Nonradical activation of Oxone over Fe-doped nitrogen carbon (Fe@NC) armor catalysts for efficient degradation of anthropogenic phenolics (p-nitrophenol, 4-chlorophenol) in groundwater matrices
Chemical Engineering Journal ( IF 13.3 ) Pub Date : 2023-10-24 , DOI: 10.1016/j.cej.2023.146920
Lei Su , Yifan Li , Zhenkai Wang , Yao-Yin Lou , Qi-Zheng Zheng , Zhangxiong Wu , Sheng-Peng Sun
Chemical Engineering Journal ( IF 13.3 ) Pub Date : 2023-10-24 , DOI: 10.1016/j.cej.2023.146920
Lei Su , Yifan Li , Zhenkai Wang , Yao-Yin Lou , Qi-Zheng Zheng , Zhangxiong Wu , Sheng-Peng Sun
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Iron-based catalysts are widely used in peroxysulfate-based AOPs but suffering from low catalytic performance at neutral pH conditions, which limits the application in groundwater remediation. Herein, this study investigated the efficacy, mechanism and long-term durability of Fe-doped nitrogen carbon (Fe@NC) armor catalysts toward peroxysulfate activation for the degradation of anthropogenic phenolics (APs) in groundwater matrices. The results showed that nonradical activation of Oxone (i.e., HSO5 – ) was obtained over the as-prepared Fe-3 % @NC-700 catalyst, high-valent Fe species ( Fe(IV) O) and 1 O2 were identified as the dominant reactive species for the efficient degradation of APs by experiments and density functional theory (DFT) calculations. Notably, the DFT results indicated that HSO5 – was favorably adsorbed on the Fe atoms owing to the electrostatic interaction, which transformed exothermically into SO4 2– and 1 O2 over Fe3 C, accompanied by the generation of Fe(IV) O. Additionally, the Fe-3 % @NC-700 catalyst displayed long-term activity for in situ activation of Oxone in groundwater matrices without pH adjustment, resulting in ΔAPs: ΔOxone stoichiometry efficiencies at 4.2–5.0 % . Wheat seeds germination tests revealed that the biotoxicity of the treated water was reduced notably by the present catalytic system, which holds large potential application in treatment of APs-contaminated groundwater.
中文翻译:
Oxone on Fe 掺杂氮碳 (Fe@NC) 装甲催化剂的非自由基活化,用于高效降解地下水基质中的人为酚类物质(对硝基苯酚、4-氯苯酚)
铁基催化剂广泛用于基于过氧硫酸盐的 AOP,但在中性 pH 条件下催化性能低,这限制了在地下水修复中的应用。在此,本研究研究了 Fe 掺杂氮碳 (Fe@NC) 装甲催化剂对过硫酸盐活化降解地下水基质中人为酚类物质 (AP) 的功效、机制和长期持久性。结果表明,在制备的 Fe-3 % @NC-700 催化剂上获得了 Oxone (即 HSO5–) 的非自由基活化,通过实验和密度泛函理论 (DFT) 计算确定高价 Fe 物种 (Fe(IV)O) 和 1O2 是高效降解 AP 的主要反应物种。值得注意的是,DFT 结果表明,由于静电相互作用,HSO5– 被很好地吸附在 Fe 原子上,静电相互作用在 Fe3C 上放热转化为 SO42– 和 1O2,并伴有 Fe(IV)O 的产生。此外,Fe-3 % @NC-700 催化剂在地下水基质中显示出对 Oxone 的原位活化的长期活性,无需调节 pH 值, 导致 ΔAPs:ΔOxone 化学计量效率为 4.2–5.0 %。小麦种子发芽试验表明,目前的催化系统显著降低了处理水的生物毒性,这在处理 APs 污染的地下水中具有很大的潜在应用。
更新日期:2023-10-24
中文翻译:

Oxone on Fe 掺杂氮碳 (Fe@NC) 装甲催化剂的非自由基活化,用于高效降解地下水基质中的人为酚类物质(对硝基苯酚、4-氯苯酚)
铁基催化剂广泛用于基于过氧硫酸盐的 AOP,但在中性 pH 条件下催化性能低,这限制了在地下水修复中的应用。在此,本研究研究了 Fe 掺杂氮碳 (Fe@NC) 装甲催化剂对过硫酸盐活化降解地下水基质中人为酚类物质 (AP) 的功效、机制和长期持久性。结果表明,在制备的 Fe-3 % @NC-700 催化剂上获得了 Oxone (即 HSO5–) 的非自由基活化,通过实验和密度泛函理论 (DFT) 计算确定高价 Fe 物种 (Fe(IV)O) 和 1O2 是高效降解 AP 的主要反应物种。值得注意的是,DFT 结果表明,由于静电相互作用,HSO5– 被很好地吸附在 Fe 原子上,静电相互作用在 Fe3C 上放热转化为 SO42– 和 1O2,并伴有 Fe(IV)O 的产生。此外,Fe-3 % @NC-700 催化剂在地下水基质中显示出对 Oxone 的原位活化的长期活性,无需调节 pH 值, 导致 ΔAPs:ΔOxone 化学计量效率为 4.2–5.0 %。小麦种子发芽试验表明,目前的催化系统显著降低了处理水的生物毒性,这在处理 APs 污染的地下水中具有很大的潜在应用。