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Fe 和 Zn 共掺杂碳纳米粒子作为过一硫酸盐的高效 2,4-二氯苯酚降解活化剂。

Fe and Zn co-doped carbon nanoparticles as peroxymonosulfate activator for efficient 2,4-dichorophenol degradation.

机构信息

School of Environmental Science and Engineering, Tianjin University, Tianjin, 300350, China.

School of Environmental Science and Engineering, Tianjin University, Tianjin, 300350, China.

出版信息

Environ Res. 2024 Jan 1;240(Pt 1):117313. doi: 10.1016/j.envres.2023.117313. Epub 2023 Oct 20.

DOI:10.1016/j.envres.2023.117313
PMID:37866532
Abstract

Iron-mediated activation of peroxymonosulfate (PMS) has been of great interest for the effective removal of contaminants, but it still suffered from ineffective metal redox cycle rate, which resulted in unsatisfactory catalytic efficiency. Constructing bimetallic carbonaceous materials was effective way to improve the catalytic performance of iron-based heterogeneous system. In this study, magnetic bimetallic porous carbon composite (FZC) was synthesized via Fe/Zn bi-MOFs pyrolysis for 2,4-dichlorophenol (2,4-DCP) degradation by peroxymonosulfate. Influences of different systems exhibited that 100% of 2,4-DCP was rapidly degraded at the conditions of catalyst dosage = 0.1 g L, PMS = 0.5 mM and initial pH = 9.0 within 30 min. The as-prepared FZC displayed excellent reusability and stability. Quenching experiments and EPR analysis manifested that SO and O were primarily responsible for the rapid degradation of 2,4-DCP. Moreover, XPS, EPR and EIS was used to elaborate the bimetallic synergy effect, proving that the introduction of zinc can effectively promote periodic cycle of Fe/Fe and improve catalysts durability and reusability. These findings highlighted the preparation of bimetallic based carbonaceous material with excellent PMS activation ability to remove refractory organics from wastewater and provided a depth insight into the promotion of bimetal synergy between zinc and iron on PMS activation process.

摘要

铁介导的过一硫酸盐(PMS)的活化对于有效去除污染物具有重要意义,但它仍然存在金属氧化还原循环速率低的问题,导致催化效率不理想。构建双金属碳质材料是提高铁基多相体系催化性能的有效方法。本研究通过 Fe/Zn 双金属 MOFs 热解合成了磁性双金属多孔碳复合材料(FZC),用于过一硫酸盐降解 2,4-二氯苯酚(2,4-DCP)。不同体系的影响表明,在催化剂用量为 0.1 g·L、过一硫酸盐为 0.5 mM 和初始 pH 值为 9.0 的条件下,2,4-DCP 在 30 min 内可迅速降解 100%。所制备的 FZC 显示出优异的可重复使用性和稳定性。猝灭实验和 EPR 分析表明,SO 和 O 是 2,4-DCP 快速降解的主要原因。此外,XPS、EPR 和 EIS 用于阐述双金属协同效应,证明锌的引入可以有效促进 Fe/Fe 的周期性循环,提高催化剂的耐久性和可重复使用性。这些发现突出了制备具有优异 PMS 活化能力的双金属基碳质材料,以去除废水中的难处理有机物,并深入了解锌和铁之间的双金属协同作用对 PMS 活化过程的促进作用。

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