MgAlFe-Mixed Metal Oxides Derived from Layered Double Hydroxides Enhanced Peroxydisulfate Activation for Ciprofloxacin Degradation via an Electron Transfer Mechanism

IF 3.9 3区 工程技术 Q2 ENGINEERING, CHEMICAL Industrial & Engineering Chemistry Research Pub Date : 2025-04-25 DOI:10.1021/acs.iecr.5c00333
Lihong Cao, Chen Li, Fazhi Zhang, Xiaoxiao Guo, Xiaodong Lei, Yiping Wang
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Abstract

Advanced oxidation processes (AOPs) based on peroxydisulfate (PDS) dominated by the nonradical pathway have aroused great concern in organic pollutant degradation due to the high tolerance to interference. However, secondary pollution caused by leached metal ions remains a scientific challenge for PDS activators that are mainly composed of transition metals. To develop efficient and green metal catalysts for PDS activation, we proposed a coprecipitation combined with calcination approach to prepare MgAlFe-mixed metal oxides (MMOs). MMO-700 obtained by calcination at 700 °C possesses a large specific surface area (213.14 m2/g) and atomically dispersed active sites, which synergistically facilitated the enrichment of abundant ciprofloxacin (CIP) and PDS on the catalyst surface, thereby providing a prerequisite step for PDS activation. This featured system selectively generated the MMO-700/PDS* complex, resulting in an efficient degradation efficiency of 79.7% for CIP with almost no leaching of Fe detected. Impressively, MMO-700 also exhibited excellent environmental adaptability and desirable catalytic efficiency in the PDS* complex-mediated electron transfer process. In addition, CIP degradation involved three possible pathways including the opening and oxidation of the piperazine ring, the opening of the cyclopropyl ring, and the transformation of the quinolone group. This study provides a new strategy for developing efficient and green catalysts to achieve PDS nonradical activation and contribute to wastewater treatment.

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层状双氢氧化物衍生的mgalfe -混合金属氧化物通过电子转移机制增强过硫酸氢盐活化降解环丙沙星
以非自由基途径为主的过硫酸氢盐(PDS)为基础的高级氧化工艺(AOPs)因其对干扰的耐受性强,在有机污染物降解中引起了广泛关注。然而,对于以过渡金属为主的PDS活化剂来说,金属离子浸出造成的二次污染仍然是一个科学难题。为了开发高效、绿色的PDS催化剂,我们提出了共沉淀法结合煅烧法制备mgalfe混合金属氧化物(MMOs)的方法。700℃煅烧得到的MMO-700具有较大的比表面积(213.14 m2/g)和原子分散的活性位点,协同促进了丰富的环丙沙星(CIP)和PDS在催化剂表面的富集,从而为PDS活化提供了先决条件。该系统选择性地生成MMO-700/PDS*络合物,对CIP的高效降解效率为79.7%,几乎没有检测到铁的浸出。令人印象深刻的是,MMO-700在PDS*络合物介导的电子转移过程中也表现出优异的环境适应性和理想的催化效率。此外,CIP的降解还包括哌嗪环的打开和氧化、环丙基环的打开和喹诺酮基的转化三种可能的途径。本研究为开发高效、绿色的催化剂实现PDS非自由基活化和废水处理提供了新的思路。
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来源期刊
Industrial & Engineering Chemistry Research
Industrial & Engineering Chemistry Research 工程技术-工程:化工
CiteScore
7.40
自引率
7.10%
发文量
1467
审稿时长
2.8 months
期刊介绍: ndustrial & Engineering Chemistry, with variations in title and format, has been published since 1909 by the American Chemical Society. Industrial & Engineering Chemistry Research is a weekly publication that reports industrial and academic research in the broad fields of applied chemistry and chemical engineering with special focus on fundamentals, processes, and products.
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