合成具有三维开孔结构的 CuO-PEI-JE 作为过二硫酸盐的高效异质活化剂用于苯酚降解。

IF 7.7 2区 环境科学与生态学 Q1 ENVIRONMENTAL SCIENCES Environmental Research Pub Date : 2024-11-06 DOI:10.1016/j.envres.2024.120308
Shengli Zhang , Zhili Du , Mingxi Wang , Diyang Yu , Yiyue Yang , Maohong Li , Weizhen Fang , Junmin Chen
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引用次数: 0

摘要

异相催化体系的核心是设计高性能的异相催化剂。本研究在交联法制备的三维结构 PEI-JE 上原位沉淀 CuO,合成了 CuO-PEI-JE。它具有大尺寸和三维开孔结构,易于分离,对 PDS 的活化具有超强性能。与单独的 PDS(0.0017 min-1)相比,CuO-PEI-JE + PDS + NaHCO3 系统的 kobs(0.3526 min-1)提高了 207 倍,20 分钟内苯酚降解率达到 100%,30 分钟内 TOC 去除率达到 87%。该系统在苯酚降解方面的表现优于许多其他已发表的过硫酸盐异构系统。同时,所开发的系统在阴离子或不同水基质共存的情况下表现出良好的抗干扰能力。在连续五个循环后,降解率仍保持在 100%,显示出 CuO-PEI-JE 极佳的可重复使用性。此外,CuO-PEI-JE 的制备具有制备条件温和(60 °C)、原料易得等优点。活化机理主要涉及活性 PDS 的形成及其进一步分解为-OHads、SO4--ads、O2--和 1O2。表面官能团和苯酚是活性 PDS 的电子供体。苯酚首先被降解为六二烯二酸,然后被氧化为丙烷二酸和草酸,最后矿化为 CO2 和 H2O。这项工作为制备有效的异质过硫酸盐活化剂提供了一种新策略,在处理含酚废水方面具有很大的潜力。
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Synthesized CuO-PEI-JE with 3D open-cell structure as an efficient heterogeneous activator of peroxodisulfate for phenol degradation
The core of heterogeneous catalytic systems is to design high-performance heterogeneous catalysts. In the present study, CuO-PEI-JE was synthesized via in situ precipitation of CuO on the 3D structure of PEI-JE prepared by a cross-linking method. It possessed a macro-size and 3D open-cell structure, being easily separated and having super-performance for PDS activation. Compared to PDS alone (0.0017 min−1), the CuO-PEI-JE + PDS + NaHCO3 system increased the kobs (0.3526 min−1) by a factor of 207 with 100% phenol degradation within 20 min and 87% TOC removal at 30 min. It outperformed many other published heterogeneous persulfate systems in phenol degradation. Meanwhile, the developed system displayed a good anti-interference ability in the coexistence of anions or different water matrixes. After five successive cycles, the degradation rate still kept 100%, exhibiting the excellent reusability of CuO-PEI-JE. Furthermore, the preparation of CuO-PEI-JE had the advantages with moderate preparation conditions (60 °C) and readily available raw materials. The activation mechanism was mainly involved in the formation of active PDS and its further decomposition into ·OHads, SO4·ads, O2·- and 1O2. Surface functional groups and phenol acted as electron donors for active PDS. Phenol was first degraded into hexadienedioic acid, then oxidized to propane diacid and oxalic acid, and finally mineralized into CO2 and H2O. This work provides a new strategy for preparing effective heterogeneous persulfate activators and has high potential for the treatment of phenol-containing wastewater.
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来源期刊
Environmental Research
Environmental Research 环境科学-公共卫生、环境卫生与职业卫生
CiteScore
12.60
自引率
8.40%
发文量
2480
审稿时长
4.7 months
期刊介绍: The Environmental Research journal presents a broad range of interdisciplinary research, focused on addressing worldwide environmental concerns and featuring innovative findings. Our publication strives to explore relevant anthropogenic issues across various environmental sectors, showcasing practical applications in real-life settings.
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