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AgSiO/Cu(II)-修饰坡缕石复合材料可见光辅助过硫酸盐活化用于通过自由基和非自由基途径有效降解有机污染物。

Visible-light-assisted peroxydisulfate activation over AgSiO/Cu(II)-modified palygorskite composite for the effective degradation of organic pollutants by radical and nonradical pathways.

机构信息

College of Chemistry & Material Science, Key Laboratory of Synthetic and Natural Functional Molecule of the Ministry of Education, Northwest University, Xi'an 710069, PR China.

State Key Laboratory of Eco-hydraulics in Northwest Arid Region of China, Xi'an University of Technology, Xi'an 710048, PR China.

出版信息

Environ Res. 2022 Nov;214(Pt 4):113970. doi: 10.1016/j.envres.2022.113970. Epub 2022 Aug 18.

DOI:10.1016/j.envres.2022.113970
PMID:35987371
Abstract

Photoassisted persulfate activation (PPA) is highly efficient oxidation process, but the eligible catalysts are scarce. Herein, a visible-light-responsive AgSiO was anchored on Cu(II)-exchanged attapulgite (Cu-Pal) via a facile precipitation-deposition method to construct a novel PDS activator. The synthesized catalyst was systemically analyzed by a series of characterization techniques. The results revealed that AgSiO nanoparticles were evenly dispersed on Cu-Pal to form heterojunction. 16%-AgSiO/Cu-Pal, an optimal catalyst exhibited excellent catalytic performance and stability in the visible-light-assisted PDS activation for AR18 degradation. The influences of reaction parameters on this process were investigated. Under the optimal conditions ([catalyst] = 1.0 g L, [PDS] = 3.9 mM, pH = 5.1), 50 mg L of AR18 was completely degraded within 30 min. More importantly, quenching experiments and EPR tests revealed that besides the common SO and •OH, O and O were generated as main reactive oxygen species in the PPA by 16%-AgSiO/Cu-Pal. Moreover, it was found that surface hydroxyl groups of the catalyst and copper species incorporated in Pal could significantly influence PDS activation and ROS generation. Based on these results, together with PDS decomposition, fluorescent probe analysis, and XPS analysis of the used catalyst, the possible mechanisms of the PPA by 16%-AgSiO/Cu-Pal were proposed. Finally, the versatility and practicability of the established PPA process were verified by degrading other organic contaminants and testing effects of the coexisting anions and water matrices on AR18 degradation. This study may provide new insights for designing and developing the efficient heterogeneous catalysis for wastewater treatment via persulfate-based AOP.

摘要

光辅助过硫酸盐活化(PPA)是一种高效的氧化过程,但合适的催化剂却很稀缺。在此,通过一种简便的沉淀-沉积方法,将负载在 Cu(II)交换坡缕石(Cu-Pal)上的可见光响应型 AgSiO 锚定,构建了一种新型的 PDS 活化剂。通过一系列的表征技术对合成的催化剂进行了系统的分析。结果表明,AgSiO 纳米颗粒均匀分散在 Cu-Pal 上形成了异质结。在可见光辅助 PDS 活化降解 AR18 反应中,16%-AgSiO/Cu-Pal 作为最佳催化剂表现出了优异的催化性能和稳定性。考察了该过程中反应参数的影响。在最佳条件下([催化剂]=1.0 g L,[PDS]=3.9 mM,pH=5.1),50 mg L 的 AR18 在 30 min 内完全降解。更重要的是,猝灭实验和 EPR 测试表明,除了常见的 SO 和 •OH 外,在 16%-AgSiO/Cu-Pal 的 PPA 中还生成了 O 和 O 作为主要的活性氧物质。此外,研究发现催化剂表面的羟基和 Pal 中掺入的铜物种可以显著影响 PDS 的活化和 ROS 的生成。基于这些结果,结合 PDS 分解、荧光探针分析和使用后的催化剂 XPS 分析,提出了 16%-AgSiO/Cu-Pal 光辅助过硫酸盐活化的可能机制。最后,通过降解其他有机污染物和考察共存阴离子和水基质对 AR18 降解的影响,验证了所建立的 PPA 过程的多功能性和实用性。本研究可为基于过硫酸盐的 AOP 设计和开发高效的废水处理异相催化提供新的思路。

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