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界面锚定钴物种介导的高级氧化:有机污染物的降解性能与机制

Interfacial anchoring cobalt species mediated advanced oxidation: Degradation performance and mechanism of organic pollutants.

作者信息

Chen Zidan, Meng Guanghao, Han Zenghui, Li Hongjiang, Chi Shaoming, Hu Guangzhi, Zhao Xue

机构信息

Yunnan Key Laboratory of Modern Separation Analysis and Substance Transformation, College of Chemistry and Chemical Engineering, Yunnan Normal University, Kunming 650500, China.

College of Chemistry Biology and Environment, Yuxi Normal University, Yuxi 653100, China.

出版信息

J Colloid Interface Sci. 2025 Feb;679(Pt B):67-78. doi: 10.1016/j.jcis.2024.10.097. Epub 2024 Oct 20.

Abstract

The development of highly catalytic activity, low-cost and environmentally friendly catalysts is crucial for the use of advanced oxidation processes (AOPs) to treat organic pollutants. In this study, to reduce costs, enhance catalytic activity and avoid secondary pollution form metal ions, pomelo peel was used as raw material, combined with surface crystallization, carbon layer protection and heat treatment technology to effectively construct AOPs catalyst that can efficiently activate peroxymonosulfate (PMS) to degrade harmful organic pollutants. Under the optimal conditions, the Co/BC-PMS system can degrade about 100 % of tetracycline (TC, a spectral antibiotic) within 5 min, and the degradation rate of TC can still reach 100 % even if Co/BC (cobalt anchored on biochar) was reused for 6 times. The Co/BC-PMS system can resist complex environmental conditions, including acidic solution, alkaline solution, coexisting ions, different water quality, and is universal for the degradation of most organic pollutants. The integrated purification column with Co/BC as the core realizes the continuous and complete degradation of organic pollutants and has the ability of practical application. Radical capture and monitoring combined with density-functional-theory calculations confirmed that the Co(111) and amorphous CoO sites in Co/BC are the key to driving PMS to degrade organic pollutants, Co/BC can efficiently adsorb PMS and promote the dissociation of PMS into highly active OH, SO and O, and these reactive oxygen species jointly promote the degradation of organic pollutants. This study provides experimental support and theoretical insights for the design of efficient AOPs catalysts, and plays an important role in promoting the development of AOPs.

摘要

开发具有高催化活性、低成本且环境友好的催化剂对于采用高级氧化工艺(AOPs)处理有机污染物至关重要。在本研究中,为降低成本、提高催化活性并避免金属离子造成二次污染,以柚子皮为原料,结合表面结晶、碳层保护和热处理技术,有效构建了一种能高效活化过一硫酸盐(PMS)以降解有害有机污染物的AOPs催化剂。在最佳条件下,Co/BC - PMS体系在5分钟内可降解约100%的四环素(TC,一种光谱抗生素),即使Co/BC(负载在生物炭上的钴)重复使用6次,TC的降解率仍能达到100%。Co/BC - PMS体系能够抵抗复杂的环境条件,包括酸性溶液、碱性溶液、共存离子、不同水质,并且对大多数有机污染物的降解具有通用性。以Co/BC为核心的集成净化柱实现了有机污染物的连续完全降解,具备实际应用能力。自由基捕获与监测结合密度泛函理论计算证实,Co/BC中的Co(111)和非晶态CoO位点是驱动PMS降解有机污染物的关键,Co/BC能够高效吸附PMS并促进PMS分解为高活性的OH、SO和O,这些活性氧物种共同促进有机污染物的降解。本研究为高效AOPs催化剂的设计提供了实验支持和理论见解,对推动AOPs的发展具有重要作用。

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