Cobalt doped g-C3N4 activated peroxymonosulfate for organic pollutant degradation: Alterations in cobalt species and reactive oxygen species

IF 8.1 2区 环境科学与生态学 Q1 ENVIRONMENTAL SCIENCES Chemosphere Pub Date : 2024-12-01 DOI:10.1016/j.chemosphere.2024.143763
Yuesen Wang , Yanchun Huang , Yi Chen , Luming Dou , Yi Ren , Naiwen Li , Bo Lai , Bo Tan
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Abstract

Cobalt-based materials are promising catalysts for activating peroxymonosulfate (PMS) to degrade organic pollutants. Among various cobalt-based catalysts, the alteration in cobalt species and the reactive species produced are not fully understood. Herein, four materials were synthesized by controlling synthesis methods and doping of g-C3N4 to regulate cobalt species. Through two methods, ZIF/Co and Co3O4, whose main cobalt species are Co–O/Co–N and CoO/O–CoO, were synthesized. On this basis, ZIF/Co–CN and Co3O4–CN were synthesized by adding g-C3N4. Then, the four materials were used to activate PMS for carbamazepine (CBZ) degradation, focusing on the correlation between active sites and reactive species. CoO/O–CoO mainly led to the formation of free radicals, while Co–N tended to produce non-free radicals. The addition of g-C3N4 would facilitate non-free radical catalysis by promoting the conversion of Co–O to Co–N and enhancing the catalytic role of C and N. Finally, the systems with a high proportion of non-free radicals showed better degradation performance when multiple pollutants co-existed, and reactive species may be selective to different pollutants. The findings have significance for the synthesis design of cobalt-based catalysts and the regulation of reactive species to degrade different pollutants practically.

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掺钴 g-C3N4 活化过硫酸盐降解有机污染物:钴物种和活性氧物种的变化。
钴基材料是一种很有前景的催化剂,可激活过一硫酸盐(PMS)降解有机污染物。在各种钴基催化剂中,钴物种的变化和产生的活性物种尚未完全清楚。本文通过控制合成方法和 g-C3N4 的掺杂来调节钴的种类,合成了四种材料。通过两种方法合成了 ZIF/Co 和 Co3O4,其主要钴物种为 Co-O/Co-N 和 Co=O/O-Co=O。在此基础上,加入 g-C3N4 合成了 ZIF/Co-CN 和 Co3O4-CN。然后,将这四种材料用于活化 PMS 以降解卡马西平(CBZ),重点研究了活性位点与反应物之间的相关性。Co=O/O-Co=O 主要导致自由基的形成,而 Co-N 则倾向于产生非自由基。最后,当多种污染物共存时,非自由基比例高的体系表现出更好的降解性能,而反应物种可能对不同污染物具有选择性。这些发现对钴基催化剂的合成设计和调节反应物种类以实际降解不同污染物具有重要意义。
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来源期刊
Chemosphere
Chemosphere 环境科学-环境科学
CiteScore
15.80
自引率
8.00%
发文量
4975
审稿时长
3.4 months
期刊介绍: Chemosphere, being an international multidisciplinary journal, is dedicated to publishing original communications and review articles on chemicals in the environment. The scope covers a wide range of topics, including the identification, quantification, behavior, fate, toxicology, treatment, and remediation of chemicals in the bio-, hydro-, litho-, and atmosphere, ensuring the broad dissemination of research in this field.
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