锰基负载氮化碳活化过一硫酸盐对4-氯酚的降解效果

doi:10.14088/j.cnki.issn0439-8114.2025.10.013

湖北农业科学 ›› 2025, Vol. 64 ›› Issue (10): 83-93.doi: 10.14088/j.cnki.issn0439-8114.2025.10.013

锰基负载氮化碳活化过一硫酸盐对4-氯酚的降解效果

王莎莎^1a, 崔鹏飞², 阮新潮^1a,1b, 石胜宇^1a, 龙军^1a, 杨小俊^1a,1b

1.武汉纺织大学,a.资源与环境学院;b.纺织印染清洁生产教育部工程研究中心,武汉 430200;
2.北京碧水源科技股份有限公司,北京 102206

收稿日期:2025-04-10 出版日期:2025-10-25 发布日期:2025-11-14
通讯作者: 杨小俊（1974-）,男,副教授,博士,研究方向为污水处理,（电子信箱）xjyang@wtu.edu.cn。
作者简介:王莎莎（2000-）,女,贵州贵阳人,在读硕士研究生,研究方向为水处理,（电子信箱）sswang0819@163.com。
基金资助:
武汉纺织大学校级基金项目（20230627）

Degradation efficiency of 4-chlorophenol by manganese-based loaded carbon nitride activated peroxymonosulfate

WANG Sha-sha^1a, CUI Peng-fei², RUAN Xin-chao^1a,1b, SHI Sheng-yu^1a, LONG Jun^1a, YANG Xiao-jun^1a,1b

1a. School of Resources and Environment; b.Ministry of Education Engineering Research Center for Clean Production in Textile Printing and Dyeing, Wuhan Textile University, Wuhan 430200,China;
2. Beijing Originwater Technology Co., Ltd., Beijing 102206, China

Received:2025-04-10 Published:2025-10-25 Online:2025-11-14

摘要/Abstract

摘要： 针对水体中难降解有机污染物去除率低和二次污染风险高的问题,采用高温煅烧法制备Mn_0.5-CN非均相催化剂,通过活化过一硫酸盐（PMS）实现对4-氯酚（4-CP）的高效降解,且通过多种表征手段分析该催化剂的结构。结果显示,在优化条件（催化剂投加量0.5 g/L、PMS浓度0.8 mmol/L、室温）下,该催化剂在60 min内对20 mg/L的4-CP降解率达95.1%,且总有机碳（TOC）去除率达78.6%。机理研究表明,Mn(Ⅱ)/Mn(Ⅲ)的氧化还原循环在PMS活化过程中起主导作用,其中单线态氧（¹O₂）为主要活性氧物种,羟基自由基（·OH）辅助降解。催化剂在经过5次循环使用后,对4-CP的降解率仍保持在80%以上。此外,该系统具有良好的pH（3~11）适应性和环境适用性（不同水体和阴离子）。该体系通过C-Cl键断裂和芳香环开环反应实现污染物的矿化,为4-CP的处理提供了高效、稳定且环境友好的解决方案。

关键词: 锰基催化剂, 氮化碳, 过一硫酸盐, 4-氯苯酚, 价态循环, 降解效果

Abstract: To address the problems of low removal efficiency and high risk of secondary pollution of difficult-to-degrade organic pollutants in water bodies, a Mn_0.5-CN non-homogeneous catalyst was prepared by high-temperature calcination, and the efficient degradation of 4-chlorophenol (4-CP) was achieved by activating peroxymonosulfate (PMS), and the catalyst was structurally analyzed by various characterization means. The results showed that under the optimized conditions (catalyst dosage of 0.5 g/L, PMS concentration of 0.8 mmol/L, room temperature), the catalyst achieved 95.1% removal of 4-CP at 20 mg/L and 78.6% removal of total organic carbon (TOC) within 60 min. Mechanistic studies showed that the redox cycle of Mn(Ⅱ)/Mn(Ⅲ) played a dominant role in the activation process of PMS, in which single-linear oxygen (¹O₂) was the main active species, and hydroxyl radical (·OH) assisted the degradation. The catalyst maintained more than 80% degradation efficiency after five cycles of use. In addition, the system had good pH（3~11） adaptability and good environmental applicability (different water bodies and anions). This system provided an efficient, stable and environmentally friendly solution for 4-CP treatment by mineralizing pollutants through C-Cl bond breaking and aromatic ring opening reactions.

Key words: manganese-based catalysts, carbon nitride, peroxymonosulfate, 4-chlorophenol, valence cycling, degradation efficiency

中图分类号:

X703.1

王莎莎, 崔鹏飞, 阮新潮, 石胜宇, 龙军, 杨小俊. 锰基负载氮化碳活化过一硫酸盐对4-氯酚的降解效果[J]. 湖北农业科学, 2025, 64(10): 83-93.

WANG Sha-sha, CUI Peng-fei, RUAN Xin-chao, SHI Sheng-yu, LONG Jun, YANG Xiao-jun. Degradation efficiency of 4-chlorophenol by manganese-based loaded carbon nitride activated peroxymonosulfate[J]. HUBEI AGRICULTURAL SCIENCES, 2025, 64(10): 83-93.

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锰基负载氮化碳活化过一硫酸盐对4-氯酚的降解效果

Degradation efficiency of 4-chlorophenol by manganese-based loaded carbon nitride activated peroxymonosulfate

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