复合水凝胶衍生的零价铜催化剂高效活化过硫酸盐降解氯酚
CSTR:
作者:
作者单位:

南京大学 环境学院,南京 210023

作者简介:

刘权(1999- ),男,主要从事重金属吸附研究,E-mail:liuquan21250065@163.com。
LIU Quan (1999- ), main research interest: heavy metal adsorption, E-mail: liuquan21250065@163.com.

通讯作者:

刘福强(通信作者),男,教授,博士生导师,E-mail:lfq@nju.edu.cn。

中图分类号:

X703.1

基金项目:

十二五水专项课题(2014ZX07204-008)


Zero-valent copper catalysts derived from composite hydrogels efficiently activate persulfate for the degradation of chlorophenols
Author:
Affiliation:

School of the Environment, Nanjing University, Nanjing 210023, P. R. China

Fund Project:

Special Project of Water in the 12th Five-Year Plan (No. 2014ZX07204-008)

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    摘要:

    过渡金属/碳复合催化剂能高效活化过硫酸盐(PMS)降解有机污染物。通过简单的热解法成功将吸附Cu(Ⅱ)的复合水凝胶吸附剂转化为零价铜/碳复合催化剂(C-Cu),该催化剂能高效活化PMS并快速降解2,4-二氯苯酚 (2,4-DCP)。在pH值为5、C-Cu投加量为5 mg、PMS浓度为0.20 g/L的条件下,5 min内可完全去除0.1 mmol/L的2,4-DCP,反应动力学常数达3.434 2 min-1,较已报道的金属氧化物催化剂提高3个数量级。在满足《污水综合排放标准》(GB 8978—1996)一级排放标准的条件下,C-Cu可在柱状动态反应器中稳定运行81.3 h。在pH值为5~9、常规无机盐和天然有机质共存的条件下,C-Cu/PMS体系对2,4-DCP的降解未受到明显抑制,表现出良好的环境耐受性。同时,该体系对多种氯酚类污染物均具有优异的去除效果。活性物种淬灭实验及电子顺磁共振波谱(EPR)测试结果一致,表明零价铜作为PMS的活化位点,可产生大量1O2和·O2-。液相色谱-质谱联用分析结果表明,2,4-DCP通过脱氯、开环等过程实现降解与矿化。

    Abstract:

    Transition metal/carbon composite catalysts can effectively activate persulfate (PMS) to degrade organic pollutants. In the present study, a simple pyrolysis technique was used to effectively transform a composite hydrogel adsorbent loaded with Cu(Ⅱ) into a zerovalent copper/carbon composite catalyst (C-Cu), which efficiently activated PMS and rapidly degraded 2,4-dichlorophenol (2,4-DCP). Under conditions of pH= 5, a C-Cu dosage of 5 mg, and PMS concentration of 0.20 g/L, 2,4-DCP (0.1 mmol/L) was completely removed within 5 minutes, with a reaction kinetic constant as high as 3.434 2 min-1, which was 3 orders of magnitude higher than those of reported metal oxides. In compliance with the Integrated Wastewater Discharge Standard (GB 8978—1996) Grade I, C-Cu could stably operate for 81.3 hours in a dynamic column reactor. Under the coexistence conditions of pH=5-9, conventional inorganic salts, and natural organic matter, the degradation of 2,4-DCP in the C-Cu/PMS system was not significantly inhibited, demonstrating good environmental tolerance. Moreover, the C-Cu/PMS system showed superior removal performance for various chlorophenol pollutants. Quenching experiments of active species and EPR results consistently indicated that zerovalent copper acts as the active site for PMS activation, generating a large amount of 1O2 and ·O2-. LC-MS analysis results suggested that 2,4-DCP underwent processes such as dechlorination and ring-opening to achieve degradation and mineralization.

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引用本文

刘权,刘子帆,岳彩良,刘福强.复合水凝胶衍生的零价铜催化剂高效活化过硫酸盐降解氯酚[J].土木与环境工程学报(中英文),2026,48(3):217-227. LIU Quan, LIU Zifan, YUE Cailiang, LIU Fuqiang. Zero-valent copper catalysts derived from composite hydrogels efficiently activate persulfate for the degradation of chlorophenols[J]. JOURNAL OF CIVIL AND ENVIRONMENTAL ENGINEERING,2026,48(3):217-227.10.11835/j. issn.2096-6717.2024.033

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  • 收稿日期:2024-02-28
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  • 在线发布日期: 2026-06-10
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