钢渣强化铁氮多孔碳活化过硫酸盐降解四环素

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摘要通过机械球磨法将由木屑一步热解制成的铁氮多孔碳(PC-_Fe,N)与钢渣(SS)结合得到一种新型磁性铁氮多孔碳/钢渣复合材料(PC-_Fe,N/SS),并用其活化过硫酸盐(PMS)降解四环素(TC).结果表明,在TC初始浓度为20mg/L,PMS和催化剂用量为0.50g/L, pH值为7.0时,PC-_Fe,N/SS/PMS体系在30min内对TC的降解率达87.50%,主要是因为KHCO₃和N掺杂改善了多孔碳的表面孔隙结构和内部电子结构,为PMS提供了更多的反应位点;球磨法协同PC-_Fe,N和SS的功能优势,同时减少了材料表面铁纳米颗粒的团聚现象,促进了PMS活化和TC的降解.VSM和XPS表征结果表明,材料的饱和磁化强度为28.93emu/g,有利于分离回收;Fe⁰和Fe²⁺在降解TC过程中发挥重要作用.自由基淬灭实验与电子顺磁共振(EPR)测试结果揭示了PC-_Fe,N/SS/PMS体系降解TC的主要活性物种是硫酸根自由基(SO₄^•-).

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关键词 ：多孔碳, 铁氮共掺杂, 机械球磨法, 四环素, 催化降解, 过硫酸盐

Abstract：A new magnetic iron-nitrogen porous carbon with steel slag composite (PC-_Fe,N/SS) was obtained by combining iron-nitrogen porous carbon (PC-_Fe,N) made from wood chips with steel slag (SS) by a mechanical ball milling method to degrade tetracycline (TC) with its activated peroxymonosulfate (PMS). The results showed that the TC degradation rate of PC-_Fe,N/SS/PMS system was 87.50% at initial TC concentration of 20mg/L, PMS and catalyst dosage of 0.50g/L, and pH value of 7.0 within 30min. This was mainly because the surface pore structure and internal electronic structure of porous carbon were improved by KHCO₃ and N doping, which provided more reaction sites for PMS; the functional advantages of PC-_Fe,N and SS were synergized by the ball milling method, while the agglomeration of Fe nanoparticles on the surface of the material were reduced, which promoted the activation of PMS and the degradation of TC. The VSM and XPS characterization results showed that the saturation magnetization intensity of the material was 28.93emu/g, which was favorable for the separation and recovery; Fe⁰ and Fe²⁺ played an important role in the degradation of TC. The results of radical quenching experiments and electron paramagnetic resonance (EPR) tests revealed that the main active species in the degradation of TC by the PC-_Fe,N/SS/PMS system was the sulfate radical (SO₄^•-).

Key words： porous carbon iron-nitrogen co-doping mechanical ball milling method tetracycline catalytic degradation peroxymonosulfate

收稿日期: 2022-11-16

PACS:

X703.5

基金资助:国家自然科学基金项目(42220104005,42207101);陕西省重点研发计划项目(2022ZDLSF06-06);陕西省自然科学基础研究计划项目(2021JM-152,2021JM-153);大学生创新创业训练计划创新训练项目(G202210710067)

通讯作者: 卫潇,副教授,chdwx@chd.edu.cn E-mail: chdwx@chd.edu.cn

作者简介: 陈爱侠(1967-),女,陕西富平人,副教授,博士,主要从事水污染控制和生态修复研究.发表论文50余篇.aixiach@chd.edu.cn

引用本文:

陈爱侠, 雷婵娟, 田铮, 卫潇, 王宁, 杨旭麟. 钢渣强化铁氮多孔碳活化过硫酸盐降解四环素[J]. 中国环境科学, 2023, 43(6): 2853-2863. CHEN Ai-xia, LEI Chan-juan, TIAN Zheng, WEI Xiao, WANG Ning, YANG Xu-lin. Steel slag enhanced iron-nitrogen porous carbon activated peroxymonosulfate to degrade tetracycline. CHINA ENVIRONMENTAL SCIENCECE, 2023, 43(6): 2853-2863.

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http://www.zghjkx.com.cn/CN/ 或 http://www.zghjkx.com.cn/CN/Y2023/V43/I6/2853

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