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铁酸镍负载杉木屑生物炭活化过一硫酸盐降解磷酸氯喹

王俊辉 张菁玮 孙静 鄢经缘 徐梓淞 江露莹 黄燕 韩彪 张寒冰 郝格日乐 何思静 朱华凤

王俊辉, 张菁玮, 孙静, 等. 铁酸镍负载杉木屑生物炭活化过一硫酸盐降解磷酸氯喹[J]. 复合材料学报, 2023, 42(0): 1-14.
引用本文: 王俊辉, 张菁玮, 孙静, 等. 铁酸镍负载杉木屑生物炭活化过一硫酸盐降解磷酸氯喹[J]. 复合材料学报, 2023, 42(0): 1-14.
WANG Junhui, ZHANG Jingwei, SUN Jing, et al. Preparation of nickel ferrite loaded fir sawdust biochar to activate peroxymonosulfate for Chloroquine Phosphate degradation[J]. Acta Materiae Compositae Sinica.
Citation: WANG Junhui, ZHANG Jingwei, SUN Jing, et al. Preparation of nickel ferrite loaded fir sawdust biochar to activate peroxymonosulfate for Chloroquine Phosphate degradation[J]. Acta Materiae Compositae Sinica.

铁酸镍负载杉木屑生物炭活化过一硫酸盐降解磷酸氯喹

基金项目: 国家自然科学基金(No. 52263029); 广西自然科学基金(No. 2020GXNSFAA297036); 广西石化资源加工及过程强化技术重点实验室主任基金(No. 2022Z005)
详细信息
    通讯作者:

    张寒冰,博士,副教授,硕士生导师,研究方向为: 环保材料制备及水污染修复 E-mail: 24346260@qq.com

  • 中图分类号: X703;TB332

Preparation of nickel ferrite loaded fir sawdust biochar to activate peroxymonosulfate for Chloroquine Phosphate degradation

Funds: National Natural Science Foundation of China (No. 52263029); National Natural Science Foundation of Guangxi (No. 2020GXNSFAA297036); Petrochemical Resources Processing and Process Reinforcement Technology Key Laboratory Project of Guangxi province (No. 2022Z005)
  • 摘要: 近年来,磷酸氯喹(Chloroquine Phosphate, CQP)作为治疗新冠的特效药得到广泛应用,并且由于其具有优异的抗炎症和抗疟疾能力,在疫情结束后仍发挥着重要作用。磷酸氯喹的大量使用对环境造成严重的潜在危害。将废弃的木屑资源化利用,通过共沉淀-无氧煅烧法制备出具有磁回收能力的铁酸镍负载杉木屑生物炭复合材料(Nickel ferrate loaded biochar, NiFe2O4@BC),并研究其活化过一硫酸盐(Peroxymonosulfate, PMS)降解CQP的性能。利用多种表征对NiFe2O4@BC复合材料的组成结构、表面官能团和石墨化程度进行分析,相较于未改性的杉木屑生物炭(Fir sawdust biochar, BC),将具有磁性NiFe2O4的负载在生物炭上,使得复合材料的石墨化程度提高,缺陷活性位点也得到增多,对CQP的去除效果得到巨大提高。主要考察了NiFe2O4@BC投加量、PMS浓度、溶液初始pH、共存无机阴离子与腐殖酸在降解CQP过程中的影响。研究表明,当NiFe2O4@BC投加量为0.5 g/L,PMS浓度为1.0 mmol/L,CQP浓度为10 mg/L的条件下,CQP去除率在120分钟达到89%。在偏酸性或者偏碱的条件下更有利于CQP的降解,腐殖酸(Humic acid, HA)对NiFe2O4@BC活化PMS降解CQP具有促进作用。淬灭实验证实,自由基途径和非自由基途径生成的•OH与1O2主导了NiFe2O4@BC/PMS体系对CQP的降解。在同等条件下,对多种污染物均能达到80%以上的降解效果。此外,NiFe2O4@BC循环使用5次后,活化PMS去除CQP的效率仍能达到74%左右。本研究为废弃杉木屑高效、绿色的资源化利用提供了新策略和借鉴意义。

     

  • 图  1  杉木屑生物炭(BC) (a)、NiFe2O4 (b)、NiFe2O4@BC (c)和5次循环后NiFe2O4@BC (d)的的SEM图谱

    Figure  1.  SEM images of Fir sawdust biochar (BC) (a), NiFe2O4 (b), NiFe2O4@BC (c) and NiFe2O4@BC after 5 cycles of recycling (d).

    图  2  BC和NiFe2O4@BC的氮气吸附脱附曲线(a)和孔径分布图(b)

    Figure  2.  N2 adsorption-desorption isotherms(a) and Pore size distribution(b) of BC and NiFe2O4@BC.

    图  3  BC、NiFe2O4、NiFe2O4@BC和5次循环后NiFe2O4@BC的XRD谱图

    Figure  3.  XRD patterns of BC, NiFe2O4, NiFe2O4@BC and NiFe2O4@BC after 5 cycles of recycling

    图  4  BC、NiFe2O4、NiFe2O4@BC和5次循环后NiFe2O4@BC的FT-IR图谱(a),XPS全谱图(b),C 1s谱图(c)和N 1s谱图(d).

    Figure  4.  FT-IR spectra (a)、Full spectrum of XPS spectra(b)、 C 1s spectra(c) and O 1s spectra(d) of BC, NiFe2O4, NiFe2O4@BC and NiFe2O4@BC after 5 cycles of recycling

    图  5  BC和NiFe2O4@BC的拉曼光谱

    Figure  5.  Raman spectra of BC and NiFe2O4@BC

    图  6  NiFe2O4@BC降解CQP前后的磁滞回线

    Figure  6.  The hysteresis loops of NiFe2O4@BC and NiFe2O4@BC after 5 cycles of recycling

    图  7  不同材料吸附(a)和活化PMS (b)去除CQP的性能

    Figure  7.  Adsorption (a) and degradation via PMS activation (b) by different materials for CQP removal.

    图  8  NiFe2O4@BC投加量(a)和PMS浓度(b)对CQP降解的影响

    Figure  8.  Effect of NiFe2O4@BC dosage (a) and PMS concentrations (b) for CQP degradation

    图  9  不同初始pH (a)、阴阳离子和腐殖酸(b)对NiFe2O4@BC活化PMS降解CQP的影响

    Figure  9.  Effect of initial pH (a), ions and humic acid (b) by NiFe2O4@BC activated PMS for CQP degradation

    图  10  不同淬灭剂对NiFe2O4@BC活化PMS降解CQP的影响

    Figure  10.  Effects of different trapping agents by NiFe2O4@BC activated PMS for CQP degradation

    图  11  NiFe2O4@BC活化PMS对不同有机污染物的降解(a)和对CQP的5次循环降解效果(b)

    Figure  11.  Degradation effect of NiFe2O4@BC activated PMS on different organic pollutants(a) and five cycles of CQP (b)

    图  12  NiFe2O4@BC反应前后的Fe 2 p(a)和Ni 2 p(b)轨道图谱、NiFe2O4@BC /PMS体系去除CQP的机制(c)和CQP及其中间产物的发育毒性(d)

    Figure  12.  Fe 2 p(a) and Ni 2 p(b) spectra before and after NiFe2O4@BC use , Mechanism of CQP removal by NiFe2O4@BC/PMS system(c) and Developmental toxicity of CQP and their intermediate products(d)

    图  13  CQP在NiFe2O4@BC活化PMS体系中的降解途径

    Figure  13.  Degradation pathway of CQP in NiFe2O4@BC activated PMS system

    表  1  BC和NiFe2O4@BC比表面积和孔隙结构

    Table  1.   Specific surface area and pore structure of BC and NiFe2O4@BC

    Sample Surface
    Area /(m2∙g−1)
    Pore volume/
    (cm3∙g−1)
    Average pore
    diameter/nm
    BC 5.702 0.008 9.404
    NiFe2O4@BC 94.712 0.065 9.539
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  • 收稿日期:  2023-10-11
  • 修回日期:  2023-11-13
  • 录用日期:  2023-12-09
  • 网络出版日期:  2023-12-28

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