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木质垃圾与废铁泥制备Fe0-BC材料及其对水中Cr(Ⅵ)的去除行为

陈超 刘建国 赵光琪 刘美佳 李丽

陈超, 刘建国, 赵光琪, 刘美佳, 李丽. 木质垃圾与废铁泥制备Fe0-BC材料及其对水中Cr(Ⅵ)的去除行为[J]. 环境科学研究, 2023, 36(5): 995-1005. doi: 10.13198/j.issn.1001-6929.2023.02.12
引用本文: 陈超, 刘建国, 赵光琪, 刘美佳, 李丽. 木质垃圾与废铁泥制备Fe0-BC材料及其对水中Cr(Ⅵ)的去除行为[J]. 环境科学研究, 2023, 36(5): 995-1005. doi: 10.13198/j.issn.1001-6929.2023.02.12
CHEN Chao, LIU Jianguo, ZHAO Guangqi, LIU Meijia, LI Li. Preparation of Fe0-BC Using Wood Waste and Iron Sludge and Its Application for Removing Cr(Ⅵ)[J]. Research of Environmental Sciences, 2023, 36(5): 995-1005. doi: 10.13198/j.issn.1001-6929.2023.02.12
Citation: CHEN Chao, LIU Jianguo, ZHAO Guangqi, LIU Meijia, LI Li. Preparation of Fe0-BC Using Wood Waste and Iron Sludge and Its Application for Removing Cr(Ⅵ)[J]. Research of Environmental Sciences, 2023, 36(5): 995-1005. doi: 10.13198/j.issn.1001-6929.2023.02.12

木质垃圾与废铁泥制备Fe0-BC材料及其对水中Cr(Ⅵ)的去除行为

doi: 10.13198/j.issn.1001-6929.2023.02.12
基金项目: 国家重点研发计划项目(No.2018YFC1902906,2019YFC1906900)
详细信息
    作者简介:

    陈超(1990-),男,江西吉安人,助理研究员,博士,主要从事固体废物热处理方向研究,chen.chao@craes.org.cn

    通讯作者:

    ①刘建国(1972-),男,甘肃武威人,教授,博士,博导,主要从事固体废物综合治理研究,jgliu@tsinghua.edu.cn

    ②李丽(1975-),女,河北献县人,研究员,博士,主要从事固体废物环境管理与污染控制研究,li_li@craes.org.cn

  • 中图分类号: X705

Preparation of Fe0-BC Using Wood Waste and Iron Sludge and Its Application for Removing Cr(Ⅵ)

Funds: National Key Research and Development Program of China (No.2018YFC1902906, 2019YFC1906900)
  • 摘要: 含铬废水的直接排放会对自然环境造成严重危害. 为探究零价铁-生物炭材料(Fe0-BC)与Cr(Ⅵ)的反应效能,以木质垃圾与印染行业废铁泥两种亟需处理的固体废物作为原料,在不同温度下通过碳热还原制备Fe0-BC,并将其应用于水中Cr(Ⅵ)的去除. 材料表征结果表明,1 200 ℃下制备的Fe0-BC材料(Fe0-BC-1200)性能最佳,其比表面积为105.6 m3/g,孔径为6.23 nm,物相主要由Fe0、Cu0、C以及少量杂质构成,其中Fe0以球状的颗粒形式分散附着在碳的孔结构中,且大小均匀,粒度基本达到纳米级. 通过静态试验考察了Fe0-BC材料对Cr(Ⅵ)的去除过程,发现Fe0-BC-1200对Cr(Ⅵ)的去除效果最好,在初始浓度为20 mg/L、初始pH为3.5、投加量为2.5 g/L的条件下,Cr(Ⅵ)的去除率达到95.2%. Cr(Ⅵ)的去除过程符合准二级反应动力学过程和Langmuir等温吸附模型(R2>0.99),最大吸附量为10.71 mg/g. Cr(Ⅵ)的去除是包含吸附、还原以及络合沉淀等共同作用的结果,此外,Cu0的存在有利于催化Fe0的氧化,从而促进Cr(Ⅵ)的去除. 研究显示,利用固体废物制备的Fe0-BC材料成本低且对于含Cr(Ⅵ)废水的解毒效果显著,是实现“以废治废”的环境治理新思路.

     

  • 图  1  不同温度下Fe0-BC材料的氮气吸附-脱附等温线

    Figure  1.  N2 adsorption/desorption isotherms of Fe0-BC synthesized at different temperatures

    图  2  Fe0-BC-1200的扫描电镜图及元素分布

    Figure  2.  SEM images and element distribution of Fe0-BC-1200

    图  3  不同温度下制备材料对Cr(Ⅵ)的去除效果

    Figure  3.  Removal efficiency on Cr(Ⅵ) using Fe0-BC synthesized at different temperatures

    图  4  不同BC材料和铁粉对Cr(Ⅵ)的去除效果

    Figure  4.  Removal efficiency on Cr(Ⅵ) using various BC and iron powder

    图  5  Fe0-BC-1200材料的Zeta电位

    Figure  5.  Zeta potential of Fe0-BC-1200

    图  6  初始pH对Cr(Ⅵ)去除效果的影响

    Figure  6.  Effects of initial solution pH on removal efficiency on Cr(Ⅵ)

    图  7  Fe0-BC-1200去除Cr(Ⅵ)过程中吸附量随时间的变化及其动力学方程拟合结果

    Figure  7.  Adsorption capacities of Fe0-BC-1200 on Cr(Ⅵ) with time and kinetic equation fitting

    图  8  Fe0-BC-1200去除Cr(Ⅵ)过程中的平衡吸附量随初始浓度的变化及其吸附等温线方程拟合结果

    Figure  8.  Equilibrium adsorption capacities of Fe0-BC-1200 on Cr(Ⅵ) with initial concentration and Langmuir and Freundlich equations equation fitting

    图  9  反应体系中pH随时间的变化

    Figure  9.  The curve of pH value with time in reaction system

    图  10  Fe0-BC-1200材料作用 Cr(Ⅵ)溶液前后的XRD图谱

    Figure  10.  XRD patterns of Fe0-BC-1200 before and after removal of Cr(Ⅵ)

    图  11  Fe0-BC-1200材料作用 Cr(Ⅵ)溶液前后的XPS图谱和Cr 2p轨道拟合光谱

    Figure  11.  XPS spectrum and Cr 2p fitting curve of Fe0-BC-1200 before and after removal of Cr(Ⅵ)

    图  12  Fe0-BC-1200材料去除Cr(Ⅵ)的机理示意

    Figure  12.  Mechanism diagram of Cr(Ⅵ) removal using Fe0-BC-1200

    表  1  不同温度下制备的Fe0-BC材料主要元素含量

    Table  1.   Main element content of Fe0-BC synthesized at different temperatures

    温度/ºC主要物相含量/%
    TFeFe0CCu
    平均值标准差平均值标准差平均值标准差平均值标准差
    800 Fe3O4、CuO、C 19.4 0.6 0.0 0.0 51.3 1.5 9.6 0.6
    900 Fe3O4、CuFeO2、C 21.6 0.8 0.0 0.0 50.1 1.8 10.1 0.7
    1 000 Fe3O4、Cu、C 22.8 1.6 1.1 0.2 49.2 2.1 10.8 1.1
    1 100 Fe3O4、Cu、Fe、C 24.3 1.6 15.8 1.1 48.2 0.9 11.1 0.6
    1 200 Cu、Fe、C 27.1 1.2 25.8 0.7 46.7 1.2 11.8 0.5
    下载: 导出CSV

    表  2  不同温度下制备的Fe0-BC材料的孔结构参数

    Table  2.   Pore structure parameters Fe0-BC synthesized at different temperatures

    温度/ºC比表面积/(m2/g)孔径/nm孔体积/(cm3/g)
    平均值标准差平均值标准差平均值标准差
    800156.13.74.120.50.230.02
    900137.64.24.220.30.210.02
    1 000119.16.65.170.40.170.04
    1 100109.84.96.110.10.160.03
    1 200105.64.36.230.30.140.01
    下载: 导出CSV

    表  3  Fe0-BC材料制备吨成本

    Table  3.   Fe0-BC preparation cost per ton

    类别成本/元质量/t吨成本/元备注
    建设投资 333 年投资200×104元,年运行300 d
    人工成本 100 10人,平均年薪6×104
    设备折旧及维修 33 10年折旧年限
    木质垃圾运输费 45.91 0.74 34 运输距离10 km
    废铁泥运输费 54.71 1.48 81 运输距离30 km
    破碎处理耗能 399.00 0.74 295 吨成品消耗0.74 t木质垃圾,吨耗量约为550 kW·h
    热处理耗能 522.00 2.22 1 159 吨成品消耗2.22 t总原料,吨耗量720 kW·h
    磨细处理耗能 435.00 1.00 435 吨耗量600 kW·h
    合计 2 570
    下载: 导出CSV

    表  4  Fe0-BC-1200去除Cr(Ⅵ)的吸附动力学参数

    Table  4.   Kinetics parameters for sorption of Fe0-BC-1200 on Cr(Ⅵ)

    准一级动力学方程准二级动力学方程
    qe/(mg/g)k1/min−1R2qe/(mg/g)k2/[g/(mg·min)]R2
    4.810.0370.9428.020.0130.995
    下载: 导出CSV

    表  5  Fe0-BC-1200去除Cr(Ⅵ)的吸附等温线参数

    Table  5.   Adsorption isotherm parameters for sorption of Fe0-BC-1200 on Cr(Ⅵ)

    Langmuir等温吸附模型Freundlich等温吸附模型
    qmax/(mg/g)kL/(L/mg)R2nkF/(mg/g)R2
    10.710.770.9994.455.2060.731
    下载: 导出CSV
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  • 收稿日期:  2022-11-17
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