木质垃圾与废铁泥制备Fe<sup>0</sup>-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

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

陈超^1,,
刘建国^2, ,,
赵光琪²,
刘美佳¹,
李丽^1, ,

1.
中国环境科学研究院固体废物污染控制技术研究所，北京　100012
2.
清华大学环境学院，北京　100084

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
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- 被引次数: 0
出版历程
- 收稿日期: 2022-11-17
- 修回日期: 2023-02-10

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

CHEN Chao^1
,,
LIU Jianguo^{2
, ,},
ZHAO Guangqi²,
LIU Meijia¹,
LI Li^{1
, ,}

1.
Research Institute of Solid Waste Management, Chinese Research Academy of Environmental Sciences, Beijing 100012, China
2.
School of Environment, Tsinghua University, Beijing 100084, China

Funds: National Key Research and Development Program of China (No.2018YFC1902906, 2019YFC1906900)

摘要

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.
- 木质垃圾 /
- 废铁泥 /
- 碳热还原 /
- 零价铁-生物炭材料 /
- Cr(Ⅵ)
Abstract: If chromium containing wastewater is directly discharged, it will cause serious harm to the natural environment. In order to explore the reaction efficiency of zero-valent iron/biochar (Fe⁰-BC) and Cr(Ⅵ), the Fe⁰-BC was synthesized by the carbothermal reduction of wood waste and printing and dyeing industry iron sludge at different temperatures and applied to remove Cr(Ⅵ) in water. The characteristics of Fe⁰-BC were determined by specific surface area analyzer and scanning electron microscope (SEM), and the results showed that the Fe⁰-BC-1200 prepared at 1200 ℃ had the best performance, with a specific surface area of 105.6 m³/g and a pore diameter of 6.23 nm. The Fe⁰-BC-1200 was mainly composed of Fe⁰, Cu⁰, C and a small amount of impurities. Fe⁰ particles were dispersed and attached in the pore structure of carbon as spherical particles with uniform size distribution at the nanometer level. Furthermore, the removal process of Cr(Ⅵ) by Fe⁰-BC was studied through batch experiments. The Fe⁰-BC-1200 showed the best removal performance, and the removal rate of Cr(Ⅵ) could reach 95.2% under the conditions of initial concentration of 20 mg/L, initial pH value of 3.5 and dosage of 2.5 g/L. The removal process of Cr(Ⅵ) was well predicted by the pseudo-second-order model and Langmuir equation (R²> 0.99), and the maximum adsorption capacity was 10.71 mg/g. The removal mechanisms mainly included adsorption, reduction and complex precipitation. In addition, the presence of Cu⁰ was beneficial to catalyze the oxidation of iron, thus promoting the removal of Cr(Ⅵ). The Fe⁰-BC prepared with solid waste has the advantages of low cost and significant detoxification effect on Cr(Ⅵ)-containing wastewater, which is a new idea to realize the purpose of ‘dealing pollution with waste’.
- wood waste /
- iron mud /
- carbothermal reduction /
- zero-valent iron/biochar /
- Cr(Ⅵ)

HTML全文

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

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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

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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

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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

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图 5 Fe⁰-BC-1200材料的Zeta电位

Figure 5. Zeta potential of Fe⁰-BC-1200

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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)

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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

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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

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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

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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)

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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)

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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

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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/%
		TFe		Fe⁰		C		Cu
		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

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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)
温度/ºC	平均值	标准差	平均值	标准差	平均值	标准差
800	156.1	3.7	4.12	0.5	0.23	0.02
900	137.6	4.2	4.22	0.3	0.21	0.02
1 000	119.1	6.6	5.17	0.4	0.17	0.04
1 100	109.8	4.9	6.11	0.1	0.16	0.03
1 200	105.6	4.3	6.23	0.3	0.14	0.01

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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元
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

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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
q_e/(mg/g)	k₁/min⁻¹	R²	q_e/(mg/g)	k₂/[g/(mg·min)]	R²
4.81	0.037	0.942	8.02	0.013	0.995

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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
q_max/(mg/g)	k_L/(L/mg)	R²	n	k_F/(mg/g)	R²
10.71	0.77	0.999	4.45	5.206	0.731

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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

doi: 10.13198/j.issn.1001-6929.2023.02.12

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

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

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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

doi: 10.13198/j.issn.1001-6929.2023.02.12

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

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

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出版历程

目录

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

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

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