褐煤协同球红假单胞菌固定SRB颗粒处理AMD中Fe<sup>2+</sup>、Mn<sup>2+</sup>试验研究

张健; 狄军贞; 姜国亮; 董艳荣; 王显军; 杨逾; 周新华

doi:10.13199/j.cnki.cst.2021-0473

褐煤协同球红假单胞菌固定SRB颗粒处理AMD中Fe²⁺、Mn²⁺试验研究

辽宁工程技术大学土木工程学院，辽宁阜新　123000

基金项目:

国家自然科学基金资助项目（41672247）；辽宁省“兴辽英才”青年拔尖人才计划资助项目（XLYC1807159）；辽宁工程技术大学学科创新团队资助项目（LNTU20TD-21）

详细信息

作者简介:
张健: (1995—)，男，山西和顺人，硕士研究生。E-mail：zhangjian3733@126.com

通讯作者:
狄军贞: (1979—)，男，甘肃甘谷人，教授，博士生导师，博士。E-mail：dijunzhen@126.com

中图分类号: X703
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出版历程
- 收稿日期: 2021-12-19
- 录用日期: 2021-12-19
- 网络出版日期: 2023-05-09
- 刊出日期: 2023-04-29

Experimental study on treatment of Fe²⁺ and Mn²⁺ in AMD with lignite combined with Pseudomonas aeruginosa immobilized SRB particles

College of Civil Engineering, Liaoning Technical University, Fuxin 123000, China

Funds:

National Natural Science Foundation of China (41672247); Liaoning Province "Xingliao Talents" Youth Top Talent Program Project (XLYC1807159); Subject Innovation Team Project of Liaoning Technical University (LNTU20TD-21)

摘要

摘要:
针对硫酸盐还原菌（Sulfate-Reducing Bacteria,SRB）易受高浓度重金属、低pH抑制，以及需要投加碳源材料等问题，采用微生物固定化技术，以SRB、球红假单胞菌和褐煤作为主要固定基质，制备褐煤协同球红假单胞菌固定SRB颗粒（L-P-SRB），探究L-P-SRB对酸性矿山废水（Acid Mine Drainage, AMD）中含Fe²⁺、Mn²⁺和SO₄ ²⁻的去除效果。基于还原动力学及吸附动力学结合扫描电镜（SEM）和傅里叶红外光谱仪（FT-IR）等手段，揭示L-P-SRB处理AMD的机理。同时，探究了低温处理L-P-SRB对AMD的修复效果，为低温条件下矿区处理AMD提供一定的依据。结果表明：L-P-SRB对Fe²⁺和Mn²⁺的去除率分别为91%和79%，吸附Fe²⁺和Mn²⁺的过程均符合拟一级动力学；对SO₄ ²⁻的去除率分别达到了91.28%和81.94%，还原SO₄ ²⁻的过程符合一级动力学。与Fe²⁺相比，Mn²⁺对L-P-SRB活性有一定的抑制作用。L-P-SRB能将废水中的Fe²⁺、Mn²⁺和SO₄ ²⁻一次性去除，很好的解决了褐煤只能单纯吸附重金属离子和SRB需要投加碳源的问题。低温冷藏处理不会抑制L-P-SRB的活性，为一次制备多次使用提供了依据。由SEM和FT-IR检测可得，L-P-SRB在处理废水的过程中，球红假单胞菌优先发挥作用，破坏褐煤的结构，部分官能团被破坏，褐煤中的C—C、C=O以及环烃、烷烃、烯烃的侧链断裂，产生大量小分子有机物，增大了颗粒的比表面积，提高了颗粒的吸附能力。同时褐煤为SRB还原SO₄ ²⁻提供了载体和大量的碳源，促进了SRB的生长，提高了对AMD的处理效果。
- 褐煤 /
- 酸性矿山废水 /
- 硫酸盐还原菌 /
- 球红假单胞菌 /
- 固定化技术
Abstract:
Sulfate-Reducing Bacteria (SRB) are easily inhibited by high concentrations of heavy metals, low pH as well as the need to add carbon source materials, the microbial immobilization technology was adopted, with SRB, Pseudomonas aeruginosa and lignite as the main immobilization substrates, to prepare lignite and Pseudomonas aeruginosa immobilized SRB particles (L-P-SRB) and the removal effect of L-P-SRB on Fe²⁺, Mn²⁺ and SO₄ ²⁻ in acid mine wastewater (AMD) was investigated. Based on the reduction kinetics and adsorption kinetics, the mechanism of AMD treatment by L-P-SRB was revealed by means of scanning electron microscope (SEM) and Fourier transform infrared spectroscopy (FT-IR), and the mechanism of L-P-SRB treating AMD was revealed. At the same time, the repair effect of low temperature treatment of L-P-SRB on AMD is explored, which provides a certain basis for the treatment of AMD in mining areas under the condition of low temperature. The results show that the removal rates of Fe²⁺ and Mn²⁺ by L-P-SRB are 91% and 79% respectively, and the process of adsorption of Fe²⁺ and Mn²⁺ conforms to the pseudo-first-order kinetics; the removal rate of SO₄ ²⁻ reaches 91.28% and 81.94% respectively, and the process of reducing SO₄ ²⁻ is in accordance with the first-order kinetics. Compared with Fe²⁺, Mn²⁺ has a certain inhibitory effect on the activity of L-P-SRB. L-P-SRB can remove Fe²⁺, Mn²⁺ and SO₄ ²⁻ in wastewater at one time, which well solves the problem that lignite can only adsorb heavy metal ions and SRB needs to add carbon source. Low temperature cold storage treatment will not inhibit the activity of L-P-SRB, which provides a basis for one-time preparation and multiple use. According to the detection of SEM and FT-IR, pseudomonas aeruginosa plays a priority role in the treatment of wastewater by L-P-SRB, destroying the structure of lignite, destroying some functional groups, breaking the C—C bond, C=O bond and side chain of cycloalkanes, alkanes and olefins in lignite, producing a large number of small molecule organic substances, increasing the specific surface area of particles, and improving the adsorption capacity of particles. At the same time, lignite provides a carrier and a large number of carbon sources for the reduction of SO₄ ²⁻ by SRB, which promotes the growth of SRB and improves the treatment effect of AMD.
- lignite /
- acid mine wastewater /
- sulfate reducing bacteria /
- pseudomonas aeruginosa /
- immobilization technology

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图 1 1号、2号废水中pH和ORP的变化情况

Figure 1. Changes of pH and ORP in No.1 and No.2 waste water

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图 2 L-P-SRB对SO₄ ²⁻、Fe²⁺、Mn²⁺的去除情况

Figure 2. Removal of SO₄ ²⁻, Fe²⁺, Mn²⁺ by L-P-SRB

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图 3 SO₄ ²⁻的零级反应动力学拟合曲线

Figure 3. Zero-order reaction kinetic fitting curve of SO₄ ²⁻

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图 4 SO₄ ²⁻的一级反应动力学拟合曲

Figure 4. First-order reaction kinetic fitting curve of SO₄ ²⁻

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图 5 Fe²⁺、Mn²⁺的吸附动力学拟合曲线

Figure 5. Adsorption kinetics curve of Fe²⁺ and Mn²⁺

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图 6 L-P-SRB对Fe²⁺的去除效果

Figure 6. Removal effect of L-P-SRB on Fe²⁺

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图 7 L-P-SRB对Mn²⁺的去除效果

Figure 7. Removal effect of L-P-SRB on Mn²⁺

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图 8 L-P-SRB反应前后的SEM图

Figure 8. SEM diagram of before and after L-P-SRB reaction

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图 9 L-P-SRB处理1号含Fe²⁺废水后的SEM图

Figure 9. SEM diagram of L-P-SRB after treatment of No.1 wastewater containing Fe²⁺

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图 10 L-P-SRB处理2号含Mn²⁺废水后的SEM图

Figure 10. SEM diagram of L-P-SRB after treatment of No.2 wastewater containing Mn²⁺

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图 11 L-P-SRB处理Fe²⁺、Mn²⁺废水前后的FT-IR谱图

Figure 11. FT-IR Spectra of Fe²⁺ and Mn²⁺ wastewater before and after L-P-SRB treatment

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表 1 SO₄ ²⁻反应动力学参数

Table 1 Kinetic parameters of SO₄ ²⁻ reaction

项目零级反应一级反应
k₀/(mg·L⁻¹·h⁻¹) R² k₁/h⁻¹ R²

1号 5.610 6 0.896 0.019 65 0.955
2号 5.081 4 0.879 0.013 56 0.907

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表 2 Fe²⁺、Mn²⁺的吸附动力学参数

Table 2 Adsorption kinetic parameters of Fe²⁺ and Mn²⁺

离子拟一级动力学拟二级动力学
k₁/h⁻¹ q_e/(mg·g⁻¹) R² k₂/(g·mg⁻¹·h⁻¹) q_e/(mg·g⁻¹) R²

Fe²⁺ 0.030 1 0.515 0.976 0.389 0 0.666 0.971
Mn²⁺ 0.032 4 0.316 0.996 0.089 6 0.385 0.994

下载: 导出CSV

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项目	零级反应		一级反应
项目	k₀/(mg·L⁻¹·h⁻¹)	R²	k₁/h⁻¹	R²
1号	5.610 6	0.896	0.019 65	0.955
2号	5.081 4	0.879	0.013 56	0.907

离子	拟一级动力学			拟二级动力学
离子	k₁/h⁻¹	q_e/(mg·g⁻¹)	R²	k₂/(g·mg⁻¹·h⁻¹)	q_e/(mg·g⁻¹)	R²
Fe²⁺	0.030 1	0.515	0.976	0.389 0	0.666	0.971
Mn²⁺	0.032 4	0.316	0.996	0.089 6	0.385	0.994

褐煤协同球红假单胞菌固定SRB颗粒处理AMD中Fe2+、Mn2+试验研究

作者简介: 张健: (1995—)，男，山西和顺人，硕士研究生。E-mail：zhangjian3733@126.com

通讯作者: 狄军贞: (1979—)，男，甘肃甘谷人，教授，博士生导师，博士。E-mail：dijunzhen@126.com

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出版历程

Experimental study on treatment of Fe2+ and Mn2+ in AMD with lignite combined with Pseudomonas aeruginosa immobilized SRB particles