硫酸盐还原菌法固定酸性矿山废水中重金属的研究进展

doi:10.16085/j.issn.1000-6613.2021-2532

摘要/Abstract

摘要：

硫酸盐还原菌（SRB）法是一种极具潜力的酸性矿山废水（AMD）处理技术，如何将多种重金属分级沉淀并且分相分离出来，是SRB工艺走上工程应用的关键。本文综述了SRB法固定AMD中重金属的国内外研究进展，主要包括SRB法去除AMD中重金属的原理、SRB法分级沉淀AMD中多种重金属的工艺（分离式多级pH控制工艺及厌氧折流板反应器工艺）和SRB法厌氧污泥中金属硫化物的生物矿化（SRB介导的生物矿化成矿、生物矿化成矿影响因素及生物矿化过程微观机理），分析了此方面研究工作存在的问题。最后文章针对SRB法的深入研究及应用进行展望，认为硫酸盐还原体系中硫化物成矿的调控、成矿物相演变与微生物群落演替过程的解析以及矿化固定AMD中重金属成矿机理的探索将是今后重点关注的研究内容。

关键词: 硫酸盐还原菌法, 酸性矿山废水, 重金属, 分级沉淀, 生物矿化固定

Abstract:

Sulfate reducing bacteria (SRB) method is a potential acid mine drainage (AMD) treatment technology. How to precipitate and separate a variety of heavy metals is the key to engineering application of SRB process. This paper reviews the domestic and foreign research progress of SRB fixation of heavy metals in AMD. It includes the principle of SRB method for removing heavy metals from AMD, the process of SRB method for fractional precipitation of a variety of heavy metals from AMD (separate multistage pH control process and anaerobic baffled reactor process), and the biological mineralization of metal sulfide in anaerobic sludge by SRB process (SRB mediated biological mineralization, influence factors of biological mineralization and the microscopic mechanism of biomineralization process), and the existing problems in this field are analyzed. Finally, the paper prospects the further research and application of SRB method, and it is believed that the regulation of sulfide mineralization in sulfate reduction system, the analysis of mineral-forming phases evolution and microbial community succession process, and the exploration of heavy metal mineralization mechanism in mineralization fixed AMD will be the focus of future research.

Key words: sulfate reducing bacteria method, acid mine drainage, heavy metals, fractional precipitation, biomineralization fixation

中图分类号:

X703

闻倩敏, 秦永丽, 郑君健, 韦巧艳, 张媛媛, 蒋永荣. 硫酸盐还原菌法固定酸性矿山废水中重金属的研究进展[J]. 化工进展, 2022, 41(10): 5578-5587.

WEN Qianmin, QIN Yongli, ZHENG Junjian, WEI Qiaoyan, ZHANG Yuanyuan, JIANG Yongrong. Research advances in the fixation of heavy metals in acid mine wastewater by sulfate reducing bacteria[J]. Chemical Industry and Engineering Progress, 2022, 41(10): 5578-5587.

图/表 7

表1 酸性矿山废水中主要重金属硫化物的Ksp和沉淀起始的pH条件

硫化物	溶度积K_sp/g·L^-1	起始沉淀pH
MnS	1.4×10^-15	>7
FeS	3.7×10^-19	>6
ZnS	1.2×10^-23	2~3
CuS	8.5×10^-45	1
HgS	4.0×10^-53	1
PbS	3.4×10^-28	1
NiS	3.0×10^-19~10^-25	5~6
CdS	3.6×10^-29	1
Al₂S₃	2.0×10^-7	—

表2 分离式多级pH控制的工艺应用

反应装置	碳源	COD/SO₄^2-	HRT	pH控制金属分级沉淀	文献
三级流化床反应器+硫化物沉淀池	乙醇	0.67~0.85	1d	pH=4.0，Cu²⁺沉淀率为82%； pH=6.3，Fe²⁺沉淀率为99%	［27］
硫酸盐还原反应器+铁氧化/沉淀池	甘油	—	1.96~41.7h	pH=2.3，Zn²⁺沉淀率为90%； pH=4.0，Fe²⁺沉淀率为100%	［28］
厌氧上流式反应器+硫化物沉淀池	乙醇	0.67~0.87	1d	pH<2，Cu²⁺沉淀率为92%； pH=8.0，Fe²⁺沉淀率为89%	［29］
产硫上流式生物膜反应器+连续流小型生物反应器	甘油	—	30.3~46.9h	pH=2.2~2.5，Cu²⁺沉淀率为93%； pH=4.0，Zn²⁺沉淀率为93%	［9］
两套连续流硫酸盐还原反应器	氢气	—	35h	pH=2.5，Cu²⁺沉淀率为95%； pH=3.0，Zn²⁺沉淀率为95%	［30］
床柱式反应器+连续流生物反应器+机械搅拌沉淀池	乙酸钠和氢气	—	0.9d	pH=2.8，Cu²⁺沉淀率为88%； pH=3.5，Zn²⁺沉淀率为93%； pH=6.0，Ni²⁺、Fe²⁺沉淀率为91%	［31］

表3 多隔室厌氧折流板反应器在重金属废水中的工艺应用

碳源	COD/SO $4 2 -$	HRT	pH分级	重金属去除率	文献
乙醇	0.67~0.737	2d	①pH=3.0； ②pH=4.5 ③pH=7.0~8.0	Mn²⁺（25%~77%）； Co²⁺、Cu²⁺、Fe²⁺、Ni²⁺、Zn²⁺（99%）	［38］
乳酸盐	0.67	5d	①pH=2； ②pH=3.5； ③pH=6	Mo⁴⁺（72%）； Ni²⁺、Co³⁺（76%）； V²⁺（70%）	［39］
乳酸盐	0.67	2d	①pH<2； ②pH=3.3； ③pH=6.0~7.5	Cu²⁺（100%）； Zn²⁺（83%~98%）	［40］
乙醇	0.67~0.737	1~2d	①pH=2.25~2.5； ②pH=7.2~7.38； ③pH=8.6	Cu²⁺（>99%）； Zn²⁺（98%）	［41］

表3 多隔室厌氧折流板反应器在重金属废水中的工艺应用

碳源	COD/SO $4 2 -$	HRT	pH分级	重金属去除率	文献
乙醇	0.67~0.737	2d	①pH=3.0； ②pH=4.5 ③pH=7.0~8.0	Mn²⁺（25%~77%）； Co²⁺、Cu²⁺、Fe²⁺、Ni²⁺、Zn²⁺（99%）	［38］
乳酸盐	0.67	5d	①pH=2； ②pH=3.5； ③pH=6	Mo⁴⁺（72%）； Ni²⁺、Co³⁺（76%）； V²⁺（70%）	［39］
乳酸盐	0.67	2d	①pH<2； ②pH=3.3； ③pH=6.0~7.5	Cu²⁺（100%）； Zn²⁺（83%~98%）	［40］
乙醇	0.67~0.737	1~2d	①pH=2.25~2.5； ②pH=7.2~7.38； ③pH=8.6	Cu²⁺（>99%）； Zn²⁺（98%）	［41］

图1 SRB细胞壁上纳米矿物团聚体[44]（白色箭头表示丝状菌的宽度）

图2 天然气水合物赋存区沉积物中自生矿物的SEM图

图3 实验培养基中反应产物的SEM图[55]

图4 SRB诱导金属硫化物矿物形成过程示意图

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