地下水硝酸盐污染的固相反硝化原位修复技术研究
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摘要
本研究依托于国家水体污染控制与治理科技重大专项——“南水北调中线总干渠水质安全保障关键技术与工程示范课题”，以保障地下水水质安全为目标，研发地下水硝酸盐污染修复应用技术。研究显示，利用核桃壳、褐煤、陶粒作为固相有机碳源载体，对地下水硝酸盐污染进行原位修复是可行的。
本文首先通过收集国内不同产地褐煤（1#、2#、3#、4#）、无烟煤及焦炭半惰性有机碳源载体并进行分子结构分析，采用静态试验和柱试验对其反硝化效能进行对比，运用16S rDNA基因序列分子生物学分析方法，解析反应器内的微生物群形态。发现褐煤对硝酸盐的去除率随着HRT缩短呈现下降趋势。反硝化速率随着温度的升高而增加。4种褐煤反应柱的反硝化速率从高到低依次为3#褐煤>1#褐煤>2#褐煤>4#褐煤。进水NO_3~--N浓度与反硝化速率呈线性关系。且3#褐煤反应柱内的优势菌种为假单胞菌和伯克氏菌，其中假单胞菌占85.3%，伯克氏菌占6.9%。
对已遴选出的3#褐煤与高效挂膜轻质生物陶粒、核桃壳进行对比。在无外加碳源条件下，陶粒反应柱对硝酸盐没有明显的去除率；在投加碳源而未加营养物质条件下，3#褐煤与核桃壳对硝酸盐去除率可以达到90~100%，而陶粒则只能获得25~35%的硝酸盐去除率；在投加碳源及营养物质条件下，陶粒可获得比3#褐煤与核桃壳更好的效果；引入黄孢原毛平革菌后，3#褐煤反应柱去除率最高；通过发光细菌试验检测，3种载体的反应柱出水毒理学检验合格。
将核桃壳、3#褐煤、以及适于长生物膜的陶粒，结合实际硝酸盐污染地下水，进行不同复配形式的生物修复槽试验模拟研究，在进水NO_3~--N浓度为29mg/L左右，C槽（1/2核桃壳+1/2陶粒）、E槽（1/3核桃壳+1/33#褐煤+1/3陶粒）、B槽（3#褐煤）对硝酸盐去除率分别为63%、53%、32%。确定最佳HRT为48h，C槽、E槽、B槽硝酸盐去除率分别为82%、73%、45%。
最后将选定的核桃壳、陶粒、3#褐煤进行复配应用于长春双阳地下水硝酸盐污染原位修复模拟试验研究，原水NO_3~--N浓度为30mg/L左右，出水中硝酸盐最低可达7.09mg/L。同时将槽试验的不同复配组合应用到河南焦作进行现场中试放大研究，其原水NO_3~--N浓度为80mg/L左右，填充有1/3核桃壳+1/33#褐煤+1/3陶粒的系统出水中硝酸盐稳定在17mg/L左右。最终在南水北调中线总干渠焦作段建设地下水硝酸盐污染原位修复示范工程，其原水NO_3~--N浓度为50mg/L左右，稳定运行后其出水中硝酸盐最低可达6.55mg/L，满足《地下水质量标准》GB/T14848-93中的Ⅲ类水体标准。
This study relies on Major Science and Technology Program for Water PollutionControl and Treatment–“the project of key technology and engineering demonstrationfor safety guarantee of water quality of the main channel in middle route of theSouth-to-North Water Diversion Project”, in order to guarantee the groundwaterquality. Groundwater remediation technology on nitrate pollution was studied. Theresultes indicates that using walnut shell, lignite and ceramisite as carrier forsolid-phase carbon source is practically feasible for in situ remediation ofgroundwater contaminated by nitrate.
Firstly, semi-inertia carriers for organic carbon source as lignite (1#,2#,3#,4#),anthracite and coke were collected from different domestic producing areas. And thedenitrification efficiency of these carriers were compared. The molecular structureswere analysed. And16S rDNA gene sequence analysis method of molecular biologywas used to analyse microbiota morphology in the reactor. The removal efficiency ofnitrate by lignite decreases when the HRT becomes shorter. And with the increase oftemperature, the denitrification efficiency also increases. The denitrificationefficiencies of four lignite columns are3#>1#>2#>4#. The relationship of inflowNO_3~--N concentration and denitrification efficiency obeys to zero order reaction. Thedominant bacteria in3#column are pseudomonas and Burkholderia, withpseudomonas accounting for85.3%and Burkholderia accounting for6.9%.
The selected3#lignite were compared with lightweight bio-ceramic of highbiofilm-culturing efficiency and walnut shell. The column with bio-ceramic has noremoval efficiency without the external carbon source. In condition of having additivecarbon source but no nutrition, removal rate of walnut shell and#3lignite can reach90~100%, and ceramic is only25~35%. When adding carbon source and nutrition,ceramic performs better than walnut shell and3#lignite. After introducing inPhanerochete chrysosporium,3#lignite reaction column obtains the highest removalrate. And through the photobacteria test, the effluent of three kind carriers response noacute toxicity, so they are qualified for toxicology inspection.
Then, different complex formulations of walnut shell,3#lignite, and ceramsite of suitable for biomembrane’s grow were used in biological repair trough test simulationresearch with real nitrate-bearing groundwater. The influent nitrate concentration wasabout29mg/L. The results showed that each index of the effluent of C trough (1/2walnut shell+1/2ceramsite)、E trough (1/3walnut shell+1/33#lignite+1/3ceramsite) and B trough (3#lignite) could reach the standard and the nitrate removalefficiency were63%,53%and32%respectively. When48h was determined as thebest HRT, the effluent of C、E and B trough could also reach the standard and theremoval efficiency were increased to82%,73%and45%respectively.
Finally, complex formulation of walnut shell, ceramsite,3#lignite was used asthe solid-phase organic carbon-source of simulation experimental research to removethe nitrate from groundwater in situ in Shuangyang, Changchun Province, where theinflow concentration of nitrate was about30mg/L and the effluent concentrationcould even reach7.09mg/L. Meanwhile, different complex formulations in troughtest were investigated to site pilot in Jiaozuo, Henan Province. The nitrateconcentration of raw water was about80mg/L, and the effluent concentration couldstay at the level of17mg/L after treatment system of1/3walnut shell+1/33#lignite+1/3ceramsite. At last, when the above solid-phase organic carbon-source wasapplied in Jiaozuo section of the middle route of the South-to-North water transferproject, the stable effluent concentration of nitrate in site could decrease from50mg/L to even6.55mg/L.
本文首先通过收集国内不同产地褐煤（1#、2#、3#、4#）、无烟煤及焦炭半惰性有机碳源载体并进行分子结构分析，采用静态试验和柱试验对其反硝化效能进行对比，运用16S rDNA基因序列分子生物学分析方法，解析反应器内的微生物群形态。发现褐煤对硝酸盐的去除率随着HRT缩短呈现下降趋势。反硝化速率随着温度的升高而增加。4种褐煤反应柱的反硝化速率从高到低依次为3#褐煤>1#褐煤>2#褐煤>4#褐煤。进水NO_3~--N浓度与反硝化速率呈线性关系。且3#褐煤反应柱内的优势菌种为假单胞菌和伯克氏菌，其中假单胞菌占85.3%，伯克氏菌占6.9%。
对已遴选出的3#褐煤与高效挂膜轻质生物陶粒、核桃壳进行对比。在无外加碳源条件下，陶粒反应柱对硝酸盐没有明显的去除率；在投加碳源而未加营养物质条件下，3#褐煤与核桃壳对硝酸盐去除率可以达到90~100%，而陶粒则只能获得25~35%的硝酸盐去除率；在投加碳源及营养物质条件下，陶粒可获得比3#褐煤与核桃壳更好的效果；引入黄孢原毛平革菌后，3#褐煤反应柱去除率最高；通过发光细菌试验检测，3种载体的反应柱出水毒理学检验合格。
将核桃壳、3#褐煤、以及适于长生物膜的陶粒，结合实际硝酸盐污染地下水，进行不同复配形式的生物修复槽试验模拟研究，在进水NO_3~--N浓度为29mg/L左右，C槽（1/2核桃壳+1/2陶粒）、E槽（1/3核桃壳+1/33#褐煤+1/3陶粒）、B槽（3#褐煤）对硝酸盐去除率分别为63%、53%、32%。确定最佳HRT为48h，C槽、E槽、B槽硝酸盐去除率分别为82%、73%、45%。
最后将选定的核桃壳、陶粒、3#褐煤进行复配应用于长春双阳地下水硝酸盐污染原位修复模拟试验研究，原水NO_3~--N浓度为30mg/L左右，出水中硝酸盐最低可达7.09mg/L。同时将槽试验的不同复配组合应用到河南焦作进行现场中试放大研究，其原水NO_3~--N浓度为80mg/L左右，填充有1/3核桃壳+1/33#褐煤+1/3陶粒的系统出水中硝酸盐稳定在17mg/L左右。最终在南水北调中线总干渠焦作段建设地下水硝酸盐污染原位修复示范工程，其原水NO_3~--N浓度为50mg/L左右，稳定运行后其出水中硝酸盐最低可达6.55mg/L，满足《地下水质量标准》GB/T14848-93中的Ⅲ类水体标准。
This study relies on Major Science and Technology Program for Water PollutionControl and Treatment–“the project of key technology and engineering demonstrationfor safety guarantee of water quality of the main channel in middle route of theSouth-to-North Water Diversion Project”, in order to guarantee the groundwaterquality. Groundwater remediation technology on nitrate pollution was studied. Theresultes indicates that using walnut shell, lignite and ceramisite as carrier forsolid-phase carbon source is practically feasible for in situ remediation ofgroundwater contaminated by nitrate.
Firstly, semi-inertia carriers for organic carbon source as lignite (1#,2#,3#,4#),anthracite and coke were collected from different domestic producing areas. And thedenitrification efficiency of these carriers were compared. The molecular structureswere analysed. And16S rDNA gene sequence analysis method of molecular biologywas used to analyse microbiota morphology in the reactor. The removal efficiency ofnitrate by lignite decreases when the HRT becomes shorter. And with the increase oftemperature, the denitrification efficiency also increases. The denitrificationefficiencies of four lignite columns are3#>1#>2#>4#. The relationship of inflowNO_3~--N concentration and denitrification efficiency obeys to zero order reaction. Thedominant bacteria in3#column are pseudomonas and Burkholderia, withpseudomonas accounting for85.3%and Burkholderia accounting for6.9%.
The selected3#lignite were compared with lightweight bio-ceramic of highbiofilm-culturing efficiency and walnut shell. The column with bio-ceramic has noremoval efficiency without the external carbon source. In condition of having additivecarbon source but no nutrition, removal rate of walnut shell and#3lignite can reach90~100%, and ceramic is only25~35%. When adding carbon source and nutrition,ceramic performs better than walnut shell and3#lignite. After introducing inPhanerochete chrysosporium,3#lignite reaction column obtains the highest removalrate. And through the photobacteria test, the effluent of three kind carriers response noacute toxicity, so they are qualified for toxicology inspection.
Then, different complex formulations of walnut shell,3#lignite, and ceramsite of suitable for biomembrane’s grow were used in biological repair trough test simulationresearch with real nitrate-bearing groundwater. The influent nitrate concentration wasabout29mg/L. The results showed that each index of the effluent of C trough (1/2walnut shell+1/2ceramsite)、E trough (1/3walnut shell+1/33#lignite+1/3ceramsite) and B trough (3#lignite) could reach the standard and the nitrate removalefficiency were63%,53%and32%respectively. When48h was determined as thebest HRT, the effluent of C、E and B trough could also reach the standard and theremoval efficiency were increased to82%,73%and45%respectively.
Finally, complex formulation of walnut shell, ceramsite,3#lignite was used asthe solid-phase organic carbon-source of simulation experimental research to removethe nitrate from groundwater in situ in Shuangyang, Changchun Province, where theinflow concentration of nitrate was about30mg/L and the effluent concentrationcould even reach7.09mg/L. Meanwhile, different complex formulations in troughtest were investigated to site pilot in Jiaozuo, Henan Province. The nitrateconcentration of raw water was about80mg/L, and the effluent concentration couldstay at the level of17mg/L after treatment system of1/3walnut shell+1/33#lignite+1/3ceramsite. At last, when the above solid-phase organic carbon-source wasapplied in Jiaozuo section of the middle route of the South-to-North water transferproject, the stable effluent concentration of nitrate in site could decrease from50mg/L to even6.55mg/L.
引文
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