硫磺/硫铁矿自养反硝化系统脱氮性能
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摘要
基于硫自养反硝化作用,寻求一种经济、快速、高效地污水脱氮工艺,采用硫磺/硫铁矿组合进行自养反硝化脱氮试验,以低C/N市政污水为处理对象,分别考察温度,硫磺与硫铁矿体积比和HRT等理化因素对反应器脱氮性能的影响.结果表明,在进水TN质量浓度约40 mg·L~(-1)条件下,1号反应器最佳HRT为2. 5 h,TN去除率平均稳定在72. 2%,出水TN约10. 55 mg·L~(-1); 2号反应器最佳HRT为3. 5 h,TN平均去除率约67. 8%,出水TN平均稳定至12. 90 mg·L~(-1); 3号反应器最佳HRT为3. 5 h,TN平均去除率60. 6%,出水TN稳定在15. 00 mg·L~(-1)左右.硫磺/硫铁矿自养反硝化系统比硫铁矿自养反硝化系统启动快;该系统脱氮效率随着硫磺与硫铁矿体积比减小而降低;该系统脱氮性能对温度的变化并不敏感,脱氮性能优于单独以硫铁矿为硫源的自养反硝化系统;系统中硫自养反硝化过程的主要功能菌属是Sulfurimonas和Thiobacillus,在3个反应器所占比例为1号> 2号> 3号.
In order to search for an economical,rapid,and highly efficient nitrogen removal process for sewage,a sulfur/pyrite packed column reactor was fed with low C/N municipal sewage. The effects of temperature,the sulfur-to-pyrite volume ratio,and hydraulic retention time( HRT) on nitrogen removal were studied. The results showed that with an influent total nitrogen( TN) of 40 mg·L~(-1),the optimal HRT of the No. 1 reactor was 2. 5 h,and the removal rate and effluent concentration of TN were stable at 72. 2% and 10. 55 mg·L~(-1),respectively. The optimal HRT of the No. 2 reactor was 3. 5 h,and the removal rate and effluent concentration of TN were stable at 67. 8% and 12. 90 mg·L~(-1),respectively. The optimal HRT of the No. 3 reactor was 3. 5 h,and the removal rate and effluent concentration of TN were stable at 60. 6% and 15. 00 mg·L~(-1),respectively. The sulfur/pyrite autotrophic denitrification system starts faster than the pyrite autotrophic denitrification system. Its nitrogen removal rate decreased with decreasing sulfur-to-pyrite volume ratio. The nitrogen removal performance of the system is not sensitive to temperature,and the denitrification performance is better than that of the system with pyrite alone as the sulfur source. The main functional bacteria in the system are Sulfurimonas and Thiobacillus,and the proportion of the sum of these two bacteria in the three reactors decreased from No. 1 to No. 3.
In order to search for an economical,rapid,and highly efficient nitrogen removal process for sewage,a sulfur/pyrite packed column reactor was fed with low C/N municipal sewage. The effects of temperature,the sulfur-to-pyrite volume ratio,and hydraulic retention time( HRT) on nitrogen removal were studied. The results showed that with an influent total nitrogen( TN) of 40 mg·L~(-1),the optimal HRT of the No. 1 reactor was 2. 5 h,and the removal rate and effluent concentration of TN were stable at 72. 2% and 10. 55 mg·L~(-1),respectively. The optimal HRT of the No. 2 reactor was 3. 5 h,and the removal rate and effluent concentration of TN were stable at 67. 8% and 12. 90 mg·L~(-1),respectively. The optimal HRT of the No. 3 reactor was 3. 5 h,and the removal rate and effluent concentration of TN were stable at 60. 6% and 15. 00 mg·L~(-1),respectively. The sulfur/pyrite autotrophic denitrification system starts faster than the pyrite autotrophic denitrification system. Its nitrogen removal rate decreased with decreasing sulfur-to-pyrite volume ratio. The nitrogen removal performance of the system is not sensitive to temperature,and the denitrification performance is better than that of the system with pyrite alone as the sulfur source. The main functional bacteria in the system are Sulfurimonas and Thiobacillus,and the proportion of the sum of these two bacteria in the three reactors decreased from No. 1 to No. 3.
引文
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[11] Kong Z,Feng C P,Chen N,et al. A soil infiltration system incorporated with sulfur-utilizing autotrophic denitrification(SISSAD)for domestic wastewater treatment[J]. Bioresource Technology,2014,159:272-279.
[12]李天昕,邱诚翔,徐昊,等.硫/石灰石自养反硝化处理低碳高氮城市污水的工艺[J].环境工程学报,2014,8(3):1062-1066.Li T X,Qiu C X,Xu H,et al. Low carbon and high nitrogen concentration municiple wastewater treatment with sulfur/limestone autotrophic denitrification technology[J]. Chinese Journal of Environmental Engineering,2014,8(3):1062-1066.
[13] Sahinkaya E, Yurtsever A, AktasO, et al. Sulfur-based autotrophic denitrification of drinking water using a membrane bioreactor[J]. Chemical Engineering Journal,2015,268:180-186.
[14]张菁,李睿华,李杰,等.石灰石和黄铁矿-石灰石人工湿地净化河水的研究[J].环境科学,2013,34(9):3445-3450.Zhang J,Li R H,Li J,et al. Limestone and pyrite-limestone constructed wetlands for treating river water[J]. Environmental Science,2013,34(9):3445-3450.
[15] Yang Y,Chen T H,Morrison L,et al. Nanostructured pyrrhotite supports autotrophic denitrification for simultaneous nitrogen and phosphorus removal from secondary effluents[J]. Chemical Engineering Journal,2017,328:511-518.
[16] Tong S,Rodriguez-Gonzalez L C,Feng C P,et al. Comparison of particulate pyrite autotrophic denitrification(PPAD)and sulfur oxidizing denitrification(SOD)for treatment of nitrified wastewater[J]. Water Science&Technology,2017,75(1-2):239-246.
[17]蒲娇阳.硫铁矿自养反硝化去除地下水中硝酸盐的研究[D].北京:中国地质大学(北京),2015.
[18] TorrentóC,Cama J, Urmeneta J, et al. Denitrification of groundwater with pyrite and Thiobacillus denitrificans[J].Chemical Geology,2010,278(1-2):80-91.
[19]李芳芳,施春红,周北海,等.硫磺和黄铁矿为填料的生物滤池自养反硝化强化处理二沉尾水[J].环境科学研究,2016,29(11):1693-1700.Li F F,Shi C H,Zhou B H,et al. Enhanced treatment of secondary effluent via autotrophic denitrification biofilter process using sulfur and pyrite as fillings[J]. Research of Environmental Sciences,2016,29(11):1693-1700.
[20]周彦卿,郝瑞霞,刘思远,等.新型硫铁复合填料强化再生水深度脱氮除磷[J].环境科学,2017,38(10):4309-4315.Zhou Y Q,Hao R X,Liu S Y,et al. Improving nitrogen and phosphorus removal from reclaimed water using a novel Sulfur/Iron composite filler[J]. Environmental Science,2017,38(10):4309-4315.
[21]姚鹏程,袁怡,龙震宇,等.新型单质硫自养生物膜反应器脱氮性能研究[J].现代化工,2018,38(5):181-186.Yao P C,Yuan Y,Long Z Y,et al. Study on denitrification performance of a new elemental sulfur autotrophic biofilm reactor[J]. Modern Chemical Industry,2018,38(5):181-186.
[22] Steudel R,Holdt G. Solubilization of elemental sulfur in water by cationic and anionic surfactants[J]. Angewandte Chemie International Edition,1988,27(10):1358-1359.
[23]刘续,周伟丽,董晓静,等.水力负荷对微污染水自养反硝化的影响[J].中国给水排水,2015,31(5):45-49.Liu X,Zhou W L,Dong X J,et al. Influence of hydraulic loading on sulfur-based autotrophic denitrification of micropolluted water[J]. China Water&Wastewater,2015,31(5):45-49.
[24]马航,朱强,朱亮,等.单质硫颗粒尺寸及反应器类型对硫自养反硝化反应器启动的影响[J].环境科学,2016,37(6):2235-2242.Ma H,Zhu Q,Zhu L,et al. Effect of element sulfur particle size and type of the reactor on start-up of sulfur-based autotrophic denitrification reactor[J]. Environmental Science,2016,37(6):2235-2242.
[25] Pu J Y,Feng C P,Liu Y,et al. Pyrite-based autotrophic denitrification for remediation of nitrate contaminated groundwater[J]. Bioresource Technology,2014,173:117-123.
[2] Cecconet D,Devecseri M,Callegari A,et al. Effects of process operating conditions on the autotrophic denitrification of nitratecontaminated groundwater using bioelectrochemical systems[J].Science of the Total Environment,2018,613-614:663-671.
[3]周健,黄勇,刘忻,等.硫自养反硝化耦合厌氧氨氧化脱氮条件控制研究[J].环境科学,2016,37(3):1061-1069.Zhou J,Huang Y,Liu X,et al. Element sulfur autotrophic denitrification combined anaerobic ammonia oxidation[J].Environmental Science,2016,37(3):1061-1069.
[4]任争鸣,刘雪洁,苏晓磊,等.硫自养反硝化深度脱氮中试研究[J].中国给水排水,2016,32(19):31-35.Ren Z M,Liu X J,Su X L,et al. Sulfur-based autotrophic denitrification process for advanced nitrogen removal[J]. China Water&Wastewater,2016,32(19):31-35.
[5] Kostrytsia A,Papirio S,Frunzo L,et al. Elemental sulfur-based autotrophic denitrification and denitritation:microbially catalyzed sulfur hydrolysis and nitrogen conversions[J]. Journal of Environmental Management,2018,211:313-322.
[6] Li R H,Morrison L,Collins G,et al. Simultaneous nitrate and phosphate removal from wastewater lacking organic matter through microbial oxidation of pyrrhotite coupled to nitrate reduction[J].Water Research,2016,96:32-41.
[7] Li H B,Zhou B H,Tian Z Y,et al. Efficient biological nitrogen removal by Johannesburg-Sulfur autotrophic denitrification from low COD/TN ratio municipal wastewater at low temperature[J].Environmental Earth Sciences,2015,73(9):5027-5035.
[8]袁莹,周伟丽,王晖,等.不同电子供体的硫自养反硝化脱氮实验研究[J].环境科学,2013,34(5):1835-1844.Yuan Y,Zhou W L,Wang H,et al. Study on sulfur-based autotrophic denitrification with different electron donors[J].Environmental Science,2013,34(5):1835-1844.
[9] Sahinkaya E,Dursun N. Use of elemental sulfur and thiosulfate as electron sources for water denitrification[J]. Bioprocess and Biosystems Engineering,2015,38(3):531-541.
[10]袁玉玲,李睿华.硫磺/石灰石自养反硝化系统脱氮除磷性能研究[J].环境科学,2011,32(7):2041-2046.Yuan Y L,Li R H. Performance of nitrogen and phosphorus removal of sulfur/limestone autotrophic denitrification system[J]. Environmental Science,2011,32(7):2041-2046.
[11] Kong Z,Feng C P,Chen N,et al. A soil infiltration system incorporated with sulfur-utilizing autotrophic denitrification(SISSAD)for domestic wastewater treatment[J]. Bioresource Technology,2014,159:272-279.
[12]李天昕,邱诚翔,徐昊,等.硫/石灰石自养反硝化处理低碳高氮城市污水的工艺[J].环境工程学报,2014,8(3):1062-1066.Li T X,Qiu C X,Xu H,et al. Low carbon and high nitrogen concentration municiple wastewater treatment with sulfur/limestone autotrophic denitrification technology[J]. Chinese Journal of Environmental Engineering,2014,8(3):1062-1066.
[13] Sahinkaya E, Yurtsever A, AktasO, et al. Sulfur-based autotrophic denitrification of drinking water using a membrane bioreactor[J]. Chemical Engineering Journal,2015,268:180-186.
[14]张菁,李睿华,李杰,等.石灰石和黄铁矿-石灰石人工湿地净化河水的研究[J].环境科学,2013,34(9):3445-3450.Zhang J,Li R H,Li J,et al. Limestone and pyrite-limestone constructed wetlands for treating river water[J]. Environmental Science,2013,34(9):3445-3450.
[15] Yang Y,Chen T H,Morrison L,et al. Nanostructured pyrrhotite supports autotrophic denitrification for simultaneous nitrogen and phosphorus removal from secondary effluents[J]. Chemical Engineering Journal,2017,328:511-518.
[16] Tong S,Rodriguez-Gonzalez L C,Feng C P,et al. Comparison of particulate pyrite autotrophic denitrification(PPAD)and sulfur oxidizing denitrification(SOD)for treatment of nitrified wastewater[J]. Water Science&Technology,2017,75(1-2):239-246.
[17]蒲娇阳.硫铁矿自养反硝化去除地下水中硝酸盐的研究[D].北京:中国地质大学(北京),2015.
[18] TorrentóC,Cama J, Urmeneta J, et al. Denitrification of groundwater with pyrite and Thiobacillus denitrificans[J].Chemical Geology,2010,278(1-2):80-91.
[19]李芳芳,施春红,周北海,等.硫磺和黄铁矿为填料的生物滤池自养反硝化强化处理二沉尾水[J].环境科学研究,2016,29(11):1693-1700.Li F F,Shi C H,Zhou B H,et al. Enhanced treatment of secondary effluent via autotrophic denitrification biofilter process using sulfur and pyrite as fillings[J]. Research of Environmental Sciences,2016,29(11):1693-1700.
[20]周彦卿,郝瑞霞,刘思远,等.新型硫铁复合填料强化再生水深度脱氮除磷[J].环境科学,2017,38(10):4309-4315.Zhou Y Q,Hao R X,Liu S Y,et al. Improving nitrogen and phosphorus removal from reclaimed water using a novel Sulfur/Iron composite filler[J]. Environmental Science,2017,38(10):4309-4315.
[21]姚鹏程,袁怡,龙震宇,等.新型单质硫自养生物膜反应器脱氮性能研究[J].现代化工,2018,38(5):181-186.Yao P C,Yuan Y,Long Z Y,et al. Study on denitrification performance of a new elemental sulfur autotrophic biofilm reactor[J]. Modern Chemical Industry,2018,38(5):181-186.
[22] Steudel R,Holdt G. Solubilization of elemental sulfur in water by cationic and anionic surfactants[J]. Angewandte Chemie International Edition,1988,27(10):1358-1359.
[23]刘续,周伟丽,董晓静,等.水力负荷对微污染水自养反硝化的影响[J].中国给水排水,2015,31(5):45-49.Liu X,Zhou W L,Dong X J,et al. Influence of hydraulic loading on sulfur-based autotrophic denitrification of micropolluted water[J]. China Water&Wastewater,2015,31(5):45-49.
[24]马航,朱强,朱亮,等.单质硫颗粒尺寸及反应器类型对硫自养反硝化反应器启动的影响[J].环境科学,2016,37(6):2235-2242.Ma H,Zhu Q,Zhu L,et al. Effect of element sulfur particle size and type of the reactor on start-up of sulfur-based autotrophic denitrification reactor[J]. Environmental Science,2016,37(6):2235-2242.
[25] Pu J Y,Feng C P,Liu Y,et al. Pyrite-based autotrophic denitrification for remediation of nitrate contaminated groundwater[J]. Bioresource Technology,2014,173:117-123.
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