Simultaneous removal of ciprofloxacin in PHBV biofilter denitrification process and its influencing factors
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摘要:
固相碳源是反硝化生物滤池深度脱氮过程中抗生素被同步去除的关键影响因素之一。选取典型抗生素环丙沙星（CIP）为研究对象，搭建固相碳源-聚羟基丁酸戊酸酯（PHBV）反硝化生物滤池，重点考察不同浓度CIP条件下系统的出水水质和微生物群落结构特征变化。结果表明：秋季适宜温度（3~27 ℃）条件下，当进水CIP浓度低于300 μg/L 时，NO3 −-N和CIP去除率均超过了95%；冬季低温（−8~12 ℃）条件下，当进水CIP浓度为1 000 μg/L时，NO3 −-N和CIP去除率分别为60%和49%。微生物群落结构特征分析显示，变形菌门（Proteobacteria）和丙型变形菌纲（Gammaproteobacteria）分别为最优势门和纲，其中Gammaproteobacteria良好分泌胞外聚合物的特征使其对抗生素具有耐药性。尽管系统长期暴露于CIP中，系统中反硝化菌属物种依然保持较高的相对丰度，其中最优势反硝化菌属脱氯单胞菌（Dechloromonas）在系统纵向沿程中的相对丰度均超过5%，最高达10%。研究证实PHBV反硝化生物滤池是实现深度脱氮并同步去除抗生素的有效技术，同时也为反硝化生物滤池在实际工程中低温运行提供一定的数据支撑。
Abstract:Solid carbon source is one of key factors affecting the antibiotics' simultaneous removal during the advanced nitrogen removal process in a denitrifying biofilter. The typical antibiotic ciprofloxacin (CIP) was selected as the research object, and a solid phase carbon source, poly(hydroxybutyrate-co-valerate) (PHBV) supported denitrifying biofilter, was built, focusing on the variation of effluent quality and microbial community structure characteristics of the system under the conditions of different concentrations of CIP. The results showed that the nitrate and CIP removal efficiency were both more than 95% when the influent CIP concentration was lower than 300 μg/L under the suitable temperature (3 to 27 ℃) in autumn. However, under lower temperature (−8 to 12 ℃) in winter, the nitrate and CIP removal efficiency decreased to 60% and 49%, respectively, with influent CIP of 1 000 μg/L. Microbial community structure characteristics analysis revealed that Proteobacteria and Gammaproteobacteria were the most dominant phylum and class, respectively. Gammaproteobacteria was resistant to antibiotics due to their good secretion of extracellular polymeric substances. Meanwhile, the relative abundance of denitrifying bacteria in this system still kept high under a long-term exposure to CIP. The relative abundance of Dechloromonas, the most dominant denitrifying bacteria, was all more than 5% along the longitudinal profile of the system with the highest of 10%. The study confirmed that PHBV supported denitrifying biofilter is an efficient technology to fulfill the simultaneous removal of nitrate and antibiotics. And it also provided data support for denitrifying biological filter under low temperature in practical engineering.
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图 1 PHBV反硝化生物滤池装置示意
Figure 1. Schematic diagram of PHBV supported denitrification biofilter
图 2 进出水DO、ORP、pH以及COD变化特征
Figure 2. Variation characteristics of effluent DO, ORP, pH and COD
图 3 PHBV反硝化生物滤池系统的CIP三维荧光特征
Figure 3. EEM characteristics of CIP influent and effluent in PHBV supported denitrification biofilter
图 4 PHBV反硝化生物滤池系统进出水CIP浓度变化
Figure 4. Variation of CIP concentrations in influent and effluent in PHBV supported denitrification biofilter
图 5 PHBV反硝化生物滤池系统NO3 −-N浓度变化
Figure 5. Nitrate removal performance in PHBV supported denitrification biofilter
图 6 PHBV反硝化生物滤池系统各阶段进出水NH4 +-N浓度变化
Figure 6. Concentration of NH4 +-N in influent and effluent during different phases in PHBV supported denitrification biofilter
图 7 门水平、纲水平以及属水平上微生物群落相对丰度
Figure 7. Relative abundance of microbial communities at phylum, class and genus levels
表 1 PHBV反硝化生物滤池进水水质特征和运行条件
Table 1. Influent characteristics and operation parameters in PHBV supported denitrification biofilter
阶段 运行时间/d 温度/℃ 水力停留时间（HRT）/h 进水pH NO3 −-N浓度/(mg/L) CIP浓度/(μg/L) Ⅰ 1~21 13~27 24 6.85±0.31 15.60~17.03 0 Ⅱ 22~42 8~24 30 7.02±0.11 15.53~16.74 0 Ⅲ 43~52 9~27 30 7.07±0.14 15.83~17.58 100 Ⅳ 53~72 3~19 30 7.15±0.24 15.44~17.42 300 Ⅴ 73~92 −5~16 30 7.23±0.13 15.20~17.00 500 Ⅵ 93~112 −8~12 30 7.24±0.11 15.03~16.26 1 000 
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表 2 PHBV反硝化生物滤池纵向沿程水质变化特征
Table 2. Characteristics of water quality along the longitudinal profile in PHBV supported denitrification biofilter
沿程采样点 DO浓度/(mg/L) ORP/mV pH COD/(mg/L) NO3 −-N浓度/(mg/L) NH4 +-N浓度/(mg/L) NO2 −-N浓度/(mg/L) CIP浓度/（μg/L） 进水 9.39 275.00 7.76 8.35 15.39 0.56 0.01 1 000.00 出水口① 7.18 203.20 7.39 92.58 12.86 0.99 0.04 916.01 出水口② 4.77 232.30 7.26 57.58 11.10 0.90 0.04 852.90 出水口③ 4.66 251.60 7.32 53.62 10.18 0.96 0.06 816.40 出水口④ 4.49 208.30 7.40 18.22 8.96 0.93 0.04 759.03 出水口⑤ 4.35 214.00 7.07 63.93 5.94 0.97 0.05 607.10 出水 3.57 162.90 7.25 23.59 4.31 1.07 0.20 500.06
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表 3 PHBV反硝化生物滤池系统的微生物多样性指数
Table 3. Microbial diversity index of PHBV supported denitrification biofilter
样品编号 Chao1指数 Shannon指数 a1 3 496.29 8.94 a2 4 863.72 9.65 a3 3 766.92 7.52 a4 4 101.46 7.93 a5 4 074.57 9.32 a6 2 192.23 4.77
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