短程反硝化工艺对稀土矿山废水处理的中试研究

doi:10.19965/j.cnki.iwt.2023-0866

摘要/Abstract

摘要：

通过中试规模试验研究验证在离子型稀土矿山废水处理中，短程反硝化（Part denitrification，PD）为厌氧氨氧化（Anaerobic ammonium oxidation，Anammox）提供底物NO₂ ^-的可能性。结果表明：接种城市污水处理厂剩余污泥，以实际矿山废水为进水，调控碳氮比（COD/N）降至2.1并采用实时COD/N控制策略可以保证PD反应器的启动和长期稳定运行，亚硝酸盐积累率（Nitrite accumulation ratio，NAR）保持在（58±7.32）%；微生物群落演变表明PD的主要贡献者Thauera菌属的相对丰度由初始的4.39%增至最终的17.58%；SEM-EDS显示Ca²⁺与微生物分泌的胞外聚合物（Extracellular polymeric substances，EPS）结合，使污泥拥有良好的持留能力。为短程反硝化耦合厌氧氨氧化（PD/A）技术在大规模离子型稀土矿山尾水处理工程中的应用提供重要参考。

关键词: 短程反硝化, 厌氧氨氧化, 稀土矿山废水

Abstract:

In this study,a pilot scale experiment was conducted to verify the possibility of part denitrification(PD) to provide substrate NO₂ ^- for anaerobic ammonium oxidation(Anammox) in the treatment of ion-type rare earth mine wastewater. The results showed that the start-up and long-term stable operation of the PD reactor could be ensured by inoculating the residual sludge of the municipal sewage treatment plant, taking the actual mine wastewater as influent,regulating the carbon to nitrogen ratio(COD/N) to 2.1 and adopting the real-time COD/N control strategy. Nitrite accumulation ratio(NAR) was remained at (58±7.32)%. The evolution of microbial community showed that the relative abundance of Thauera, the main contributor to PD, increased from 4.39% at the beginning to 17.58% at the end. SEM-EDS showed that Ca²⁺ combined with Extracellular polymeric substances(EPS) provided sludge good retention ability. This study provides an important reference for the application of partial denitrification coupled anammox(PD/A) technology in large-scale ion-type rare earth mine tailwater treatment engineering.

Key words: partial denitrification, Anammox, real earth mine wastewater

中图分类号:

X703.1

邓玉坤. 短程反硝化工艺对稀土矿山废水处理的中试研究[J]. 工业水处理, 2024, 44(8): 149-155.

Yukun DENG. Pilot study on treatment of rare earth mine wastewater by partial denitrification[J]. Industrial Water Treatment, 2024, 44(8): 149-155.

https://www.iwt.cn/CN/Y2024/V44/I8/149

图/表 9

参考文献 33

1	VAN DE GRAAF A A， MULDER A， DE BRUIJN P，et al. Anaerobic oxidation of ammonium is a biologically mediated process［J］. Applied and Environmental Microbiology，1995，61（4）：1246-1251. doi:10.1128/aem.61.4.1246-1251.1995
2	ZHAO Qingliang， KUGEL G. Thermophilic/mesophilic digestion of sewage sludge and organic wastes［J］. Journal of Environmental Science and Health Part A：Environmental Science and Engineering and Toxicology，1996，31（9）：2211-2231. doi:10.1080/10934529609376487
3	GU Jun， YANG Qin， LIU Yu. Mainstream anammox in a novel A-2B process for energy-efficient municipal wastewater treatment with minimized sludge production［J］. Water Research，2018，138：1-6. doi:10.1016/j.watres.2018.02.051
4	WIESMANN U. Biological nitrogen removal from wastewater［J］. Advances in Biochemical Engineering/Biotechnology，1994，51：113-154. doi:10.1007/bfb0008736
5	HANAKI K， WANTAWIN C， OHGAKI S. Nitrification at low levels of dissolved oxygen with and without organic loading in a suspended-growth reactor［J］. Water Research，1990，24（3）：297-302. doi:10.1016/0043-1354(90)90004-p
6	PARK S，BAE W， CHUNG J，et al. Empirical model of the pH dependence of the maximum specific nitrification rate［J］. Process Biochemistry，2007，42（12）：1671-1676. doi:10.1016/j.procbio.2007.09.010
7	BAE W， BAEK S， CHUNG J，et al. Optimal operational factors for nitrite accumulation in batch reactors［J］. Biodegradation，2001，12（5）：359-366. doi:10.1023/a:1014308229656
8	GANIGUÉ R， LÓPEZ H， BALAGUER M D，et al. Partial ammonium oxidation to nitrite of high ammonium content urban landfill leachates［J］. Water Research，2007，41（15）：3317-3326. doi:10.1016/j.watres.2007.04.027
9	ZHANG Zhengzhe， ZHANG Yu， CHEN Yinguang. Recent advances in partial denitrification in biological nitrogen removal：From enrichment to application［J］. Bioresource Technology，2020，298：122444. doi:10.1016/j.biortech.2019.122444
10	MA Bin， WANG Shanyun， CAO Shenbin，et al. Biological nitrogen removal from sewage via anammox：Recent advances［J］. Bioresource Technology，2016，200：981-990. doi:10.1016/j.biortech.2015.10.074
11	ZHANG Meng， WANG Siyu， JI Bin，et al. Towards mainstream deammonification of municipal wastewater：Partial nitrification-anammox versus partial denitrification-anammox［J］. Science of the Total Environment，2019，692：393-401. doi:10.1016/j.scitotenv.2019.07.293
12	GE Shijian， PENG Yongzhen， WANG Shuying，et al. Nitrite accumulation under constant temperature in anoxic denitrification process：The effects of carbon sources and COD/NO₃-N［J］. Bioresource Technology，2012，114：137-143. doi:10.1016/j.biortech.2012.03.016
13	CAO Xiangsheng， QIAN Dong， MENG Xuezheng. Effects of pH on nitrite accumulation during wastewater denitrification［J］. Environmental Technology，2013，34（1）：45-51. doi:10.1080/09593330.2012.679700
14	OH J， SILVERSTEIN J. Acetate limitation and nitrite accumulation during denitrification［J］. Journal of Environmental Engineering，1999，125（3）：234-242. doi:10.1061/(asce)0733-9372(1999)125:3(234)
15	SHI Liangliang， DU Rui， PENG Yongzhen. Achieving partial denitrification using carbon sources in domestic wastewater with waste-activated sludge as inoculum［J］. Bioresource Technology，2019，283：18-27. doi:10.1016/j.biortech.2019.03.063
16	CUI Bin， LIU Xiuhong， YANG Qing，et al. Achieving partial denitrification through control of biofilm structure during biofilm growth in denitrifying biofilter［J］. Bioresource Technology，2017，238：223-231. doi:10.1016/j.biortech.2017.04.034
17	SI Zheng， PENG Yongzhen， YANG Anming，et al. Rapid nitrite production via partial denitrification：Pilot-scale operation and microbial community analysis［J］. Environmental Science：Water Research & Technology，2018，4（1）：80-86. doi:10.1039/c7ew00252a
18	LI Wei， LI Hui， LIU Yongdi，et al. Salinity-aided selection of progressive onset denitrifiers as a means of providing nitrite for anammox［J］. Environmental Science & Technology，2018，52（18）：10665-10672. doi:10.1021/acs.est.8b02314
19	LI Wei， LIN Xiaoyu， CHEN Junjie，et al. Enrichment of denitratating bacteria from a methylotrophic denitrifying culture［J］. Applied Microbiology and Biotechnology，2016，100（23）：10203-10213. doi:10.1007/s00253-016-7859-z
20	DU Rui， CAO Shenbin， LI Baikun，et al. Performance and microbial community analysis of a novel DEAMOX based on partial-denitrification and anammox treating ammonia and nitrate wastewaters［J］. Water Research，2017，108：46-56. doi:10.1016/j.watres.2016.10.051
21	CUI Bin， LIU Xiuhong， YANG Qing，et al. Achieving partial denitrification through control of biofilm structure during biofilm growth in denitrifying biofilter［J］. Bioresource Technology，2017，238：223-231. doi:10.1016/j.biortech.2017.04.034
22	付昆明，曹相生，孟雪征，等. 污水反硝化过程中亚硝酸盐的积累规律［J］. 环境科学，2011，32（6）：1660-1664.
	FU Kunming， CAO Xiangsheng， MENG Xuezheng，et al. Characteristics of nitrite accumulation during wastewater denitrification［J］. Environmental Science，2011，32（6）：1660-1664.
23	CHEN Xiang， LAI Cheng， WANG Xinyi，et al. High-rate partial denitrification via effluent residual nitrate controlling and microbial mechanism of nitrite accumulation by carbon dosage optimization［J］. Water Science and Technology，2022，86（5）：1222-1231. doi:10.2166/wst.2022.203
24	CAO Shenbin， LAN Yu， DU Rui，et al. Robustness and stability of acetate-driven partial denitrification（PD） in response to high COD/NO₃ ^--N［J］. 2023-03-11. DOI：10.1016/J.CHEMOSPHERE. 2023.138213 .
25	QIAN Wenting， MA Bin， LI Xiyao，et al. Long-term effect of pH on denitrification：High pH benefits achieving partial-denitrifica tion［J］. Bioresource Technology，2019，278：444-449. doi:10.1016/j.biortech.2019.01.105
26	ZHOU Beibei， DUAN Jingjing， XUE Lihong，et al. Effect of plant-based carbon source supplements on denitrification of synthetic wastewater：Focus on the microbiology［J］. Environmental Science and Pollution Research，2019，26（24）：24683-24694. doi:10.1007/s11356-019-05454-x
27	SHI Liangliang， DU Rui， PENG Yongzhen. Achieving partial denitrification using carbon sources in domestic wastewater with waste-activated sludge as inoculum［J］. Bioresource Technology，2019，283：18-27. doi:10.1016/j.biortech.2019.03.063
28	SI Zheng， PENG Yongzhen， YANG Anming，et al. Rapid nitrite production via partial denitrification：Pilot-scale operation and microbial community analysis［J］. Environmental Science：Water Research & Technology，2018，4（1）：80-86. doi:10.1039/c7ew00252a
29	MORGAN-SAGASTUME F， NIELSEN J L， NIELSEN P H. Substrate-dependent denitrification of abundant probe-defined denitrifying bacteria in activated sludge［J］. FEMS Microbiology Ecology，2008，66（2）：447-461. doi:10.1111/j.1574-6941.2008.00571.x
30	LIU Chunshuang， LI Yanzhe， GAI Jianing，et al. Cultivation of sulfide-driven partial denitrification granules for efficient nitrite generation from nitrate-sulfide-laden wastewater［J］. Science of the Total Environment，2022，804：150143. doi:10.1016/j.scitotenv.2021.150143
31	赖城. 稀土矿山氨氮尾水短程反硝化实验研究［D］. 赣州：江西理工大学，2021.
	LAI Cheng. Experimental study on short-range denitrification of ammonia nitrogen tail water in rare earth mines［D］. Ganzhou：Jiangxi University of Science and Technology，2021.
32	DONG Jingjing， ZHANG Zhiming， YU Zhuodong，et al. Evolution and functional analysis of extracellular polymeric substances during the granulation of aerobic sludge used to treat p-chloroaniline wastewater［J］. Chemical Engineering Journal，2017，330：596-604. doi:10.1016/j.cej.2017.07.174
33	LI Qiang， ZHANG Bingjian， GE Qinya，et al. Calcium carbonate precipitation induced by calcifying bacteria in culture experiments：Influence of the medium on morphology and mineralogy［J］. International Biodeterioration & Biodegradation，2018，134：83-92. doi:10.1016/j.ibiod.2018.08.006

阶段	时间段	ρ（COD）/ρ（NO₃ ^-）	HRT/h	pH	加药
Ⅰ	第1~30天	5→2.1	4	8.3~8.7	搅拌时
Ⅱ	第31~44天	2.0	4	8.3~8.7	搅拌时
	第45~60天	2.0	4	8.8~9.2	搅拌时
	第61~70天	2.0	4	8.8~9.2	搅拌前
Ⅲ	第71~112天	2.0	4	8.3~8.7	搅拌前
Ⅲ	第113~120天	2.0	3	8.3~8.7	搅拌前

阶段	时间段	ρ（COD）/ρ（NO₃ ^-）	HRT/h	pH	加药
Ⅰ	第1~30天	5→2.1	4	8.3~8.7	搅拌时
Ⅱ	第31~44天	2.0	4	8.3~8.7	搅拌时
	第45~60天	2.0	4	8.8~9.2	搅拌时
	第61~70天	2.0	4	8.8~9.2	搅拌前
Ⅲ	第71~112天	2.0	4	8.3~8.7	搅拌前
Ⅲ	第113~120天	2.0	3	8.3~8.7	搅拌前

项目	方法	仪器
NH₄ ⁺	纳氏试剂分光光度法	元析仪器X-5型紫外/可见分光光度计
NO₂ ^-	N-（1-萘基）-乙二胺分光光度法
NO₃ ^-	紫外分光光度法
COD	快速测定法	连华科技5B-1型COD快速测定仪
DO	在线监测	威仪森WYS-DO10型在线溶解氧监测仪
pH	在线监测	威仪森WYS-PH10型pH/ORP计
温度	在线监测	威仪森WYS-PH10型pH/ORP计

项目	方法	仪器
NH₄ ⁺	纳氏试剂分光光度法	元析仪器X-5型紫外/可见分光光度计
NO₂ ^-	N-（1-萘基）-乙二胺分光光度法
NO₃ ^-	紫外分光光度法
COD	快速测定法	连华科技5B-1型COD快速测定仪
DO	在线监测	威仪森WYS-DO10型在线溶解氧监测仪
pH	在线监测	威仪森WYS-PH10型pH/ORP计
温度	在线监测	威仪森WYS-PH10型pH/ORP计

样品	序列读数	OTUs	丰富度指数		多样性指数		覆盖率/%
样品	序列读数	OTUs	Ace	Chao1	Simpson	Shannon	覆盖率/%
D1	39 480	853	911.78	926.99	0.009 5	5.43	99.74
D2	39 380	746	835.03	851.17	0.045 6	4.29	99.66
D3	42 371	633	754.03	760.75	0.044 0	4.01	99.65
D4	40 644	427	521.92	506.84	0.038 4	3.85	99.75

选择文件类型/文献管理软件名称

选择包含的内容