Construction of a coupled process integrating dissimilatory nitrate reduction and anaerobic ammonia oxidation/denitrification for wastewater treatment

doi:10.16085/j.issn.1000-6613.2023-0449

Abstract

Abstract:

An anaerobic expanded granular sludge bed reactor (EGSB) was used to treat simulated wastewater containing COD, ammonia and nitrate nitrogen to rapidly establish anaerobic ammonium oxidation (Anammox) process in a high-concentration organic wastewater treatment system. By inoculating a small amount of Anammox sludge and gradually increasing the concentration of ammonia nitrogen, the system successfully started the Anammox reaction after 58d of continuous operation, at which the total nitrogen and COD removal efficiencies were stable to over 97% and 98%, respectively. Mass balance showed that the contribution of Anammox reaction pathway to nitrogen removal gradually increased, and dissimilatory nitrate reduction (DNRA) coupled with Anammox and denitrification together contributed to simultaneous nitrogen and carbon removal in the system. Microbial community analysis found that the relative abundance of Candidatus Kuenenia rapidly increased from 0.27% to 35.87%, and DNRA bacteria (Ignavibacterium, Thermogutta) and denitrification bacteria (Azospira, Gp3) co-existed in the system. The key functional genes of Anammox, DNRA, nitrate reduction and nitrite reduction were detected by gene annotation method. During the operation, the granular sludge turned reddish in color and its particle size increased. Extracellular polymeric substance (EPS) analysis showed an increase in polysaccharide (PS) and protein (PN) contents and a decrease in PN/PS. Three-dimensional fluorescence spectroscopy revealed an increase in humic acid-like substances. These results of the study provide a novel process pathway for efficient treatment of high concentration organic nitrogenous wastewater.

Key words: expanded granular sludge bed reactor, high concentration organic nitrogenous wastewater, dissimilatory nitrate reduction, anaerobic ammonia oxidation, denitrification, coupled nitrogen removal

摘要：

采用厌氧膨胀颗粒污泥床反应器（EGSB）处理含COD、氨氮和硝氮的模拟废水，旨在高浓度有机废水处理系统中快速构建厌氧氨氧化（Anammox）运行工艺。通过接种少量Anammox污泥和逐步提高氨氮浓度的操作方式，在连续运行58d后，系统成功启动Anammox反应，此时的总氮和COD去除率稳定在97%和98%以上。物料衡算显示，Anammox反应途径对氮的去除贡献逐渐增加，硝酸盐异化还原（DNRA）耦合Anammox和反硝化共同促进了系统的同步脱氮除碳。对微生物群落分析发现，Candidatus Kuenenia相对丰度由0.27%快速升高至35.87%，DNRA菌（Ignavibacterium、Thermogutta）及反硝化菌（Azospira、Gp3）在体系内共存。通过基因注释法，检测出了Anammox、DNRA、硝酸盐还原及亚硝酸盐还原关键基因。运行过程中，颗粒污泥颜色变红且粒径增大；胞外聚合物（EPS）分析表明多糖（PS）和蛋白质（PN）含量增加而PN/PS下降；三维荧光光谱发现腐殖酸类物质增多。研究结果为高浓度有机含氮废水高效处理提供了一种新的工艺途径。

关键词: 膨胀颗粒污泥床反应器, 高浓度有机含氮废水, 硝酸盐异化还原, 厌氧氨氧化, 反硝化, 耦合脱氮

CLC Number:

X703

ZHAO Ruiqiang, ZHOU Xin, NIU Bingxin. Construction of a coupled process integrating dissimilatory nitrate reduction and anaerobic ammonia oxidation/denitrification for wastewater treatment[J]. Chemical Industry and Engineering Progress, 2024, 43(3): 1593-1605.

赵瑞强, 周鑫, 牛冰心. 废水处理硝酸盐异化还原与厌氧氨氧化/反硝化耦合工艺构建[J]. 化工进展, 2024, 43(3): 1593-1605.

Figures/Tables 12

阶段	时间/d	COD/mg·L^-1	NO $3 -$ -N/mg·L^-1	NH $4 +$ -N/mg·L^-1	总氮进水负荷/kg N·m^-3·d^-1	COD进水负荷/kg COD·m^-3·d^-1	HRT/d	C/N
S1	1~24	2000	500	0	0.25	1.0	2	4.0
S2	25~40	2000	500	50	0.27	1.0	2	3.6
S3	41~58	2000	500	100	0.30	1.0	2	3.3
S4	59~75	2000	500	200	0.35	1.0	2	2.8

阶段	时间/d	COD/mg·L^-1	NO $3 -$ -N/mg·L^-1	NH $4 +$ -N/mg·L^-1	总氮进水负荷/kg N·m^-3·d^-1	COD进水负荷/kg COD·m^-3·d^-1	HRT/d	C/N
S1	1~24	2000	500	0	0.25	1.0	2	4.0
S2	25~40	2000	500	50	0.27	1.0	2	3.6
S3	41~58	2000	500	100	0.30	1.0	2	3.3
S4	59~75	2000	500	200	0.35	1.0	2	2.8

阶段	出水			TN去除负荷/kg·m^-3·d^-1	TN去除率/%	COD去除率/%
阶段	NH $4 +$ -N/mg·L^-1	NO $2 -$ -N/mg·L^-1	NO $3 -$ -N/mg·L^-1	TN去除负荷/kg·m^-3·d^-1	TN去除率/%	COD去除率/%
S1	13.3±5.8	6.9±1.0	9.0±3.8	0.22±0.01	93.7±1.4	94.8
S2	3.7±4.3	3.6±2.2	6.1±4.0	0.25±0.01	97.3±1.6	97.1
S3	0.0	2.0±2.4	3.7±1.8	0.29±0.01	99.0±0.6	98.1
S4	8.0±7.4	4.6±2.2	6.4±2.5	0.34±0.01	97.3±1.2	98.6

阶段	出水			TN去除负荷/kg·m^-3·d^-1	TN去除率/%	COD去除率/%
阶段	NH $4 +$ -N/mg·L^-1	NO $2 -$ -N/mg·L^-1	NO $3 -$ -N/mg·L^-1	TN去除负荷/kg·m^-3·d^-1	TN去除率/%	COD去除率/%
S1	13.3±5.8	6.9±1.0	9.0±3.8	0.22±0.01	93.7±1.4	94.8
S2	3.7±4.3	3.6±2.2	6.1±4.0	0.25±0.01	97.3±1.6	97.1
S3	0.0	2.0±2.4	3.7±1.8	0.29±0.01	99.0±0.6	98.1
S4	8.0±7.4	4.6±2.2	6.4±2.5	0.34±0.01	97.3±1.2	98.6

反应器	主要反应	进水COD浓度 /mg·L^-1	C/N	进水氮类型	TN进水负荷 /kg·m^-3·d^-1	TN去除负荷 /kg·m^-3·d^-1	TN去除率 /%	参考文献
EGSB	DNRA、Anammox、反硝化	2000	2.8	NH $4 +$ -N、NO $3 -$ -N	0.35	0.34	97.3	本研究
UASB	PD/A	102	1.7	NH $4 +$ -N、NO $3 -$ -N	0.96	0.79	82.3	[19]
UASB	PD/A	210	2	NH $4 +$ -N、NO $3 -$ -N	0.50	0.45	90	[20]
SBR	SAD	150	0.625	NH $4 +$ -N、NO $2 -$ -N	0.72	0.65	86.7	[21]
nMBR	DNRA、Anammox、反硝化	850	10	NO $3 -$ -N	0.24	0.10	40	[22]

反应器	主要反应	进水COD浓度 /mg·L^-1	C/N	进水氮类型	TN进水负荷 /kg·m^-3·d^-1	TN去除负荷 /kg·m^-3·d^-1	TN去除率 /%	参考文献
EGSB	DNRA、Anammox、反硝化	2000	2.8	NH $4 +$ -N、NO $3 -$ -N	0.35	0.34	97.3	本研究
UASB	PD/A	102	1.7	NH $4 +$ -N、NO $3 -$ -N	0.96	0.79	82.3	[19]
UASB	PD/A	210	2	NH $4 +$ -N、NO $3 -$ -N	0.50	0.45	90	[20]
SBR	SAD	150	0.625	NH $4 +$ -N、NO $2 -$ -N	0.72	0.65	86.7	[21]
nMBR	DNRA、Anammox、反硝化	850	10	NO $3 -$ -N	0.24	0.10	40	[22]

反应器	接种污泥	培养方式	进水氮源	最高总氮去除率/%	启动时间/d	参考文献
EGSB	厌氧颗粒污泥、5%厌氧氨氧化污泥	有机添加	NH $4 +$ -N、NO $3 -$ -N	99.0±0.6	58	本研究
UASB	厌氧氨氧化污泥和活性污泥，体积比1∶2	无机添加	NH $4 +$ -N、NO $2 -$ -N	87.60	90	[23]
EGSB	厌氧颗粒污泥	无机添加	NH $4 +$ -N、NO $2 -$ -N	83	93	[24]
	好氧活性污泥	无机添加		81	63
ABBR	好氧活性污泥	无机添加	NH $4 +$ -N、NO $2 -$ -N	＞70	47	[25]
UASB	混合活性污泥	无机添加	NH $4 +$ -N、NO $2 -$ -N	98	85	[26]
MBR	混合活性污泥	无机添加	NH $4 +$ -N、NO $2 -$ -N	＞90	59	[27]
ASBR	恶臭沉积物	无机添加	NH $4 +$ -N、NO $2 -$ -N	53.7	60	[16]

反应器	接种污泥	培养方式	进水氮源	最高总氮去除率/%	启动时间/d	参考文献
EGSB	厌氧颗粒污泥、5%厌氧氨氧化污泥	有机添加	NH $4 +$ -N、NO $3 -$ -N	99.0±0.6	58	本研究
UASB	厌氧氨氧化污泥和活性污泥，体积比1∶2	无机添加	NH $4 +$ -N、NO $2 -$ -N	87.60	90	[23]
EGSB	厌氧颗粒污泥	无机添加	NH $4 +$ -N、NO $2 -$ -N	83	93	[24]
	好氧活性污泥	无机添加		81	63
ABBR	好氧活性污泥	无机添加	NH $4 +$ -N、NO $2 -$ -N	＞70	47	[25]
UASB	混合活性污泥	无机添加	NH $4 +$ -N、NO $2 -$ -N	98	85	[26]
MBR	混合活性污泥	无机添加	NH $4 +$ -N、NO $2 -$ -N	＞90	59	[27]
ASBR	恶臭沉积物	无机添加	NH $4 +$ -N、NO $2 -$ -N	53.7	60	[16]

EPS	阶段	A峰		B峰		C峰		D峰		E峰
EPS	阶段	（E_x/E_m） /(nm/nm)	荧光强度	（E_x/E_m） /(nm/nm)	荧光强度	（E_x/E_m） /(nm/nm)	荧光强度	（E_x/E_m） /(nm/nm)	荧光强度	（E_x/E_m） /(nm/nm)	荧光强度
S-EPS	S1	222/330	64983	282/315	44313	354/460	18571	256/460	19266
	S4	218/295	40230	270/300	36790
LB-EPS	S1	220/335	59948	278/335	41359	362/460	14143	254/460	14757
	S4	216/295	23497	272/300	24818
TB-EPS	S1	226/345	326406	286/350	750172					382/465	30047
	S4	226/345	214944	284/345	472846

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