硫自养反硝化工艺亚硝酸盐积累研究进展

doi:10.19965/j.cnki.iwt.2023-0786

摘要/Abstract

摘要：

厌氧氨氧化（Anammox）由于具有不需外加碳源、污泥产量少、运行费用低等优势，被认为是一种最为高效、经济的污水生物脱氮新技术。然而，亚硝酸盐（NO₂ ^--N）积累是Anammox发生的必要前提。研究表明：短程硝化存在亚硝酸盐氧化菌活性难以稳定抑制的问题，而异养短程反硝化又存在需要外加碳源、碳排放量大等问题。近年来，硫驱动的短程自养反硝化（SPAD）作为一种NO₃ ^--N还原为NO₂ ^--N的新方法，因其具有不需要投加有机碳源、经济成本低、环境友好等优势而受到广泛关注。基于此，结合大量国内外文献，全面介绍了SPAD的工艺原理、NO₂ ^--N积累影响因素、脱氮过程副产物、关键菌群和功能基因，并系统总结了SPAD处理效能，最后对各种类型SPAD工艺的经济性能进行了比较分析并提出了未来的研究展望。

关键词: 硫短程自养反硝化, 亚硝酸盐积累, 电子供体

Abstract:

Anaerobic ammonia oxidation (Anammox) is regarded as one of the most cost-effective wastewater biological nitrogen removal technologies due to no need for external organics, low sludge production,and low operating costs. However, nitrite (NO₂ ^--N) accumulation is an necessary prerequisite for Anammox. Researches have shown that partial nitrification has the difficulty of stably suppressing the activity of nitrite oxidizing bacteria, while heterotrophic partial denitrification has some issues such as additional carbon source and high carbon emissions. In recent years, sulfur-based partial autotrophic denitrification(SPAD) as a new method of reducing NO₃ ^--N to NO₂ ^--N has attracted extensive attentions because of no need for external organic carbons, low economic costs, and environmental friendliness. Therefore, the study comprehensively reviewed the process principle, NO₂ ^--N accumulation influencing factors, by-products of denitrification process, key bacterial and functional genes and systematically summarized the efficiency of SPAD. Finally, the economic performance of different types of SPAD was compared and the future research prospect was proposed.

Key words: sulfur-based partial autotrophic denitrification, nitrite accumulation, electronic donors

中图分类号:

X703

平彩霞, 周鑫, 聂裕婷. 硫自养反硝化工艺亚硝酸盐积累研究进展[J]. 工业水处理, 2024, 44(8): 21-28.

Caixia PING, Xin ZHOU, Yuting NIE. Research progress on nitrite accumulation in sulfur-based autotrophic denitrification process[J]. Industrial Water Treatment, 2024, 44(8): 21-28.

https://www.iwt.cn/CN/Y2024/V44/I8/21

图/表 4

表1 硫自养反硝化反应方程式和反应吉布斯自由能

Table 1 Reaction equation and Gibbs free energy of reaction of sulfur autotrophic denitrification

电子供体	反应方程式	ΔG/（kJ·mol^-1）	参考文献
S^2-	S^2-+1.6NO₃ ^-+1.6H⁺ $→$ 0.8N₂+SO₄ ^2-+0.8H₂O	-744.0	〔6-8〕
	S^2-+0.4NO₃ ^-+2.4H⁺ $→$ 0.2N₂+S⁰+1.2H₂O	-240.3
	S^2-+0.4NO₃ ^-+2.4H⁺ $→$ 0.2N₂+S⁰+1.2H₂O	-191.0
	S^2-+4NO₃ ^- $→$ 4NO₂ ^-+SO₄ ^2-	-130.4
	S^2-+NO₃ ^-+2H⁺ $→$ NO₂ ^-+S⁰+H₂O	-130.4
HS^-	5HS^-+8NO₃ ^-+3H⁺ $→$ 4N₂+5SO₄ ^2-+4H₂O	-3 848.0	〔9-11〕
	HS^-+4NO₃ ^- $→$ 4NO₂ ^-+SO₄ ^2-+4H⁺	-480.2
	HS^-+0.4NO₃ ^-+1.4H⁺ $→$ 0.2N₂+5S⁰+1.2H₂O	-252.8
	HS^-+NO₃ ^-+H⁺ $→$ 0.2NO₂ ^-+S⁰+H₂O	-130.3
	5HS^-+5NO₃ ^-+5H⁺ $→$ 2.5N₂+2.5SO₄ ^2-+2.5S⁰+5H₂O	—
SCN^-	SCN^-+1.6NO₃ ^-+0.2H₂O+1.6H⁺+HCO₃ ^- $→$ SO₄ ^2-+NH₃+2CO₂+0.8N₂	—	〔12-13〕
	5SCN^-+8NO₃ ^- $→$ 5SO₄ ^2-+5NH₄ ⁺+5HCO₃ ^-+4N₂+3OH^-	—
	3SCN^-+11NO₂ ^-+8H⁺ $→$ 3SO₄ ^2-+3CO₂+7N₂	—
S⁰	S⁰+1.2NO₃ ^-+0.4H₂O $→$ SO₄ ^2-+0.6N₂+0.8H⁺	-548.0	〔6，14〕
S⁰	S⁰+2NO₃ ^-+4H⁺ $→$ SO₄ ^2-+N₂+2H₂O	-1 269.6	〔6，14〕
S₂O₃ ^2-	S₂O₃ ^2-+1.6NO₃ ^-+0.2H₂O $→$ 2SO₄ ^2-+0.8N₂+0.4H⁺	-766.0	〔6，15〕
	S₂O₃ ^2-+NO₃ ^- $→$ SO₄ ^2-+NO₂ ^-+S⁰	—
	0.75S₂O₃ ^2-+2NO₂ ^-+0.5H⁺ $→$ 1.5SO₄ ^2-+N₂+0.25H₂O	—
SO₃ ^2-	SO₃ ^2-+NO₃ ^- $→$ NO₂ ^-+SO₄ ^2-	-184.0	〔16〕
	3SO₃ ^2-+2NO₂ ^-+2H⁺ $→$ N₂+3SO₄ ^2-+H₂O	-854.0
	5SO₃ ^2-+2NO₃ ^-+H₂O $→$ N₂+5SO₄ ^2-+2OH^-	-1 225.0

表1 硫自养反硝化反应方程式和反应吉布斯自由能

Table 1 Reaction equation and Gibbs free energy of reaction of sulfur autotrophic denitrification

电子供体	反应方程式	ΔG/（kJ·mol^-1）	参考文献
S^2-	S^2-+1.6NO₃ ^-+1.6H⁺ $→$ 0.8N₂+SO₄ ^2-+0.8H₂O	-744.0	〔6-8〕
	S^2-+0.4NO₃ ^-+2.4H⁺ $→$ 0.2N₂+S⁰+1.2H₂O	-240.3
	S^2-+0.4NO₃ ^-+2.4H⁺ $→$ 0.2N₂+S⁰+1.2H₂O	-191.0
	S^2-+4NO₃ ^- $→$ 4NO₂ ^-+SO₄ ^2-	-130.4
	S^2-+NO₃ ^-+2H⁺ $→$ NO₂ ^-+S⁰+H₂O	-130.4
HS^-	5HS^-+8NO₃ ^-+3H⁺ $→$ 4N₂+5SO₄ ^2-+4H₂O	-3 848.0	〔9-11〕
	HS^-+4NO₃ ^- $→$ 4NO₂ ^-+SO₄ ^2-+4H⁺	-480.2
	HS^-+0.4NO₃ ^-+1.4H⁺ $→$ 0.2N₂+5S⁰+1.2H₂O	-252.8
	HS^-+NO₃ ^-+H⁺ $→$ 0.2NO₂ ^-+S⁰+H₂O	-130.3
	5HS^-+5NO₃ ^-+5H⁺ $→$ 2.5N₂+2.5SO₄ ^2-+2.5S⁰+5H₂O	—
SCN^-	SCN^-+1.6NO₃ ^-+0.2H₂O+1.6H⁺+HCO₃ ^- $→$ SO₄ ^2-+NH₃+2CO₂+0.8N₂	—	〔12-13〕
	5SCN^-+8NO₃ ^- $→$ 5SO₄ ^2-+5NH₄ ⁺+5HCO₃ ^-+4N₂+3OH^-	—
	3SCN^-+11NO₂ ^-+8H⁺ $→$ 3SO₄ ^2-+3CO₂+7N₂	—
S⁰	S⁰+1.2NO₃ ^-+0.4H₂O $→$ SO₄ ^2-+0.6N₂+0.8H⁺	-548.0	〔6，14〕
S⁰	S⁰+2NO₃ ^-+4H⁺ $→$ SO₄ ^2-+N₂+2H₂O	-1 269.6	〔6，14〕
S₂O₃ ^2-	S₂O₃ ^2-+1.6NO₃ ^-+0.2H₂O $→$ 2SO₄ ^2-+0.8N₂+0.4H⁺	-766.0	〔6，15〕
	S₂O₃ ^2-+NO₃ ^- $→$ SO₄ ^2-+NO₂ ^-+S⁰	—
	0.75S₂O₃ ^2-+2NO₂ ^-+0.5H⁺ $→$ 1.5SO₄ ^2-+N₂+0.25H₂O	—
SO₃ ^2-	SO₃ ^2-+NO₃ ^- $→$ NO₂ ^-+SO₄ ^2-	-184.0	〔16〕
	3SO₃ ^2-+2NO₂ ^-+2H⁺ $→$ N₂+3SO₄ ^2-+H₂O	-854.0
	5SO₃ ^2-+2NO₃ ^-+H₂O $→$ N₂+5SO₄ ^2-+2OH^-	-1 225.0

表2 SPAD相关关键菌群、微生物功能和还原产物

Table 2 Key bacteria，microbial functions and denitrifying products related to SPAD

菌属	门类	功能	还原产物
Thiobacillus	变形杆菌门	硫自养（短程）反硝化	N₂、N₂O、NO、NO₂ ^--N
Thiomonas	变形杆菌门	兼性自养硫氧化	NO₂ ^--N
Sulfurimonas	弯曲杆菌门	氢和硫氧化	NO₂ ^--N
Thauera	变形杆菌门	短程反硝化	NO₂ ^--N、N₂
Thermomonas	变形杆菌门	硫自养（短程）反硝化	N₂、N₂O、NO、NO₂ ^--N
Azoarcus	变形杆菌门	硫自养反硝化	N₂

表3 SPAD工艺亚硝酸盐积累性能

Table 3 Nitrite accumulation performance of SPAD process

电子供体	反应器	NO₃ ^--N	pH	S/N	NAR/%	参考文献
S^2-	UASB	300 mg/L 100 mg/L	7.5	0.29 1.32	80 70	〔38〕
S^2-	SBR	180 mg/L 120 mg/L	8.0	0.8	55.3 35.6	〔7〕
S^2-	DSSADN	100 mg/L	8~8.5	0.8	81.9	〔18〕
S^2-	CSTR	200 mg/L	7.6	0.65	70	〔10〕
HS^-	CSTR	100 mg/L	7.6	1.76 0.67	5 63	〔10〕
HS^-	CSTR	110 mg/L 200 mg/L	7.6	0.65	63 70	〔10〕
S⁰	SBR	50 mg/L 100 mg/L 400 mg/L	8	NA	70.65 100 45	〔17〕
S⁰	SBR	50 mg/L	7 8	NA	50.32 90.82	〔17〕
S⁰	SBR	100 mg/L 200 mg/L 300 mg/L	8.5	—	100 80 80	〔24〕
S₂O₃ ^2-	UASB	100 mg/L	8	3.5 2	7.2 18.6	〔1〕
S₂O₃ ^2-	UASB	100 mg/L 200 mg/L	8	2	18.6 52.2	〔1〕
S₂O₃ ^2-	血清瓶	10 mmol/L	7 8	1	100 80	〔15〕
S₂O₃ ^2-	血清瓶	10 mmol/L	7	5 1	<100 100	〔15〕
SO₃ ^2-	SBR	100 mg/L	7	0.44	21.9	〔36〕
SO₃ ^2-	SBBR	250 mg/L	7.5	0.8 1.7 2.6	32.3 64.7 12	〔25〕

表4 不同类型SPAD工艺技术和经济性能评价

Table 4 Evaluation of different types of SPAD process technology and economic performance

电子供体	还原性	可利用性	毒性	是否加碱	NO₂ ^--N 积累难度	可获取性	经济成本
S^2-	最强	高	高	需要	较高	容易	低
HS^-	最强	高	高	需要	较高	容易	低
S⁰	居中	最低	无	不需要	较低	较难	高
S₂O₃ ^2-	居中	高	低	需要	较低	较难	较高
SO₃ ^2-	较弱	高	低	不需要	较低	较容易	较低

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