ABR产酸-硫酸盐还原相颗粒污泥富集PHAs产生菌

doi:10.16085/j.issn.1000-6613.2023-0203

摘要/Abstract

摘要：

为探究硫酸盐有机废水厌氧处理合成聚羟基脂肪酸酯（PHAs）的可行性，利用五隔室厌氧折流板反应器（ABR）以硫酸盐有机废水为底物富集PHAs产生菌合成PHAs，考察不同进水COD/SO₄^2-比值（12.5、9.3、4.0）对ABR产酸-硫酸盐还原相（第1、第2隔室）颗粒污泥PHAs合成效果的影响，进而探讨该体系中PHAs合成模式。结果表明：随进水COD/SO₄^2-比值降低，产酸-硫酸盐还原相的COD与SO₄^2-去除沿程后移，第1隔室呈现丁酸型代谢类型为主，第2隔室由乙酸型转为丁酸型代谢类型为主；颗粒污泥PHAs的高含量隔室由第1隔室后移至第2隔室，其中COD/SO₄^2-比值为9.3时，产酸-硫酸盐还原相中颗粒污泥PHAs产生菌大量富集、PHAs合成效果最好；在颗粒污泥中PHAs产生菌个体大，PHAs颗粒密集地布满整个菌体细胞；产酸-硫酸盐还原相中存在产酸菌（APB）、脂肪酸型硫酸盐还原菌（FSRB）、乙酸型硫酸盐还原菌（ASRB）生物链式协同代谢模式，并且在菌体内形成大量PHAs。该研究为硫酸盐有机废水的资源化利用提供理论支持。

关键词: 聚羟基脂肪酸酯, 厌氧折流板反应器, 产酸-硫酸盐还原相, 代谢类型, 合成途径

Abstract:

In order to investigate the feasibility of synthesizing polyhydroxyalkanoates (PHAs) from sulfate organic wastewater through anaerobic treatment, a five-compartment anaerobic baffled reactor (ABR) was utilized to enrich PHAs-producing bacteria using sulfate organic wastewater as substrate, and the effects of different influent COD/SO₄^2- ratios (12.5, 9.3 and 4.0) on PHAs synthesis efficiency of granular sludge in the acidogenic sulfate-reducing phase (the first and second compartments) of ABR were examined to explore the PHA synthesis pattern in this system. The results showed that as the inflow COD/SO₄^2- ratio decreased, the removal of COD and SO₄^2- in the acidogenic sulfate-reduction phase shifted downstream. In the first compartment, the dominant microbial metabolism type was the butyric acid type, while in the second compartment, it shifted from the acetic acid type to the butyric acid type. The compartment with high content of PHAs in the granular sludge shifted from the first compartment to the second compartment. The best PHAs synthesis effect was observed when the inflow COD/SO₄^2- ratio was 9.3, which led to a large enrichment of PHAs-producing bacteria and high production of PHAs in the granular sludge of the acidogenic sulfate-reduction phase. The PHAs-producing bacteria in the granular sludge were large, and the PHAs granules were densely distributed throughout the bacterial cells. In the acidogenic sulfate-reducing phase, there existed a bio-chain cooperation relationship among acid-producing bacteria (APB), fatty-acid utilized sulfate reducing bacteria (FSRB) and acetic-acid utilized sulfate reducing bacteria (ASRB), and a large amount of PHAs was formed inside the bacterial cells. This study provided theoretical support for the resource utilization of sulfate organic wastewater.

Key words: polyhydroxyalkanoates, anaerobic baffled reactor, acidogenic sulfate-reducing phase, metabolic type, synthesis pathway

中图分类号:

X703

汪晨祥, 秦永丽, 蒋永荣, 葛仕佳, 郑国权, 孙振举. ABR产酸-硫酸盐还原相颗粒污泥富集PHAs产生菌[J]. 化工进展, 2023, 42(12): 6658-6665.

WANG Chenxiang, QIN Yongli, JIANG Yongrong, GE Shijia, ZHENG Guoquan, SUN Zhenju. Enrichment of PHAs-producing bacteria by granular sludge in ABR acidogenic sulfate-reducing phase[J]. Chemical Industry and Engineering Progress, 2023, 42(12): 6658-6665.

图/表 8

图1 不同进水COD/SO42-比值下COD和SO42-平均去除率

表1 不同COD/SO42-值VFAs浓度及占比

VFAs	COD/SO₄^2-=12.5		COD/SO₄^2-=9.3		COD/SO₄^2-=4.0
VFAs	第1隔室	第2隔室	第1隔室	第2隔室	第1隔室	第2隔室
乙酸/mg·L^-1	414(29%)	894(69%)	462(28%)	1056(73%)	420(22%)	696(34%)
丙酸/mg·L^-1	215(15%)	140(11%)	251(15%)	96(7%)	200(11%)	185(9%)
丁酸/mg·L^-1	659(46%)	255(20%)	774(48%)	299(20%)	994(54%)	941(45%)
乳酸/mg·L^-1	135(10%)	未检出	144(9%)	未检出	234(13%)	243(12%)
总和/mg·L^-1	1423	1289	1631	1451	1848	2065

图2 不同进水COD/SO42-比值颗粒污泥中的PHAs含量变化情况

图3 进水COD/SO42-比值为12.5时颗粒污泥TEM图

图4 进水COD/SO42-比值为9.3时颗粒污泥TEM图

图5 进水COD/SO42-比值为4.0时颗粒污泥TEM图

图6 进水COD/SO42-比值为9.3时颗粒污泥FISH图

图7 产酸-硫酸盐还原相中PHAs合成途径

参考文献 15

15	JIANG Yongrong, LIU Kehui, LIU Chengliang, et al. A biological treatment device for sulfate organic wastewater: CN203429023U[P]. 2014-02-12.
16	国家环境保护总局. 水和废水监测分析方法[M]. 4版. 北京: 中国环境科学出版社, 2002.
	Environmental Protection Administration. Monitoring and analysis methods of water and wastewater[M]. 4th ed. Beijing: China Environmental Science Press, 2002.
17	贺延龄. 废水的厌氧生物处理[M]. 北京: 中国轻工业出版社, 1998: 514-530.
	HE Yanling. Anaerobic biological treatment of wastewater[M]. Beijing: China Light Industry Press, 1998: 514-530.
18	刘艳玲, 任南琪, 刘敏, 等. 气相色谱法分析厌氧反应器中的挥发性脂肪酸(VFA)[J]. 哈尔滨建筑大学学报, 2000(6): 31-34.
	LIU Yanling, REN Nanqi, LIU Min, et al. Analysis of volatile fatty acid (VFA) in anaerobic bio-reactor by gas chromatography[J]. Journal of Harbin University of Civil Engineering and Architecture, 2000(6): 31-34.
19	OEHMEN A, KELLER-LEHMANN B, ZENG R J, et al. Optimisation of poly-‍β‍-hydroxyalkanoate analysis using gas chromatography for enhanced biological phosphorus removal systems[J]. Journal of Chromatography A, 2005, 1070(1/2): 131-136.
20	BASSAS M. Isolation and analysis of storage compounds[M]. Handbook of Hydrocarbon and Lipid Microbiology, 2010.
21	左剑恶, 杨洋, 沈平, 等. 荧光原位杂交(FISH)技术在厌氧颗粒污泥研究中的应用[J]. 中国沼气, 2004, 22(1): 3-6.
	ZUO Jian'e, YANG Yang, SHEN Ping, et al. Application of fluorescent in situ hybridization technology in study on anaerobic granular sludge[J]. China Biogas, 2004, 22(1): 3-6.
22	郑维爽, 于盛洋, 翟生强, 等. 利用含油培养基富集、分离和评估海洋产聚羟基脂肪酸酯细菌[J]. 微生物学通报, 2021, 48(12): 4507-4520.
	ZHENG Weishuang, YU Shengyang, ZHAI Shengqiang, et al. Enrichment, isolation, and evaluation of polyhdroxyalkanoate-producing marine bacteria from oil-containing culture medium[J]. Microbiology China, 2021, 48(12): 4507-4520.
23	任南琪, 王爱杰, 林明. 乙酸型顶极群落的内平衡与反馈调节机制研究[J]. 环境科学学报, 2002, 22(5): 581-585.
	REN Nanqi, WANG Aijie, LIN Ming. The internal balance and the feedback adjustment of acetic acid type climax community[J]. Acta Scientiae Circumstantiae, 2002, 22(5): 581-585.
24	TAMANG P, NOGUEIRA R. Valorisation of waste cooking oil using mixed culture into short- and medium-chain length polyhydroxyalkanoates: Effect of concentration, temperature and ammonium[J]. Journal of Biotechnology, 2021, 342: 92-101.
25	王攀, 邱银权, 陈锡腾, 等. 以餐厨垃圾水解酸化液为碳源合成PHA研究[J]. 环境工程, 2018, 36(6): 145-149.
	WANG Pan, QIU Yinquan, CHEN Xiteng, et al. PHA production from the liquid of hydrolytic-acidogenic fermentation of food waste[J]. Environmental Engineering, 2018, 36(6): 145-149.
26	HAO Jiuxiao, WANG Xiujin, WANG Hui. Investigation of polyhydroxyalkanoates (PHAs) biosynthesis from mixed culture enriched by valerate-dominant hydrolysate[J]. Frontiers of Environmental Science & Engineering, 2017, 11(1): 5.
27	王琴, 陈银广. 活性污泥合成聚羟基烷酸(PHAs)的研究进展[J]. 环境科学与技术, 2007, 30(5): 111-114, 121.
	WANG Qin, CHEN Yinguang. Advance on polyhydroxyalkanoates production by activated sludge[J]. Environmental Science & Technology, 2007, 30(5): 111-114, 121.
28	LEMOS P C, SERAFIM L S, REIS M A M. Synthesis of polyhydroxyalkanoates from different short-chain fatty acids by mixed cultures submitted to aerobic dynamic feeding[J]. Journal of Biotechnology, 2006, 122(2): 226-238.
29	JIA Qianqian, WANG Hui, WANG Xiujin. Dynamic synthesis of polyhydroxyalkanoates by bacterial consortium from simulated excess sludge fermentation liquid[J]. Bioresource Technology, 2013, 140: 328-336.
30	NYGAARD D, YASHCHUK O, HERMIDA É B. PHA granule formation and degradation by Cupriavidus necator under different nutritional conditions[J]. Journal of Basic Microbiology, 2021, 61(9): 825-834.
1	COLOMBO B, PEPÈ SCIARRIA T, REIS M, et al. Polyhydroxyalkanoates (PHAs) production from fermented cheese whey by using a mixed microbial culture[J]. Bioresource Technology, 2016, 218: 692-699.
2	陶怡, 柯彦, 李俊彪, 等. 我国生物可降解塑料产业发展现状与展望[J]. 化工新型材料, 2020, 48(12): 1-4.
	TAO Yi, KE Yan, LI Junbiao, et al. Development status and prospect of biodegradable plastics industry in China[J]. New Chemical Materials, 2020, 48(12): 1-4.
3	陈心宇, 李梦怡, 陈国强. 聚羟基脂肪酸酯PHA代谢工程研究30年[J]. 生物工程学报, 2021, 37(5): 1794-1811.
	CHEN Xinyu, LI Mengyi, CHEN Guoqiang. Thirty years of metabolic engineering for biosynthesis of polyhydroxyalkanoates[J]. Chinese Journal of Biotechnology, 2021, 37(5): 1794-1811.
4	王娜, 宋秀兰, 昝博韬. 复合菌群利用模拟APG协同FNA预处理剩余污泥水解液合成PHA[J]. 化工进展, 2022, 41(2): 1017-1024.
	WANG Na, SONG Xiulan, ZAN Botao. Synthesis of PHA by mixed microorganisms using simulative hydrolysate liquid from the excess sludge by APG combined with FNA pretreatment[J]. Chemical Industry and Engineering Progress, 2022, 41(2): 1017-1024.
5	TAN Giin, CHEN Chia-Lung, LI Ling, et al. Start a research on biopolymer polyhydroxyalkanoate (PHA): A review[J]. Polymers, 2014, 6(3): 706-754.
6	郭子瑞, 黄龙, 陈志强, 等. 活性污泥合成聚羟基脂肪酸酯工艺过程研究进展[J]. 哈尔滨工业大学学报, 2016, 48(2): 1-8.
	GUO Zirui, HUANG Long, CHEN Zhiqiang, et al. Advances in polyhydroxyalkanoates synthesis by activated sludge[J]. Journal of Harbin Institute of Technology, 2016, 48(2): 1-8.
7	罗娜, 朱仲广, 秦永丽, 等. COD/SO₄ ^2-对硫酸盐有机废水厌氧处理颗粒污泥活性的影响[J]. 环境科学与技术, 2019, 42(1): 23-30.
	LUO Na, ZHU Zhongguang, QIN Yongli, et al. Effect of COD/SO₄ ^2- on activity of granular sludge in anaerobic treatment of organic wastewater containing sulfate[J]. Environmental Science & Technology, 2019, 42(1): 23-30.
31	TOJA ORTEGA S, VAN DEN BERG L, PRONK M, et al. Hydrolysis capacity of different sized granules in a full-scale aerobic granular sludge (AGS) reactor[J]. Water Research X, 2022, 16: 100151.
32	冉依禾, 郭亮, 刘一平, 等. 不同比例乙酸和丙酸对活性污泥微生物合成聚羟基脂肪酸酯的影响[J]. 环境工程学报, 2017, 11(2): 1276-1280.
	RAN Yihe, GUO Liang, LIU Yiping, et al. Effect of different ratios of acetic acid and propionic acid on microbial polyhydroxyalkanoate synthesis with activated sludge[J]. Chinese Journal of Environmental Engineering, 2017, 11(2): 1276-1280.
33	陈宏, 胡颖冰, 陈晨, 等. 氨氮和硫酸盐对谷氨酸厌氧生物降解性能的抑制及机理[J]. 中国环境科学, 2020, 40(10): 4342-4347.
	CHEN Hong, HU Yingbing, CHEN Chen, et al. Inhibition and process mechanism of ammonia nitrogen and sulfate on anaerobic degradation of glutamate[J]. China Environmental Science, 2020, 40(10): 4342-4347.
34	TUFAIL S, MUNIR Sa, JAMIL N. Variation analysis of bacterial polyhydroxyalkanoates production using saturated and unsaturated hydrocarbons[J]. Brazilian Journal of Microbiology, 2017, 48(4): 629-636.
35	WIDDEL F, G-W KOHRING, MAYER F. Studies on dissimilatory sulfate-reducing bacteria that decompose fatty acids[J]. Archives of Microbiology, 1983, 134(4): 286-294.
36	HAI T, LANGE D, RABUS R, et al. Polyhydroxyalkanoate (PHA) accumulation in sulfate-reducing bacteria and identification of a class III PHA synthase (PhaEC) in Desulfococcus multivorans [J]. Applied and Environmental Microbiology, 2004, 70(8): 4440-4448.
8	JIANG Yongrong, LI Hua, QIN Yongli, et al. Spatial separation and bio-chain cooperation between sulfidogenesis and methanogenesis in an anaerobic baffled reactor with sucrose as the carbon source[J]. International Biodeterioration & Biodegradation, 2019, 138: 99-105.
9	李金娟, 赵林, 谭欣, 等. 利用淀粉酸化废水驯化活性污泥合成聚-β-羟基脂肪酸酯及其表征[J]. 化工进展, 2011, 30(7): 1618-1622.
	LI Jinjuan, ZHAO Lin, TAN Xin, et al. Synthesis and characterization of PHA produced by acclimated activated sludge from acidified starchy wastewater[J]. Chemical Industry and Engineering Progress, 2011, 30(7): 1618-1622.
10	王爱杰, 任南琪, 杜大仲, 等. 硫酸盐还原过程中乙酸型代谢方式的形成及其稳定性[J]. 环境科学, 2004, 25(2): 73-76.
	WANG Aijie, REN Nanqi, DU Dazhong, et al. Formation of an acetic-acid type microbial metabolism pathway and its stability during the course of sulfate-reduction[J]. Environmental Science, 2004, 25(2): 73-76.
11	蒋永荣, 胡明成, 李学军, 等. ABR处理硫酸盐有机废水的相分离特性研究[J]. 环境科学, 2010, 31(7): 1544-1553.
	JIANG Yongrong, HU Mingcheng, LI Xuejun, et al. Phase separation characteristics of an anaerobic baffled reactor treating organic wastewater containing sulphate[J]. Environmental Science, 2010, 31(7): 1544-1553.
12	JIANG Yongrong, QIN Yongli, YU Fangming, et al. Is COD/SO₄ ^2- ratio responsible for metabolic phase-separation shift in anaerobic baffled reactor treating sulfate-laden wastewater?[J]. International Biodeterioration & Biodegradation, 2018, 126: 37-44.
13	王爱杰, 任南琪, 黄志, 等. 产酸脱硫反应器中COD/SO₄ ^2-比制约的群落生态演替规律[J]. 环境科学, 2002, 23(2): 34-38.
	WANG Aijie, REN Nanqi, HUANG Zhi, et al. The ecological succession of climax community restricted by COD/SO₄ ^2- ratio in acidogenic desulfate bioreactor[J]. Chinese Journal of Enviromental Science, 2002, 23(2): 34-38.
14	秦清, 张艳萍. 3种短链脂肪酸对活性污泥储存PHA的影响[J]. 环境工程学报, 2014, 8(7): 2859-2864.
	QIN Qing, ZHANG Yanping. Impact of three short-chain fatty acids on PHA storage by activated sludge[J]. Chinese Journal of Environmental Engineering, 2014, 8(7): 2859-2864.
15	蒋永荣, 刘可慧, 刘成良, 等. 一种硫酸盐有机废水生物处理装置: CN203429023U[P]. 2014-02-12.

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