微生物燃料电池处理含柠檬酸钠废水的研究

doi:10.11949/0438-1157.20190428

摘要/Abstract

摘要：

柠檬酸钠由于其优良的性质被广泛应用于食品、医药、化工等诸多领域，越来越广泛的应用导致工业和市政污水中柠檬酸钠的含量升高，加剧了水体的富营养化。将柠檬酸钠作为微生物燃料电池（microbial fuel cell, MFC）阳极底物，研究得到了柠檬酸钠单独作为混合菌种MFC底物时的产电性能。结果显示，与乙酸钠和葡萄糖相比，以柠檬酸钠为底物的MFC（Na₃C₆H₅O₇-MFC）获得的最大功率密度为742.96 mW·m^-2，是乙酸钠（NaAc-MFC）和葡萄糖（Glu-MFC）的1.77倍和1.12倍。NaAc-MFC和Glu-MFC的启动时间分别约为Na₃C₆H₅O₇-MFC（57 h）的1.8倍和2.9倍。同时，Na₃C₆H₅O₇-MFC对COD的去除率为87.65%，与NaAc-MFC和Glu-MFC相差不大。Na₃C₆H₅O₇-MFC的库仑效率高达61.31%，明显优于NaAc-MFC和Glu-MFC。实验结果表明MFC可以有效地降解柠檬酸钠，能够处理含柠檬酸钠废水，并为柠檬酸钠单独作为底物应用于MFC提供了依据。

关键词: 柠檬酸钠, 微生物, 燃料电池, 降解, 废水

Abstract:

Sodium citrate (Na₃C₆H₅O₇) is widely used for food, medicine, chemical industry and many other fields due to its excellent performance. The extensive application has resulted in an increase of sodium citrate in industrial and municipal sewage and it aggravates the eutrophication of the water body. In this study, sodium citrate is applied as substrate for the anode electricigens and with which microbial fuel cell (MFC) represents good electricity generation performance. The results show that Na₃C₆H₅O₇-MFC achieves a maximum power density of 742.96 mW·m^-2, which is 1.77 and 1.12 times of that of sodium acetate (NaAc-MFC) and glucose (Glu-MFC), respectively. The start-up time of NaAc-MFC and Glu-MFC are about 1.8 and 2.9 times of that of Na₃C₆H₅O₇-MFC (57 h). The Coulombic efficiency of Na₃C₆H₅O₇-MFC is 61.31%, which is obviously superior to NaAc-MFC and Glu-MFC. This indicates that MFC can degrade sodium citrate in wastewater effectively, which provides a possibility of sodium citrate alone as substrate for MFC research.

Key words: sodium citrate, microbial, fuel cell, degradation, wastewater

中图分类号:

TK 6

陈稳稳,刘中良,姜克隽,侯俊先,娄晓歌,李艳霞,廖强,朱恂. 微生物燃料电池处理含柠檬酸钠废水的研究[J]. 化工学报, 2019, 70(S2): 322-328.

Wenwen CHEN,Zhongliang LIU,Kejun JIANG,Junxian HOU,Xiaoge LOU,Yanxia LI,Qiang LIAO,Xun ZHU. Study of wastewater containing sodium citrate degraded by microbial fuel cell[J]. CIESC Journal, 2019, 70(S2): 322-328.

图/表 7

图1 实验组电压曲线

Fig.1 Voltage output of experimental group

图2 重复组电压曲线

Fig.2 Voltage output of repeating group

图3 Na3C6H5O7-MFC、NaAc-MFC和Glu-MFC的极化曲线和功率密度曲线

Fig.3 Polarization curves and power density curves of Na3C6H5O7-MFC, NaAc-MFC and Glu-MFC

图4 Na3C6H5O7-MFC、NaAc-MFC和 Glu-MFC的循环伏安曲线

Fig.4 CVs of Na3C6H5O7-MFC, NaAc-MFC and Glu-MFC

图5 Na3C6H5O7-MFC、NaAc-MFC和Glu-MFC的电化学阻抗谱

Fig.5 EISs of Na3C6H5O7-MFC, NaAc-MFC and Glu-MFC

图6 空白碳布(a)和Na3C6H5O7-MFC (b)、NaAc-MFC (c)、Glu-MFC (d)阳极碳布的SEM图(放大倍数均为×5000)

Fig.6 SEM images of CC (a), anodes of Na3C6H5O7-MFC (b), NaAc-MFC (c) and Glu-MFC (d) under ×5000

表1 三种底物COD去除率和库仑效率

Table 1 COD removal rate and Coulombic efficiency of glucose, NaAc and Na3C6H5O7

MFC	周期持续时间t _b/h	COD₁	COD₂	COD去除率/%	库仑效率/%
Na₃C₆H₅O₇-MFC	约66	590.1	72.89	87.65	61.31
NaAc-MFC	约74	768.8	99.78	87.02	44.7
Glu-MFC	约68	1007.0	107.1	89.36	29.7

参考文献 31

1	Logan B E . Microbial Fuel Cell [M]. Hoboken: John Wiley and Sons, Inc., 2008: 43-56.
2	《2015年中国环境状况公报》公布[J]. 中国环保产业, 2016, (6): 15.
	Environmental aspect bulletin of China in 2015 [J]. China Environmental Protection Industry, 2016, (6): 15.
3	Goh P S , Ismail A F . A review on inorganic membranes for desalination and wastewater treatment [J]. Desalination, 2018, 434: 60-80.
4	Shizas I , Bagley D M . Experimental determination of energy content of unknown organics in municipal wastewater streams [J]. Journal of Energy Engineering, 2004, 130(2): 45-53.
5	周宇, 刘中良, 侯俊先, 等 . 化学氧化改性微生物燃料电池阳极[J]. 化工学报, 2015, 66(3): 1171-1177.
	Zhou Y , Liu Z L , Hou J X , et al . Microbial fuel cell anode modified by chemical oxidation [J]. CIESC Journal, 2015, 66(3): 1171-1177.
6	Tony S , Claude P C . Sodium citrate reduces residual levels of carbohydrates and increases bacterial counts in a fermented mixed vegetables medium [J]. Food Bioscience, 2017, 18: 34-37.
7	Li Y P , Lise A , Haijia S . Combining microwave irradiation with sodium citrate addition improves the pre-treatment on anaerobic digestion of excess sewage sludge [J]. Journal of Environmental Management, 2018, 213: 271-278.
8	高俊彦 . 柠檬酸钠水合物连续结晶过程研究[D]. 天津: 天津大学, 2012.
	Gao J Y . Investigation on continuous crystallization of trisodium citrate hydrates [D]. Tianjin: Tianjin University, 2012.
9	刘柯 . 尿液微生物燃料电池研究[D]. 北京: 中国科学院大学, 2014.
	Liu K . Study on urine microbial fuel cell [D]. Beijing: University of Chinese Academy of Sciences, 2014.
10	Wishart D S , Knox C , Guo A C , et al . HMDB: a knowledgebase for the human metabolome [J]. Nucleic Acids Research, 2009, 37(Database issue): D603-D610.
11	Hou J X , Liu Z L , Yang S Q , et al . Three-dimensional macroporous anodes based on stainless steel fiber felt for high-performance microbial fuel cells [J]. Journal of Power Sources, 2014, 258(3): 204-209.
12	Xu S , Liu H . New exoelectrogen Citrobacter sp. SX-1 isolated from a microbial fuel cell [J]. Journal of Applied Microbiology, 2011, 111(5): 1108-1115.
13	Feng Y J , He L , Wang X , et al . Continuous electricity generation by a graphite granule baffled air-cathode microbial fuel cell [J]. Bioresource Technology, 2010, 101(2): 632-638.
14	Hou J X , Liu Z L , Zhang P Y . A new method for fabrication of graphene/polyaniline nanocomplex modified microbial fuel cell anodes [J]. Journal of Power Sources, 2013, 224(4): 139-144.
15	Abdullah A , Waqar A , Mahad S B , et al . A review of microbial desalination cell technology: configurations, optimization and applications [J]. Journal of Cleaner Production, 2018, 183: 458-480.
16	Edson B E , Jesús H , Liliana G , et al . Domestic wastewater treatment and power generation in continuous flow air-cathode stacked microbial fuel cell: effect of series and parallel configuration [J]. Journal of Environmental Management, 2018, 214: 232-241.
17	Li X , Zhen H . Applications and perspectives of phototrophic microorganisms for electricity generation from organic compounds in microbial fuel cells [J]. Renewable and Sustainable Energy Reviews, 2014, 37: 550-559.
18	Pant D , Bogaert G V , Diels L , et al . A review of the substrates used in microbial fuel cells (MFCs) for sustainable energy production [J]. Bioresource Technology, 2009, 101(6): 1533-1543.
19	Zhang Y , Min B , Huang L , et al . Electricity generation and microbial community response to substrate changes in microbial fuel cell [J]. Bioresource Technology, 2011, 102(2): 1166-1173.
20	Wang A , Sun D , Cao G , et al . Integrated hydrogen production process from cellulose by combining dark fermentation, microbial fuel cells, and a microbial electrolysis cell [J]. Bioresource Technology, 2011, 102(5): 4137-4143.
21	Wang Y , Chen H , Liu Y X , et al . An adsorption-release-biodegradation system for simultaneous biodegradation of phenol and ammonium in phenol-rich wastewater [J]. Bioresource Technology, 2016, 211: 711-719.
22	孙朦朦 . 两株海水异养硝化-好氧反硝化菌的分离、鉴定、培养、硝化性能及脱氮性能研究[D]. 天津: 天津农学院, 2014.
	Sun M M . Isolation, identification and cultivation of two strains of heterotrophic nitrification and aerobic denitrification bacteria and integrated denitrification research [D]. Tianjin: Tianjin Agricultural University, 2014.
23	彭月, 朱能武, 聂红燕 . 一株克雷伯氏菌(Klebsiella sp.)Z6的分离及其产电特性研究[J]. 环境科学学报, 2013, 33(4): 1035-1042.
	Peng Y , Zhu N W , Nie H Y . Isolation of an electrogen Klebsiella sp. Z6 from anodic biofilm and its electricity-generating characteristics [J]. Acta Scientiae Circumstantiae, 2013, 33(4): 1035-1042.
24	Hou J X , Liu Z L , Yang S Q , et al . A comparative study of graphene-coated stainless steel fiber felt and carbon cloth as anodes in MFCs [J]. Bioprocess and Biosystems Engineering, 2015, 38(5): 881-888.
25	李建海 . 海底沉积物微生物燃料电池阳极表面改性及电极构型研究[D]. 青岛: 中国海洋大学, 2010.
	Li J H . Research of anode surface modification and electrode shape in the benthic sediment microbial fuel cell [D]. Qingdao: Ocean University of China, 2010.
26	Fang Z , Song H L , Cang N , et al . Performance of microbial fuel cell coupled constructed wetland system for decolorization of azo dye and bioelectricity generation [J]. Bioresource Technology, 2013, 144: 165-171.
27	Long X Z , Pan Q R , Wang C Q , et al . Microbial fuel cell-photoelectrocatalytic cell combined system for the removal of azo dye wastewater [J]. Bioresource Technology, 2017, 244(1): 182-191.
28	邹立钟 . 微生物燃料电池中产电微生物的电诱导驯化[D]. 徐州: 中国矿业大学, 2015.
	Zou L Z . Study on microorganisms before and after electric induction of domestication in microbial fuel cells [D]. Xuzhou: China University of Mining and Technology, 2015.
29	Kim H J , Park H S , Hyun M S , et al . A mediator-less microbial fuel cell using a metal reducing bacterium, Shewanella putrefaciens [J]. Enzyme & Microbial Technology, 2002, 30(2): 145-152.
30	Renslow R , Babauta J , Dohnalkova A , et al . Metabolic spatial variability in electrode-respiring Geobacter sulfurreducens biofilms [J]. Energy & Environmental Science, 2013, 6: 1827-1836.
31	Papaharalabos G , Greenman J , Melhuish C , et al . A novel small scale microbial fuel cell design for increased electricity generation and waste water treatment [J]. International Journal of Hydrogen Energy, 2015, 40(11): 4263-4268.

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