藻炭改性电极强化微生物燃料电池产电及去除硝基苯性能

徐戴非; 吴兵党; 杨晶晶; 沈正栋; 黄天寅

doi:10.12153/j.issn.1674-991X.20230092

藻炭改性电极强化微生物燃料电池产电及去除硝基苯性能

doi: 10.12153/j.issn.1674-991X.20230092

徐戴非^{1, 2,},
吴兵党^{1, 2},
杨晶晶^{1, 2},
沈正栋^{1, 2},
黄天寅^{1, 2, ,}

1.
苏州科技大学环境科学与工程学院
2.
苏州市海绵城市技术重点实验室

基金项目: 国家自然科学基金面上项目（52070137）；苏州市社会发展科技创新项目(SS202107)；苏州市姑苏创新创业领军人才计划项目（ZXL2022500）

详细信息

作者简介:
徐戴非(1998—)，男，硕士研究生，主要从事水污染控制研究，a1013699818@163.com

通讯作者:
黄天寅(1975—)，男，教授，主要从事水环境治理与水生态修复研究，huangtianyin111@163.com

中图分类号: X703
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- 被引次数: 0
出版历程
- 收稿日期: 2023-02-07
- 网络出版日期: 2023-11-24

Removal efficiency of nitrobenzene and electricity generation by microbial fuel cell with algal biochar modified electrode

XU Daifei^{1, 2
,},
WU Bingdang^{1, 2},
YANG Jingjing^{1, 2},
SHEN Zhengdong^{1, 2},
HUANG Tianyin^{1, 2
, ,}

1.
School of Environmental Science and Engineering, Suzhou University of Science and Technology
2.
Key Laboratory of Suzhou Sponge City Technology

摘要

摘要:
开发利于微生物富集和优异导电性能的电极是提高微生物燃料电池（MFC）性能的关键。通过碱活化和酸活化方式制备螺旋藻生物炭（简称藻炭）并将其修饰于阳极炭毡（CF），以硝基苯为难降解污染物代表，通过检测电极电化学性能和污染物降解过程，探究基于藻碳MFC产电及转化污染物的性能。结果表明：在700 ℃-NaOH改性藻炭修饰炭毡的电极体系（NaOH-AC700/CF），MFC电压最高可达670 mV，比CF体系高26%，且驯化时间由7 d缩短至2 d。修饰电极体系产电的同时高效降解污染物，阴极对硝基苯的去除率最高可达99.9%；相比于CF体系，NaOH-AC700/CF体系的降解效率提高了22.1%，苯胺生成率提高了123.3%。微生物种类分析结果表明，电极表面的产电菌主要为弧形杆菌属（Arcobacter）和铜绿假单胞菌属（Pseudomonas），且在NaOH-AC700/CF阳极表面产电菌丰度最高，因而利于MFC产电以及硝基苯的还原。
- 微生物燃料电池（MFC） /
- 藻炭 /
- 改性电极 /
- 硝基苯 /
- 弧形杆菌属
Abstract:
Development of electrodes that facilitate microbial enrichment and excellent electrical conductivity is the key to improving the performance of microbial fuel cell (MFC). By acid and base activation way, the anode carbon felt (CF) with spirulina biochar (one type of algal biochar) was modified. The performance of MFC based on modified electrodes for electricity generation and pollutant conversion was explored with nitrobenzene as a representative of refractory pollutants, by detecting the electrochemical performance of the electrode and the pollutant degradation process. The results showed that the maximum MFC voltage in the modified CF electrode system (NaOH-AC700, 700 ℃ and modified by NaOH) could reach up to 670 mV, which was 26% higher than CF system, and the acclimation time was reduced from 7 days to 2 days. The modified electrode system could efficiently generate electricity while also degrading pollutants. The removal of nitrobenzene by the cathode in the modified CF electrode system was 99.9%, which was 22.1% higher than the unmodified CF electrode system, and the aniline production was increased by 123.3%. Microbial community analysis showed that the electrogenic microorganisms on the electrode surface were mainly Arcobacter and Pseudomonas, and the highest abundance of electrogenic microorganisms was found on the surface of NaOH-AC700/CF anode, thus facilitating the electrogenesis of MFC and the reduction of nitrobenzene.
- microbial fuel cell (MFC) /
- algal biochar /
- modified electrode /
- nitrobenzene /
- Arcobacter

HTML全文

图 1 MFC反应器原理

Figure 1. MFC reactor schematic diagram

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图 2 MFC反应器装置

Figure 2. Device diagram of MFC reactor

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图 3 藻炭材料SEM图

Figure 3. SEM diagram of algal biochar

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图 4 MFC阳极表面微生物附着情况SEM图

Figure 4. SEM diagram of microorganism adhesion on MFC anode surface

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图 5 藻炭修饰电极CV曲线

注：电势为测试电极与Ag/AgCl电极间的电位差。

Figure 5. CV diagram of algal biochar modified electrodes

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图 6 不同藻炭修饰阳极MFC驯化阶段和稳定阶段的电压输出

Figure 6. Voltage output of MFC with different algal biochar modified anodes at acclimation stage and stabilization stage

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图 7 不同藻炭修饰阳极MFC功率密度曲线与极化曲线

Figure 7. MFC power density curve and polarization curve of different algal biochar modified anodes

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图 8 不同阳极MFC体系硝基苯降解、产物生成及电压变化

Figure 8. Nitrobenzene degradation, product formation and voltage variation in different anode MFC systems

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图 9 不同初始pH条件下硝基苯降解和产物生成变化

Figure 9. Nitrobenzene degradation and product formation changes at various initial pH

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图 10 各条件下反应终点产物占比

Figure 10. Proportion of end products under various conditions

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图 11 硝基苯阴极还原降解路径

Figure 11. Cathodic reduction degradation pathway of nitrobenzene

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图 12 藻炭修饰阳极微生物驯化前后属水平下菌群相对丰度（排名前20）

Figure 12. Relative abundance of bacteria at genus level before and after acclimation of algal biochar modified anodes （top 20 genus）

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表 1 不同电极的MFC反应器名称

Table 1. MFC reactor with different electrodes

编号	阳极	阴极	反应器名称
1	CF	泡沫镍	CF- MFC
2	BC700/CF	泡沫镍	BC700/CF-MFC
3	HCl-AC700/CF	泡沫镍	HCl-AC700/CF-MFC
4	NaOH-AC700/CF	泡沫镍	NaOH-AC700/CF-MFC

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表 2 不同类型藻炭比表面积

Table 2. Specific surface area of different types of algal biochar

藻炭活化方式及名称		比表面积/(m²/g)
未活化	BC500	0.846 6
未活化	BC700	0.762 0
酸活化	HCl-AC500	0.481 3
酸活化	HCl-AC700	0.158 3
碱活化	NaOH-AC500	46.726 4
碱活化	NaOH-AC700	664.203 4

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表 3 生物种群Alpha多样性分析

Table 3. Alpha diversity analysis of biological population

样品	Ace 指数	Chao1 指数	Shannon 指数	Simpson 指数	覆盖率
接种污泥	148.794	146.5	5.14	0.938	1
CF	139.000	139	5.819	0.969	1
BC700/CF	133.237	138.5	4.863	0.925	1
HCl-AC700/CF	137.743	138	3.822	0.835	1
NaOH-AC700/CF	129.693	129	2.553	0.559	1

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参考文献(44)

[1]	XU P, XU H, SHI Z. A novel bio-electro-Fenton process with FeVO₄/CF cathode on advanced treatment of coal gasification wastewater[J]. Separation and Purification Technology,2018,194:457-461. doi: 10.1016/j.seppur.2017.11.073
[2]	BOND D R, LOVLEY D R. Electricity production by Geobacter sulfurreducens attached to electrodes[J]. Applied and Environmental Microbiology,2003,69(3):1548-1555. doi: 10.1128/AEM.69.3.1548-1555.2003
[3]	MODESTRA J A, CHIRANJEEVI P, MOHAN S V. Cathodic material effect on electron acceptance towards bioelectricity generation and wastewater treatment[J]. Renewable Energy,2016,98:178-187. doi: 10.1016/j.renene.2016.03.066
[4]	CHAKRABORTY I, SATHE S M, DUBEY B K, et al. Waste-derived biochar: applications and future perspective in microbial fuel cells[J]. Bioresource Technology,2020,312:123587. doi: 10.1016/j.biortech.2020.123587
[5]	BOND D R, HOLMES D E, TENDER L M, et al. Electrode-reducing microorganisms that harvest energy from marine sediments[J]. Science,2002,295(5554):483-485. doi: 10.1126/science.1066771
[6]	WU Y N, WANG L, JIN M, et al. Simultaneous copper removal and electricity production and microbial community in microbial fuel cells with different cathode catalysts[J]. Bioresource Technology,2020,305:123166. doi: 10.1016/j.biortech.2020.123166
[7]	OON Y S, ONG S A, HO L N, et al. Microbial fuel cell operation using monoazo and diazo dyes as terminal electron acceptor for simultaneous decolourisation and bioelectricity generation[J]. Journal of Hazardous Materials,2017,325:170-177. doi: 10.1016/j.jhazmat.2016.11.074
[8]	PUIG S, SERRA M, VILAR-SANZ A, et al. Autotrophic nitrite removal in the cathode of microbial fuel cells[J]. Bioresource Technology,2011,102(6):4462-4467. doi: 10.1016/j.biortech.2010.12.100
[9]	LOGAN B E. Scaling up microbial fuel cells and other bioelectrochemical systems[J]. Applied Microbiology and Biotechnology,2010,85(6):1665-1671. doi: 10.1007/s00253-009-2378-9
[10]	李朝明, 许丹, 黄铭意, 等.不同阳极设置对人工湿地-微生物燃料电池脱氮及产能的影响[J]. 环境工程技术学报,2023,13(1):205-213. LI C M, XU D, HUANG M Y, et al. Effects of different anode settings on the performance of nitrogen removal and electrogenesis capacity in constructed wetland-microbial fuel cells[J]. Journal of Environmental Engineering Technology,2023,13(1):205-213.
[11]	ALI YAQOOB A, IBRAHIM M N M, RODRÍGUEZ-COUTO S. Development and modification of materials to build cost-effective anodes for microbial fuel cells (MFCs): an overview[J]. Biochemical Engineering Journal,2020,164:107779. doi: 10.1016/j.bej.2020.107779
[12]	KIM M, KIM H W, NAM J Y, et al. Recent progress of nanostructure modified anodes in microbial fuel cells[J]. Journal of Nanoscience and Nanotechnology,2015,15(9):6891-6899. doi: 10.1166/jnn.2015.10723
[13]	CAI T, MENG L J, CHEN G, et al. Application of advanced anodes in microbial fuel cells for power generation: a review[J]. Chemosphere,2020,248:125985. doi: 10.1016/j.chemosphere.2020.125985
[14]	HOJJATI-NAJAFABADI A, DAVAR F, ENTESHARI Z, et al. Antibacterial and photocatalytic behaviour of green synthesis of Zn_0.95Ag_0.05O nanoparticles using herbal medicine extract[J]. Ceramics International,2021,47(22):31617-31624. doi: 10.1016/j.ceramint.2021.08.042
[15]	GURAV R, BHATIA S K, CHOI T R, et al. Adsorptive removal of crude petroleum oil from water using floating pinewood biochar decorated with coconut oil-derived fatty acids[J]. Science of the Total Environment,2021,781:146636. doi: 10.1016/j.scitotenv.2021.146636
[16]	熊江磊, 罗嘉豪, 严群.改性蓝藻生物炭促进生物电化学系统阴极氢自养反硝化过程研究[J]. 环境工程技术学报,2022,12(5):1640-1646. XIONG J L, LUO J H, YAN Q. Research on modified cyanobacterial biochar promoting cathodic hydrogen autotrophic denitrification in bioelectrochemical system[J]. Journal of Environmental Engineering Technology,2022,12(5):1640-1646.
[17]	李怡冰, 李涵, 黄文轩, 等.生物炭的制备及其在强化电子传递和催化性能等方面的研究进展[J]. 环境科学研究,2021,34(5):1157-1167. LI Y B, LI H, HUANG W X, et al. Research progress on the biochar production and its applications in enhancing electron transport and catalysis performance[J]. Research of Environmental Sciences,2021,34(5):1157-1167.
[18]	WANG B W, WANG Z F, JIANG Y, et al. Enhanced power generation and wastewater treatment in sustainable biochar electrodes based bioelectrochemical system[J]. Bioresource Technology,2017,241:841-848. doi: 10.1016/j.biortech.2017.05.155
[19]	LAN L H, LI J, FENG Q, et al. Enhanced current production of the anode modified by microalgae derived nitrogen-rich biocarbon for microbial fuel cells[J]. International Journal of Hydrogen Energy,2020,45(6):3833-3839. doi: 10.1016/j.ijhydene.2019.06.199
[20]	LIN Y Z, YIN J, WANG J H, et al. Performance and microbial community in hybrid anaerobic baffled reactor-constructed wetland for nitrobenzene wastewater[J]. Bioresource Technology,2012,118:128-135. doi: 10.1016/j.biortech.2012.05.056
[21]	DONG X Q, ZHANG Y N, XU Y W, et al. Catalytic mechanism study on manganese oxide in the catalytic supercritical water oxidation of nitrobenzene[J]. RSC Advances,2015,5(59):47488-47497. doi: 10.1039/C5RA04322K
[22]	KUŞÇU Ö S, SPONZA D T. Effect of increasing nitrobenzene loading rates on the performance of anaerobic migrating blanket reactor and sequential anaerobic migrating blanket reactor/completely stirred tank reactor system[J]. Journal of Hazardous Materials,2009,168(1):390-399. doi: 10.1016/j.jhazmat.2009.02.060
[23]	WEI W, SUN R, JIN Z, et al. Hydroxyapatite-gelatin nanocomposite as a novel adsorbent for nitrobenzene removal from aqueous solution[J]. Applied Surface Science,2014,292:1020-1029. doi: 10.1016/j.apsusc.2013.12.127
[24]	夏甫, 杨昱, 万朔阳, 等.预处理方式对氧化-还原联合技术修复硝基苯污染地下水的影响[J]. 环境科学研究,2020,33(9):2001-2010. XIA F, YANG Y, WAN S Y, et al. Influence of pre-treatment on remediation of nitrobenzene contaminated groundwater by combined oxidation-reduction techniques[J]. Research of Environmental Sciences,2020,33(9):2001-2010.
[25]	ZHANG W, CHEN L, CHEN H, et al. The effect of Fe⁰/Fe²⁺/Fe³⁺ on nitrobenzene degradation in the anaerobic sludge[J]. Journal of Hazardous Materials,2007,143(1/2):57-64.
[26]	LU Y, XIE Q Q, TANG L, et al. The reduction of nitrobenzene by extracellular electron transfer facilitated by Fe-bearing biochar derived from sewage sludge[J]. Journal of Hazardous Materials,2021,403:123682. doi: 10.1016/j.jhazmat.2020.123682
[27]	刘荣华. 微生物燃料电池中污染物的强化降解[D]. 合肥: 中国科学技术大学, 2014.
[28]	侯俊先. 微生物燃料电池阳极改性及生物膜内部传递现象的研究[D]. 北京: 北京工业大学, 2018.
[29]	刘昊佳. 基于二维层状电极的高性能微生物燃料电池[D]. 南京: 东南大学, 2020.
[30]	LIU G L, YATES M D, CHENG S A, et al. Examination of microbial fuel cell start-up times with domestic wastewater and additional amendments[J]. Bioresource Technology,2011,102(15):7301-7306. doi: 10.1016/j.biortech.2011.04.087
[31]	彭本齐. 基于纳米硅藻材料的MFC阳极制备及性能研究[D]. 哈尔滨: 哈尔滨工业大学, 2019.
[32]	HUGGINS T, WANG H M, KEARNS J, et al. Biochar as a sustainable electrode material for electricity production in microbial fuel cells[J]. Bioresource Technology,2014,157:114-119. doi: 10.1016/j.biortech.2014.01.058
[33]	程浩毅. 生物电化学系统定向还原硝基苯及能量循环补偿模式研究[D]. 哈尔滨: 哈尔滨工业大学, 2013.
[34]	HARWOOD W H, HURD R M, JORDAN W H Jr. Electrochemical reduction of nitrobenzene at controlled potentials[J]. Industrial & Engineering Chemistry Process Design and Development,1963,2(1):72-77.
[35]	李婉君. 藻/菌微生物燃料电池pH自中和、降解偶氮染料与产电研究[D]. 广州: 华南理工大学, 2014.
[36]	徐文英, 樊金红, 高廷耀.硝基苯类物质在铜电极上的电还原特性及pH的影响[J]. 环境科学,2005,26(2):102-107. XU W Y, FAN J H, GAO T Y. Electrochemical reduction characteristics of nitro-benzene compounds at the copper electrode and the influence of pH on reduction[J]. Environmental Science,2005,26(2):102-107.
[37]	黄子安, 李陵岚, 刘辉.氧化偶氮苯类化合物合成研究进展[J]. 化学试剂,2020,42(11):1318-1326. HUANG Z A, LI L L, LIU H. Progress in the synthesis of azoxybenzene compound[J]. Chemical Reagents,2020,42(11):1318-1326.
[38]	JIN M, LIU Y Y, ZHANG X, et al. Selective electrocatalytic hydrogenation of nitrobenzene over copper-platinum alloying catalysts: experimental and theoretical studies[J]. Applied Catalysis B:Environmental,2021,298:120545. doi: 10.1016/j.apcatb.2021.120545
[39]	庞绍婕. 改性电极微生物燃料电池处理硝基苯废水的性能研究[D]. 太原: 太原理工大学, 2021.
[40]	MU Y, ROZENDAL R A, RABAEY K, et al. Nitrobenzene removal in bioelectrochemical systems[J]. Environmental Science & Technology,2009,43(22):8690-8695.
[41]	YATES M D, KIELY P D, CALL D F, et al. Convergent development of anodic bacterial communities in microbial fuel cells[J]. The ISME Journal,2012,6(11):2002-2013. doi: 10.1038/ismej.2012.42
[42]	杨思霞, 邵琼丽, 许坤德, 等.电化学参数影响下微生物电解池阳极膜上电活性微生物群落的变化[J]. 化学研究与应用,2022,34(3):549-557. YANG S X, SHAO Q L, XU K D, et al. Community evolution of exoelectrogens on anodic biofilm in microbial electrolysis cells: influence of electrochemical parameters[J]. Chemical Research and Application,2022,34(3):549-557.
[43]	高崇洋, 吴唯民, 王爱杰, 等.平行启动的微生物燃料电池阳极微生物群落差异性解析[J]. 哈尔滨工业大学学报,2016,48(2):15-20. GAO C Y, WU W M, WANG A J, et al. Comparison of anodic microbial communities in parallel-operated microbial fuel cells[J]. Journal of Harbin Institute of Technology,2016,48(2):15-20.
[44]	谢丽, 马玉龙.微生物燃料电池中产电微生物的研究进展[J]. 宁夏农林科技,2011,52(7):104-107. XIE L, MA Y L. Progress in research of electricigens in microbial fuel cell[J]. Ningxia Journal of Agriculture and Forestry Science and Technology,2011,52(7):104-107. ⊗