现代化工

现代化工 ›› 2025, Vol. 45 ›› Issue (10) : 78-83. DOI: 10.16606/j.cnki.issn0253-4320.2025.10.014

技术进展

微生物电化学技术耦合人工湿地工艺减污降碳及影响因素研究

李川 ¹^,^* ,
徐元 ¹ ,
顾勇 ² ,
金新港 ³ ,
许明 ³

作者信息 +

Study on behavior of constructed wetland coupled with microbial electrochemical technology in reducing pollution and carbon dioxide emission as well as its influencing factors

Chuan LI ¹^,^* ,
Yuan XU ¹ ,
Yong GU ² ,
Xin-gang JIN ³ ,
Ming XU ³

Author information +

文章历史 +

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摘要

微生物电化学技术(MET)耦合人工湿地(CW)正成为CW处理污染物的双赢方案,这些携带电活性的CW在近10年来被广泛研究。人工湿地-微生物电化学技术(CW-MET)耦合系统与传统人工湿地相比,CW-MET提升了氮、磷及抗生素等污染物的去除效率,并在低温、低碳氮比等条件下同样实现。CW-MET的CH₄、N₂O和CO₂的排放分别减少了17.9%~36.9%、7.2%~38.7%和5.9%~32.4%。综述了CW-MET的运行原理、减污降碳效果、影响因素和潜在应用等,有助于更深入地了解CW-MET的性能,以期为CW-MET未来的发展和工程化应用提供有利信息。

Abstract

Microbial electrochemical technology (MET) coupled with constructed wetland (CW) is emerging as an effective solution for pollutants treatment.Over the past decade,CW carried with electrical activity has been extensively studied.Compared with traditional constructed wetland,CW-MET coupling system enhances the removal efficiencies of nitrogen,phosphorus,and antibiotics even under low temperature and low carbon-to-nitrogen ratio conditions.Emissions of CH₄,N₂O and CO₂ from CW-MET are reduced by 17.9%-36.9%,7.2%-38.7% and 5.9%-32.4%,respectively.This account reviews CW-MET’s operational principle,effects in reducing pollution and carbon dioxide emission,influencing factors and potential applications,which is helpful to understand the performance of CW-MET and offers valuable insights for the development and engineering application of CW-MET technology in the future.

Graphical abstract

关键词

微生物电化学技术 / 影响因素 / 减污降碳 / 人工湿地

Key words

microbial electrochemical technology / influencing factor / pollution reduction and carbon reduction / constructed wetland

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College of Environment, Hohai University, Nanjing 210098, China), AuthorCompanyExt(id=1241416672088650211, tenantId=1226480274814496768, journalId=1226484258170171394, articleId=1240720151164711409, companyId=1241416672080261601, language=CN, country=null, province=null, city=null, postcode=null, companyName=null, departmentName=null, remark=3.河海大学环境学院, 江苏南京 210098)])])] 李川,徐元,顾勇,金新港,许明. 微生物电化学技术耦合人工湿地工艺减污降碳及影响因素研究[J]. , 2025, 45(10): 78-83 DOI:10.16606/j.cnki.issn0253-4320.2025.10.014

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人工湿地(constructed wetland,CW)具有去污能力强、环境友好、经济可靠等优势^[1],已经发现对许多常规污染物(COD、TN、TP等)和新兴污染物(抗生素、农药等)具有良好的处理效果^[2-3]。微生物电化学技术(microbial eletrochemical technology,MET)是利用电活性微生物在电连接下产生电子转移,从而实现电催化或电合成反应促进物质转化和降解的技术^[4]。基于此开发的人工湿地-微生物电化学(CW-MET)耦合系统,解决了传统人工湿地中缺乏电子供体和电子受体的问题。CW-MET包括人工湿地-微生物燃料电池(CW-MFC)、人工湿地-微生物电解池(CW-MEC)和人工湿地-微生物电化学通气管(CW-MES)等。本文中对CW-MET的系统发展、减污降碳效能及影响因素等进行了概述,并探讨CW-MET的潜在应用前景及挑战。

1 CW-MET的发展和功能

1.1 CW-MFC

Yadav等^[5]首次提出了CW-MFC的概念,采用垂直流MFC-CW处理含亚甲基蓝废水,结果表明耦合系统能够促进染料氧化,并且产生了最大功率密度为15.73 mW/m²的电能。CW-MFC一般由1个阳极室、1个阴极室、1个分隔器和外电路系统组成,反应器的原理见图1(a)。除了传统的单级升流式CW-MFC[图1(b)],CW-MFC的构型还包括下流式[图1(c)]、多电极模式[图1(d)]、串联模式[图1(e)]等。

1.2 CW-MEC

在前人研究基础上,Srivastava等^[6]再次开发了基于微生物电解池(microbial electrolysis cell,MEC)和CW耦合的CW-MEC耦合系统,该耦合系统的NO₃-N去除率达到69.3%,实现了低有机物投放,高NO₃-N去除的效果。CW-MEC[图2(a)]由于外加电压,体系中可以实现热力学上无法自发的反应,包括产生H₂、CH₄和醇等一些有价值的化合物^[7]。CW-MEC比CW-MFC有更多的电极配置选择,包括传统构型[图2(b)]、多个电极[图2(c)、(d)]或多对电极[图2(e)]。当湿地以水平流形式构建时,电极还可以放置在两侧的对称位置。

1.3 CW-MES

CW-MES是基于CW-MFC开发的一种电化学湿地,没有外部电路形成闭合回路,而是直接将导电材料植入人工湿地[图3(a)]。CW-MES系统有2种基本方式,一是导电材料形成的电极组件[图3(b)],二是全部由导电基质构成的人工湿地[图3(c)]。由于这种构成,CW-MES无法收集电流,而是仅用于污染物的去除,但体系中可以形成更大面积的电活性生物群,并且电子可以在导电材料中快捷传递,因此处理效果较优于一般带外电路的CW-MET。由于CW-MES构造简单,依赖生物电化学原理来优化CW工艺,能最大限度地消耗底物,促使污染物的高效去除,并减少生物质积累和甲烷的生成,具有在短时间内形成大规模应用的可能。

2 CW-MET减污降碳效果

如图4所示,生物电化学技术耦合人工湿地领域的国内外文献显示,CW-MFC、脱氮、电化学、抗生素抗性基因等为当前的研究热点。以下对近年来CW-MET处理常规污染物、新兴污染物、温室气体减排效果及脱氮机理进行分析。

2.1 常规污染物

CW-MET系统对常规污染物的去除率要高于传统人工湿地,并在低温、低碳氮比等条件下同样实现。Ji等^[8]的研究发现,与开路CW-MFC系统(相当于传统人工湿地)相比,闭路CW-MFC系统的氨氮去除率提高了26.83%,闭路系统有利于硝化菌和反硝化菌的富集,提高脱氮效果。Wang等^[9]在CW-MES的导电层中敷设不锈钢管网,添加缓释氧基质和铁棒,考察了系统在低温条件下的处理效能,结果表明,相比不添加缓释氧基质组,COD、NH₃-N、TP去除率分别提高了1.52、2.97、3.95倍,而相比不添加铁棒组,分别提高了2.21、1.68、1.76倍。

2.2 新兴污染物

目前CW-MET已被用于通过底物吸收、微生物群落利用及共代谢途径等去除新兴污染物。Xu等^[10]针对CW-MFC体系中磺胺嘧啶(SDZ)和盐酸环丙沙星(CIP)的去除研究发现,SDZ的浓度从 2 mg/L下降到0.064 mg/L,达到了96.79%的去除率;而CIP的去除率也达到了98.64%,同时产生了5.34 mW/m²的功率密度,电池的平均输出电压达到了520 mV,证明了抗生素在CW-MFC中实现降解和能量回收的可行性^[11]。

2.3 温室气体减排效果

控制温室气体排放是人工湿地应用领域的关键,而CW-MET耦合系统可有效减少温室气体的排放。与传统人工湿地相比,CW-MET减少了17.9%~36.9%的CH₄、7.2~38.7%的N₂O和5.9%~32.4%的CO₂。CW-MET中温室气体的减排与基因的丰度密切相关,CH₄的生成包括甲烷生成(mcrA)和甲烷氧化(pmoA)基因的参与;N₂O是硝化和反硝化的副产物,排放以nosZ、nirS、amoA和nirK等基因为主。然而,针对CW-MET的温室气体排放情况仍然欠缺全面的研究。Li等^[12]认为,CW-MFC中温室气体排放通量的减少主要有3个因素:电化学活性细菌与产甲烷菌之间的底物竞争增强,异化金属还原细菌与产甲烷菌之间的底物竞争效应,以及湿地内存在金属驱动的厌氧甲烷氧化。

2.4 CW-MET的脱氮机理

CW-MFC反硝化原理是基于传统的生物反硝化原理发展起来的,主要包括直接反硝化、硝化、反硝化、同步硝化反硝化和厌氧氨氧化作用等方面^[13]。CW-MFC中氮的最终去除取决于硝酸盐向氮气或氮氧化物的转化,脱氮机理见图5。CW-MEC的反硝化原理与CW-MFC基本一致,但两者的电子来源不同,脱氮机理见图6。CW-MEC通过外部电源提供电子,而CW-MFC只能通过微生物消耗有机物来提供电子。CW-MEC可以在较低的C/N条件下,通过外部电源来补充反硝化作用所需的大量电子^[14]。CW-MEC与仅以有机物为电子源的生物反硝化作用相比,电解作用增强了反硝化在CW-MEC系统中的优势,提高了脱氮效率。CW-MES是一种短路的CW-MFC,其生物阳极进行有机物氧化反应释放电子,产生的电子可以自由流向水中的生物阴极,在阴极中硝酸根、亚硝酸根可被进一步还原^[15],脱氮机理见图7。在CW-MES系统中支持异化硝酸盐还原的微生物可能在该系统产生N₂O中发挥关键作用。

3 CW-MET的影响因素

在实际操作中CW-MET还会受到许多因素制约,如运行条件对系统性能的影响。未来的研究应尽可能地发掘CW-MET系统对减污降碳影响的潜在因素,以确定这些因素的重要性排序。表1展示了近年来针对CW-MET减污降碳研究中的系统配置参数情况,对各重要参数的影响进行了分析。

3.1 电极材料和构型

电极材料是影响电气性能的首要因素。许多具有良好生物相容性、较高比表面积和孔隙率的电极材料,如碳毡、活性炭、石墨等,被用作CW-MET的电极材料。在一些研究中,诸如铂、镍、钛、不锈钢和铜等金属材料被嵌入电极,实现了良好的电气性能^[21]。调整电极构型包括电极间距、电极分隔膜、电极位置等。CW-MEC需要通过外加电源提高阴、阳极之间的电位差,因此CW-MET中的电极间距通常在10~20 cm,甚至几乎直接接触^[22],这将带来电极分隔膜的问题。Xu等^[23]发现未设置分隔膜的系统比设置分隔膜的系统产电提高了143 mV,功率密度提高了49.08 mW/m²,无分隔膜系统将是未来的优选。电极位置会直接影响两极板之间的氧化还原梯度,从而影响污染物去除性能。绝大多数研究中,阴极被设置在湿地表面,而阳极根据一定的间距进行设置。未来,需要更多的研究以确定在其他CW-MET系统中不同电极位置配置对各种污染物去除效能的影响。

3.2 水力停留时间

水力停留时间(HRT)是反应器运行的重要参数。目前,大部分关于CW-MET的研究中,HRT为1~3 d,与我国人工湿地污水处理工程技术规范(HJ 2005—2010)相同,少部分研究了短于或长于这个HRT的时间。通过引入MET,CW-MET所需的HRT可以短于传统的人工湿地,从而实现更高的经济价值。但在处理某些难降解污染物时需要考虑HRT的延长。尽管CW-MET在理论上可以实现难降解污染物的有效去除,仍然需要针对特定污染物研究其合理的HRT选择,以扩大CW-MET系统HRT的普适性。

3.3 植物和基质的选择

植物和基质是人工湿地系统配置的关键组成。Zhang等^[18]研究发现,以锰砂为基质的CW-MEC实现了最高的COD和氮磷去除率,COD、NH₃-N、NO₃-N、TN、TP去除率分别为79.42%、94.60%、95.53%、94.82%、80.86%。CW-MET也需要评估植物在电场氛围下受到的影响,甚至筛选出利于CW-MFC产电的植物品种。Xiao等^[24]发现当外加电压达到5 V时,芦竹已经不能通过自我调节适应电压,并出现枯萎症状。一般CW-MEC外加电压低于0.8 V,但仍然需要评估在有限电压范围内植物可能受到的积极或消极影响。

4 CW-MET的潜在应用及挑战

4.1 强化难降解污染物去除

传统人工湿地通常依赖于进水或基质中的电子供体和受体,这极大地限制了人工湿地对难降解污染物的去除。引入微生物电化学系统后,电子受体和电子供体的供应问题被有效解决。一些研究证实了难降解污染物在CW-MET中被有效去除,然而,还需要进一步研究CW-MET工艺中难生物降解化合物的迁移和转化途径,如药品和个人护理产品、抗生素抗性基因,甚至微塑料等^[25]。由于CW-MET的表现可能因污染物类型和浓度而变化,因此迫切需要研究其他难降解污染物的可处理性和对CW-MET系统的影响。

4.2 增值产物的产生与运用

CW-MFC可以同步实现污染物去除和产电。然而,与常规MFC不同的是,CW-MFC中的电极通常只占基质中的一小部分,大部分的电子在降解污染物中流失,导致CW-MFC库仑效率(低于10%)和产能(低于50 mW/m²)普遍低下^[26]。可以通过构建CW-MFC和CW-MEC串联耦合系统,实现生物电的原位利用,同时进一步提高处理效率。

4.3 生物传感器

生物传感器对处理水体的监测和调控具有重大的生态意义。目前CW-MFC产生的生物电远不能满足商用标准,但潜在的间接利用价值是值得探索的。最重要的是,这种生物传感器只需要简单的电信号编译,而无需用任何其他复杂的设备。这样的生物传感器既可以作用在普通水质的精确变化测量上,也可以用在毒性物质的预警评估上。

5 结论与展望

CW-MFC在提升净化效果的同时可进行产电,而CW-MEC、CW-MES与CW-MFC不同,它们不以收集能量为目标,而是依赖微生物电化学原理来优化CW工艺,但目前CW-MET的工程化应用仍然存在瓶颈。相比于传统人工湿地,CW-MET的主要成本在于电极材料或导电填料。然而扩大性建设使得系统结构复杂性变得难以预测,原理的普适性需要扩大研究。未来的研究应该集中在新材料的研究和开发、系统的内部条件、接种物和系统的配置,以及增加对这些系统中电子释放、转移和使用的不同过程的理解,以期提升CW-MET耦合系统的减污降碳效果。

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