杨珍珍(1992-), 女, 河南洛阳人, 硕士, 主要从事废水和土壤的电化学修复。E-mail:
综述了有机污染土壤的电动力修复和微生物电化学修复的最新研究进展。分析了电动力修复中电极材料、运行条件等因素对污染物去除效果的影响,总结了添加表面活性剂、引入具有降解能力的基质、与化学或生物联合等方式对土壤修复效果的强化作用,阐述了微生物电化学修复的效果、影响因素和微生物群落演变的规律。电化学技术能够有效去除土壤中的有机污染物,且电动力较微生物电化学具有更好的去除效果。为了实现电化学技术在污染土壤修复中的应用,未来需要从土壤导电性、电极材料以及反应器构型等方面优化以提高修复效果;此外,电化学修复技术的机理、功能微生物的群落特征研究等也是下一步研究的重点。
The serious situation of soil pollution is now threatening the safety of agricultural products, human health and ecological environment, even though, increasing attention has been paid to remediation of soils polluted with organic chemicals in recent decades. The organic chemicals commonly found in the soil include mainly pesticides, petroleum hydrocarbons, antibiotics and so on. As an effective in-situ remediation technology, the technology of electrochemical remediation can be used to remediate organic chemical polluted soils without disturbing their ecological environments. In this paper a review is presented on recent advances in the research on use of electrochemical technologies to remediate polluted soils, including electrokinetic and microbial electrochemical system. Effects of electrode materials, operation conditions and electrode arrangement on pollutant removal efficiency in the process of electrokinetic remediation are analyzed. A conclusion has been reached that both the technologies of electrokinetic and microbial electrochemical remediations can be used to remediate organic chemical-polluted soils, when used in combination with certain facilitating agents, such as surfactants, co-solvents, nanoparticles, and oxidizing chemicals, or with in-situchemical oxidation, bioremediation and phytoremediation, all of which show a synergistic effect on the removal or elimination of organic chemical contaminants in soil. Especially, relationships between variation of the soil microbial communities in the process of soil remediation and removal of pollutants in the process of microbial electrochemical remediation are discussed. Generally speaking, both electrokinetic remediation and microbial electrochemical remediation show good effects of removing organic pollutants from soils, and the former is better than the latter. All the experiments so far carried out show that the adoption of binary metallic oxidation electrodes, nanoparticles modified carbon felt electrode and that optimized electrode arrangement and reactor configuration can improve the pollutant removal efficiency, and the optimization of applied voltage, electrolyte type, operation time, external and internal resistance, electrode area and interval between electrodes can also significantly improve the electrochemical remediation efficacy. Compared with deionized water, Na2SO4, citric acid and NaOH, the NaCl and KH2PO4 are preferable electrolyte during the electrokinetic remediation. Organic pollutants removal efficiency increases with decreasing internal resistance and external resistance. Addition of biochar, carbon fiber, graphene oxide and sand can increase the soil conductivity and mass transport capacity. And microbial electro-remediating cells without external resistance is one of the hot spots in future researches on electrochemical technologies. With the decreased electrode interval, both electricity generation and removal of organic pollutants increase. Microbial community analysis shows that the microorganisms at the anode decrease in diversity and increase in homogeneity in the process of the microbial electrochemical system removing organic pollutants from soil. The exoelectrogens play an important role in the anode cell, while degrading bacteria are effective in the soil near the cathode and anode. In addition, the coupling of electrochemical remediation with chemical oxidation, phytoremediation and bioremediation may make it possible to extrapolate the technology of electrochemistry on a large scale. In order to realize the practical application of the technology to remediation of organic-chemical polluted soils, it is necessary to improve the electrochemical remediation technology by optimizing configuration of the reactor, soil conductivity and electrode materials in the future. Moreover, it is anticipated that mechanisms of the electrochemical remediation technology and characteristics of the functional microbial community relative to type of organic pollutants will be one of the hot spots in the research on microbial electrochemical remediation.
土壤是人类赖以生存的基础。土壤有机污染物主要包括有机农药、石油烃类、塑料制品、染料、表面活性剂、增塑剂、阻燃剂以及抗生素等。其中一些农药和化工产品属于对人类健康危害较大的持久性有机污染物。它们具有毒性高、难降解等特点,不仅可在植物体中积累,还可通过食物链富集至动物和人体中,对人畜健康和生态安全产生不利影响[
电化学修复作为一种既不破坏生态环境又能修复土壤污染的原位修复技术,对于低渗透性土壤也具有较好的修复效果,是近年来土壤污染修复的热点方向之一。其主要包括电动力(electrokinetic,简称EK)修复和微生物电化学(microbial electrochemical system,简称MES)修复,其中以EK为主的研究较多。目前应用电化学技术修复土壤中重金属污染已有较多的研究报道,但以去除土壤中有机物为目标的相对较少。本文对用EK、MES及其强化联合等电化学技术修复有机污染土壤的研究进行综述,以期为后续相关研究提供参考。
土壤的EK修复是指利用电场驱动污染物在土壤中移动和转移,将污染物转运至阴极、阳极或某一特定位置,随后进一步处理的技术。转运的主要作用包括电迁移、电渗析、电泳[
电动力修复原理图
Schematic diagram of electrokinetic remediation
其中,电迁移是指带电离子在电场的作用下阳离子向阴极迁移,阴离子向阳极迁移;电渗析是指土壤颗粒表面的负电荷与孔隙水中的离子形成双电层,扩散双电层使得孔隙水由阳极向阴极移动的现象;电泳是指土壤中带电的胶体粒子(细小土壤颗粒、腐殖质和微生物细胞等)在电场作用下发生迁移。除了电动力过程,在电极表面也发生着水电解过程,电解反应的进行会使得阳极的pH降低,阴极的pH升高[
电极材料是影响电动力过程最重要的参数。常用的电极材料有石墨、碳毡、金属以及金属氧化物电极,其中石墨以价格低廉、导电性良好且不需要复杂的处理,在EK修复中广泛使用。Carboneras等[
电动力修复示意图(a)传统的电极排布;b)多电极对排排布[
Diagram of the electrokinetic remediation(a)typical electrodes, b)linear rows of electrodes[
电场强度、处理时间、电解液类型以及土壤的pH等运行条件对有机污染物的去除也有很大影响。Yuan等[
EK修复中由于电解水的发生会出现一系列的附加现象,例如,EK运输过程导致土壤养分流失、电极附近pH变化大,这些过程会对土壤中的生物修复过程造成很大影响,因此需要对反应系统的pH进行调节。由于极性反转(即电场作用于土壤的极性周期性地变化)可控制污染物的迁移方向而且不会增加额外的费用,是调节pH变化和改善土壤营养物分布的简单方法[
对于不能溶解于孔隙水中的污染物,可通过表面活性剂或助剂提高其溶解度从而实现有效去除。在土壤修复中常用的是离子和非离子表面活性剂,非离子表面活性剂例如吐温80、Brij 35和聚乙二醇辛基苯基醚(TritonX-100)等通过电渗析作用进入土壤介质;阴离子表面活性剂需要加入阴极电解液中通过电迁移方式输送至土壤中;阳离子表面活性剂与土壤颗粒的相互作用,限制了其活性,因此不能使用[
引入具有降解或分解能力的基质使污染物原位分解,是对电动力修复技术的强化措施之一。报道较多的是引入零价纳米铁(nZVI)和可渗透反应格栅(permeable reactive barrier,简称PRB)。纳米材料的出现为土壤中污染物的修复提供了新的可能,与其他纳米材料相比,nZVI因无毒、廉价易于生产受到广泛关注。nZVI由于其纳米尺寸对污染物具有更高的反应活性,是一种很有前途的土壤修复技术[
EK与化学修复的结合对低渗透性土壤中的污染物具有较好的去除效果,解决了化学修复技术在低渗透性土壤中处理效果较差的缺点。其中化学技术主要包括化学淋洗、芬顿和过硫酸盐氧化等。Risco等[
与生物修复技术的结合也是对EK修复进行强化的一种方法。EK与PR的耦合,被称为电动力辅助的植物修复(electrokinetic-assisted phytoremediation,简称EKPR),其在重金属污染土壤修复中已有研究,但对有机污染物的研究相对较少[
MES是新兴的一种微生物修复技术,其原理如
MES原理示意图
Schematic diagram of MES
MFCs是利用生物电化学技术来完成土壤中污染物的去除,同时还可产生电能。在土壤MFCs中,最常用的是空气阴极MFCs,由于空气阴极MFCs有取之不尽的电子受体(O2),同时利用微生物作为催化剂,将化学能直接转化为电能[
土壤MFCs对土壤中的PAHs[
土壤MFCs常见构型(a):双室;b):U型[
Mainstream configurations of soil MFCs(a): Dual-chamber; b): U-shape; c): Single-chamber; d): Column-type)
外加电阻对污染物的去除有影响,小外阻使得土壤中MFCs的电流增大,而污染物的降解速率随着电流的增加而加快[
以上研究表明,土壤MFCs对土壤中有机污染物具有显著的去除效果,电极材料、反应器构型、外阻和电极间距离均会影响土壤MFCs的产电和降解污染物的能力。在电极材料方面,改性后的碳毡处理效果较好,优于易老化的碳网和表面积较小的碳布,生物炭作为传统电极的替代材料,尚需要更多的研究;在外阻方面,外阻越小,土壤MFCs的电流越大,污染物去除率越高;反应器以柱型MFCs为最佳,不仅可改善传质、降低内阻,还能扩大微生物的作用半径;污染物的去除率随着电极间距离的减小而增加,但较小的间距需要更多的电极,会增加成本投入。
利用MFCs去除土壤有机污染物时,由于土壤的导电性较低或者有机污染物在土壤中的溶解度有限,常使得土壤MFCs去除污染物的能力受限。因此可通过增加土壤导电性、加入共基质或表面活性剂以及与其他技术联用等来对土壤MFCs进行强化。Li等[
此外,研究发现向土壤MFCs中加入葡萄糖作为共基质,能使电压输出增加262%,石油烃的降解效率增加200%;外加碳源可促进盐渍土中石油烃的生物电化学降解,为治理贫瘠地区和极端环境中的土壤污染提供了有效途径[
与微生物燃料电池产电有所不同,Rodrigo等[
土壤中微生物的种类丰富,随着MFCs的运行,阳极微生物群落的多样性有所降低,因此,了解土壤修复过程中微生物群落的结构和演化是揭示微生物电化学降解机理的重要途径。Yu等[
电化学技术的应用为土壤中有机污染物的去除提供了灵活、可持续、环保的解决方案,解决了低渗透性土壤难以修复的问题。电动力(EK)修复是通过施加电场,利用电迁移、电渗析、电泳和电解等达到去除土壤中有机污染物的目的,针对土壤中石油类以及农药类污染物的去除,已有大量的研究,且取得了较好的成果。MES技术在土壤修复方面的研究尚处于起步阶段,它是通过不加或施加很低的电压来刺激微生物的活性,提高污染物的去除效果,同时能够获得电能。影响电化学反应的因素有很多,通过开发新的电极材料、优化运行参数及反应器构型可很大程度上提高土壤中有机污染物的去除效果。
首先,土壤的导电能力较差,若要实现电化学技术的大规模应用,有效半径是需要考虑的一个重要参数。在实际污染修复中,除了可通过优化电极排列或电池构型来扩大电极作用的有效半径,也可向土壤中加生物炭、碳纤维、氧化石墨烯和沙子等增加土壤导电性和物质传输能力,进而扩大作用半径。特别地,作为增加土壤导电性的物质,生物质炭具有来源广泛、制造简单、能耗低、多孔结构便于微生物附着以及环境友好和可持续发展的优点,具有不可替代的优势。
其次,为了维持土壤修复的长期运行,需要考虑电极的钝化和腐蚀问题。对于EK而言,虽然金属及其氧化物电极可显著提高EK的修复效果,但大大增加了成本,而且极易钝化和腐蚀。对于MES,目前常用的电极材料是碳材料,其他材料的探索尚鲜有报道。因此,开发新的电极材料是未来的研究方向之一。
再次,添加表面活性剂能增加土壤中水溶性差的有机污染物的去除效果。其中生物表面活性剂由于可再生且对土壤无污染,具有很大的应用前景。MES中的MFCs运行时需要土壤水淹环境来保证阴阳极的离子交换,大大限制了MFCs修复的应用范围,因此需要开发其他的反应器构型以扩大其应用。
此外,电化学修复技术大量实验室规模的探索证明了其对土壤中有机污染物修复的显著作用,但增大规模对修复效果的影响尚需更多的探索。目前的研究表明,中试规模的EK对污染物的修复效果明显低于实验室研究,因此如何保证规模放大后的修复效果亦需要更多的研究。
最后,EK修复的机理是在电动力辅助下土壤中的污染物迁移积累后通过化学氧化或生物修复去除,但施加电场后对于化学氧化和生物修复的影响尚不清楚,需要进一步研究。对于土壤MES而言,污染物的去除主要是通过微生物的阳极氧化和阴极还原,但是阴阳极不同微生物之间的协同竞争关系,尚不清楚。土壤功能微生物群落的发育是决定MES系统性能的关键,为了达到修复的目的,不同土壤污染物的降解需要不同种类的微生物,但土壤性质与群落特征的相关性研究,仍存在较大的空白,亦是未来研究的关键。
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