朱濛(1991—),女,安徽桐城人,博士研究生,讲师,主要从事土壤有机金属的生物化学行为与修复研究工作。E-mail:
化学武器残留的二苯砷酸(Diphenylarsinic acid,DPAA)引起的土壤—水环境砷污染事件近年来受到广泛关注。国内外学者对土壤—水环境中DPAA的分析方法、污染状况、迁移转化和修复技术等的研究已取得一定进展。鉴于DPAA污染问题的严峻性和污染修复的迫切性,本文通过系统调研并结合笔者的研究工作,综述了土壤-水环境中DPAA分析方法、来源及污染状况的研究进展,探讨了DPAA吸附/解吸、迁移、转化过程及其关键影响因素和作用机制,阐述了对其污染的物理/化学、生物学修复机理研究;认为建立DPAA污染数据库,开展宏观及微观尺度上DPAA环境行为特征的研究,并系统构建DPAA污染的修复技术方法体系将是该领域今后研究的重点。同时,展望了未来的研究方向,旨在为促进土壤-水环境中DPAA污染及其修复的深入研究、有效降低DPAA的环境健康风险提供理论参考。
Chemical warfare agents containing organoarsenic compounds such as Clark Ⅰ (diphenylcyanoarsine) and Clark Ⅱ (diphenylchloroarsine)were widely produced and used during World Wars Ⅰ and Ⅱ. After the wars, remains of these agentswere simply dumped into the sea or buried underground, thus inevitably polluting the soil-water environments of the sits where they were disposed with the arsenic contained in the chemical weapons. In the environment, these abandoned chemical agents are easily hydrolyzed and oxidized into diphenylarsinic acid (DPAA), rather stable in structure, and other organoarsenic compounds. So far, DPAA has been detected in quite a number of the areas where these chemical weapons were dumped. The detection has aroused extensive concerns because the presence of DPAA may bring about environmental and health risks. Scholars both at home and abroad have already begun doing some researches, trying to find ways to analyze DPAA in the soil and water environments, determine their status and behaviors and remedy the polluted environments. However, few have done any to summarize systematically progresses in the research. In this paper, a review is presented to introduce some high-effect inorganic and organic extractants and GC as well as LC analytical methods for DPAA in the soil, and sources and status of the pollutant in the soil-water environments. Generally speaking, the DPAA contaminated areas are located mainly in Northeast China, and South and Southeast Japan. Especially in the chemical weapons dumping sites, the concentration of total arsenicis far beyond the criteria for safety. At the same time, the paper also discusses how DPAA is adsorbed/desorbed, translocated and transformed in the soil-water environment, what are the factors affecting the processes and what are the mechanisms. Studies in the past reported that the adsorption/desorption of DPAA in soil was controlled by a variety of factors, including pH, inorganic ions, Fe/Al oxides, organic matter, redox potential (Eh), etc. and adsorption of the substance was completed via ligand exchange reactions between hydroxyl groups of Fe/Al oxides and arsenate of DPAA, rather than the hydrophilic effect of organic matter; the effective transformation of DPAA in the soil occurred under flooded anaerobic conditions, and under sulfate-reducing conditions, in particular; and iron reduction and sulfate reduction were the two key factors controlling desorption and transformation of DPAA. In the end, the paper elaborates the physical, chemical and biological technologies available for remediation of DPAA contaminated soil-water environments, and their remediation efficiency, controlling factors and mechanisms as well. In terms of physic-chemical remediation, application of activated carbon, Fenton and Fenton-like oxidation and photochemical degradation has been demonstrated to be able to effectively remove DPAA in soil-water environments. In terms of bioremediation, certain progresses have been made, like screening of highly efficient DPAA degrading bacteria, unfolding microbial remediation and combined microbial-phyto remediationand previewing directions of the future researches. The paper holds that all the relevant research findings will serve as the oretical reference for future in-depth studies on DPAA pollution of soil-water environments, remediation of DPAA polluted environments, and protection of environmental quality and human health from DPAA pollution. For further researches, emphases should be laid on the following aspects: (1) To perfect quality assurance and quality control system for DPAA analytical methods, with focus on development of standard alternatives, purgation of internal standards and markers; (2) To launch investigations on scope and extent of DPAA contamination, while taking into the consideration of geographical locations, soil types and land-use patterns of the chemical weapon burial sites; (3) To explore forms of DPAA bonding with soil colloids, clay minerals and oxides in the soil and molecular binding mechanisms, and elucidate the mechanisms responsible for adsorption/desorption, translocation and transformation of DPAA inmulti-media environment and at microscopic interfaces; (4) To explore for developing new remediation materials, intensify researches on physic-chemical-phyto combined remediation and continue to screen out highly efficient DPAA degrading bacteria and probe mechanisms of their effectiveness at molecular as well as genetic levels, while integrating genetic engineering, molecular biology with phytoremediation technologies, so as to eventually establish a bioremediation technical system applicable to DPAA contaminated media different in type and condition.
在20世纪一战和二战期间,二苯氰砷(Diphenylcyanoarsine,DA)和二苯氯砷(Diphenylchloroarsine,DC)等含砷化学武器被大量生产,并在战争中作为呕吐剂和糜烂剂使用。战后,这些遗弃的化学武器通常仅采用土地填埋和海洋倾倒的方式进行处置,因而填埋和倾倒场所周边的土壤-水环境很容易受到化学武器中砷的污染。目前,已在日本[
如何消除化学武器残留的DA、DC及其降解产物已经引起了政府机构、国际组织和学术界的高度关注。1993年,DA和DC作为必须销毁的化学填料列入《关于禁止发展、生产、储存和使用化学武器及销毁此种武器的公约》附件。2003年,DA和DC作为限制性污染物列入《销毁日本遗弃在华化学武器土壤污染控制标准》(GB19062-2003)[
目前,日本已经对其境内DPAA的分析方法、污染状况、迁移转化和修复技术等开展了较多研究。近年来,欧洲国家针对DPAA的研究逐渐增多,研究内容主要集中于DPAA的污染调查与修复,我国的情况基本相同。鉴于土壤-水环境中DPAA污染问题的严峻性与解决的迫切性,本文将就其分析方法、污染现状、环境行为和修复技术等最新研究进展进行综述,并展望其发展趋势。
目前,DPAA检测的研究主要集中在样品前处理和检测方法上。已报道的前处理方法有固相萃取[
分析DPAA常用的有机提取剂有丙酮[
与有机提取剂相比,无机提取剂在DPAA检测中的应用更为广泛。其中,NaOH常用于土壤中DPAA的提取[
已报道的DPAA测定方法有石墨炉原子吸收光谱法[
GC方法最早被用于化学武器残留的苯砷酸类化合物的定量分析。对于DPAA,目前主要采用衍生化GC-MS方法[
与GC相比,HPLC方法在DPAA检测中的应用更为广泛。Witkiewicz等[
化学武器残留的苯砷酸类化合物的HPLC-MS/MS分析方法及其测定参数
HPLC-MS/MS analytical method and determined parameters of phenylarsinic compounds hung over from chemical weapons
化合物 |
基质 |
检测器 |
线性范围 |
检出限 |
参考文献 |
注:PAA,苯砷酸;PAO,氧化苯胂;DPAA,二苯砷酸;BDPAO,联二苯砷氧化物;TPA,三苯胂;MPAA,甲基苯砷酸;DMPAO,二甲基苯砷酸;MDPAO,甲基二苯砷酸;DA,二苯氰砷;DC,二苯氯砷;PDA,二极管阵列检测器Note: PAA, phenylarsonic acid; PAO, phenylarsinic oxide; DPAA, diphenylarsinic acid; BDPAO, bis(diphenylarsine) oxide; TPA, triphenylarsinic; MPAA, methylphenylarsinicacid; DMPAO, dimethylphenylarsine oxide; MDPAO, methyldiphenylarsine oxide; DA, diphenylchloroarsine; DC, diphenylcyanoarsine; PDA, photo-diode array | |||||
PAA/PAO/DPAA/ BDPAO/TPA | 地下水 |
PDA | 8~30/5~40/20~4 000/ 120~8 000/1~60 mg·L-1 | 0.1/0.1/0.2/10/ 0.1 mg·L-1 | [ |
DPAA | 土壤 |
PDA | 0.1~20 mg·L-1 | 53 µg·L-1 | [ |
DPAA/PAA/PAO | 地下水 |
ICP-MS | 0~120 µg·L-1 | 2.8/2.5/2.5 pg | [ |
PAA/PAO | 地下水 |
ICP-MS | 0~1000 mg·L-1 | 0.2~0.8 µg·L-1 | [ |
MPAA/DMPAO/ MDPAO/DPAA | 土壤 |
ICP-MS | 0~100 µg·L-1 | 0.1~0.2 µg·L-1 | [ |
DA/DC/BDPAO/TPA | 土壤/地下水 |
MS | [ |
||
PAA/PAO/DPAA/ BDPAO | 地下水 |
MS/MS | 0~1 mg·L | 0.0001~0.01 mg·L-1 | [ |
DPAA/PAA | 土壤 |
MS/MS | 0.01~1 mg·L | 0.01/1 µg·L-1 | [ |
DPAA尚未发现有天然形成的例子,其在环境中的出现均归结为人类活动。在一战和二战期间,大量化学武器被生产、制造和使用。资料显示,仅日本在侵华战争时期就曾生产过746万发毒气弹,且几乎研制了世界各国所装备的所有毒气[
DPAA污染的研究区域主要集中在我国东北、日本南部及东南部地区。
化学武器埋藏区环境样品中DPAA及总砷的浓度范围
Range of concentrations of diphenylarsinic acid and total arsenic in environmental samples taken from chemical weapon dumping areas
调查区域 |
基质 |
DPAA浓度 |
总砷浓度 |
参考文献 |
中国东北 |
土壤 |
0.14%~12.87% | [ |
|
中国东北 |
土壤 |
— | 62.9~1 321 mg·kg-1 | [ |
中国东北 |
土壤 |
— | 22.66~2 967 mg·kg-1 | [ |
中国东北 |
土壤 |
— | 30~1 372 mg·kg-1 | [ |
中国吉林 |
土壤 |
— | 0.09~758.4 mg·kg-1 | [ |
日本茨城县 |
地下水 |
< 15 mg·L-1 | — | [ |
日本平冢市 |
土壤 |
< 0.53 mg·kg-1 | — | [ |
日本平冢市 |
地下水 |
< 10 mg·L-1 | — | [ |
日本茨城县 |
地下水 |
0.162~7.98 mg·L-1 | — | [ |
日本筑波市 |
地下水 |
< 15 mg·L-1 | — | [ |
日本卡米苏 |
土壤 |
1.18 mg·kg-1 | 9.80 mg·kg-1 | [ |
日本茨城县 |
地下水 |
< 0.56 mg·L-1 | < 0.85 mg·L-1 | [ |
德国-波兰边境 |
土壤 |
— | 250 000 mg·kg-1 | [ |
德国 |
地下水 |
2.1 mg·L-1 | — | [ |
德国 |
地下水 |
— | < 16 mg·L-1 | [ |
波罗的海 |
沉积物 |
— | 5.1~17.0 mg·kg-1 | [ |
波罗的海 |
沉积物 |
< 9 583 mg·kg-1 | — | [ |
pH是影响DPAA吸附的关键因素。Wang等[
氧化物和有机质也是影响土壤中DPAA吸附的重要因素。Maejima[
氧化还原电位对无机砷吸附/解吸的影响主要体现在碳、铁和硫的价态变化上,其中,有机质作为电子供体促进铁还原通常被认为是导致土壤中无机砷释放的重要原因[
DPAA在土壤中的迁移一方面与吸附作用密切相关,另一方面与DPAA本身的吸附特性有关。目前,仅查到Maejima等[
土壤中DPAA的有效转化发生在淹水厌氧条件下,且与厌氧微生物的作用密切相关。Maejima等[
硫化是淹水土壤中DPAA的另一个重要转化途径。Nakamiya等[
碳-铁-硫耦合作用下土壤中DPAA形态转化与分配过程的示意图
Schematic diagram for morphological transformation and partitioningof DPAA under the coupling effects of carbon, iron and sulfur
有机污染土壤的修复技术主要分为物理/化学修复和生物修复。其中,物理/化学修复尤其适用于高浓度有机物污染场地土壤。由于我国化学武器埋藏区土壤总砷含量往往严重超标[
物理/化学方法能有效钝化或消除土壤中的DPAA。Arao等[
光化学氧化也能达到消除DPAA的目的,这方面的研究近年来开展的较多。Wang等[
至今已报道的DPAA降解菌有不动盖球菌NK0508[
近年来,利用植物去除DPAA的研究也取得了一定进展。冯仕江等[
化学武器残留的DPAA造成的土壤-水环境污染问题已经受到政府机构、国际组织和学术研究机构的高度关注。中国一直致力于解决遗留化学武器污染问题,目前日本遗弃在华化学武器销毁工作已经全面展开,但加强化学武器在长期掩埋过程中的泄露、在销毁过程中产生的弹药污水以及销毁后产生的固体残渣等引起的土壤—水环境DPAA污染的研究与治理仍然刻不容缓。未来应加强以下几个方面的研究:
1)土壤-水环境中DPAA分析方法的标准化。注重标准替代物、净化内标和标准参照物的研制,加强不同实验室之间分析结果的比对,完善质量保证与质量控制体系,建立土壤、水体与沉积物样品中DPAA的标准分析方法,为科学研究和污染监控服务。
2)DPAA的土壤—水环境调研与数据库建立。结合我国化学武器埋藏区的地理位置、土壤类型和土地利用方式等特点,开展区域性的环境介质中DPAA污染范围与浓度水平的调研,建立土壤—水环境DPAA污染数据库。
3)土壤—水环境中DPAA赋存形态和多介质、多界面环境行为。结合化学武器埋藏区的分布特点,研究DPAA在土壤、土壤胶体、黏土矿物、氧化物上的结合形态与分子结合机制,阐明DPAA在多介质环境内部和微观界面的结合/释放、迁移、转化过程及机制,服务于风险评估与污染修复。
4)土壤—水环境中DPAA污染的修复技术。化学武器的销毁与残留的苯砷酸类化合物的污染治理具有同样的重要性。需要开展新型修复材料的研发,加强物理/化学—植物联合修复的研究;继续筛选DPAA高效降解菌,在分子和基因水平上探明其机制,并融合基因工程、分子生物学与植物修复技术,建立适合不同污染介质类型、性质及条件的生物修复技术方法体系。
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