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铬(Cr)是一种过渡金属元素,亦是一种潜在有毒元素存在于整个环境中[1]。尤其是六价铬(Cr(Ⅵ))被认为是第一类致癌物质[2],Cr(Ⅵ)不仅会影响作物产量和质量[3],还会对人群健康造成有害影响,包括致癌和遗传毒性等[4]。在过去几十年中,土壤Cr污染问题越来越严峻,主要集中于皮革鞣制、金属电镀、不锈钢生产、合金制造、印染、化学品生产等行业地区[5]。据报道,在美国国家优先清单上,Cr污染场地约占11%;日本在污染场地中,Cr(Ⅵ)污染场地占14%[6];而我国Cr污染土壤问题也尤为突出,Cr污染土地面积占污染土地总面积的5.1%[7]。
目前,许多修复Cr污染的方法已被开发并应用于实践,例如固化/稳定[8]、土壤淋洗[9]、电动修复[10]、植物修复[11]和生物修复[12]等。尤其是固化/稳定化修复技术[13],该技术包括固化和稳定化2个过程。其中,固化过程通常是利用水泥基材将Cr污染物通过包埋的形式固定在土壤中。稳定化过程则是向土壤中添加稳定剂(还原剂),将高毒性、迁移性强的Cr(Ⅵ)还原成为低毒性的Cr(Ⅲ),进一步形成沉淀或难溶物质,阻止其迁移,最终稳定在土壤中。由于固化/稳定化修复技术能够以相对较低的成本实现修复目标,且具有周期短、效率高等优点。同时,该技术还能够原位或异位处置各种重金属污染物,在我国已被广泛采用。据统计,仅2017-2018年我国土壤修复工程中固化/稳定化修复技术的选取率就高达48.5%[14]。然而,我国修复场地多数以修复工程竣工验收设为终点,却忽略了土壤修复的长期有效性、缺乏对验收后Cr的环境归趋的关注。此外,Cr在修复后土壤中,具有环境行为多变、机制复杂,易迁移和转化的特点,修复后的环境风险也值得重点关注[15]。
综述了Cr在土壤中的氧化与还原、吸附与解吸、沉淀与溶解等物理化学反应以及被植物、微生物吸收与转化等生物作用的环境行为,并通过调研Cr污染场地长期监测现状,探索污染场地修复后Cr的环境归趋及其影响因素,以期为修复后场地的长期风险管理提供参考依据。
固化/稳定化修复后场地土壤中铬的环境行为与归趋
Environmental behavior and fate of chromium in the soils of solidification/stabilization post-remediation sites
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摘要: 土壤重金属铬(Cr)污染形势严峻,对人群健康和生态环境构成了严重威胁。通过固化/稳定化技术降低土壤中金属的毒性或迁移性,是Cr污染场地常用的修复技术之一。由于Cr的环境行为变化多端、机制复杂,故导致固化/稳定化修复后场地存在Cr污染反弹的环境风险。综述了Cr在土壤中的氧化还原、吸附与解吸、沉淀与溶解,以及植物、微生物吸收与转化等多种环境行为;并梳理了已修复的Cr污染场地案例及场地长期跟踪监测数据,探讨了固化/稳定化修复后Cr的环境归趋及其影响因素,以期为修复后场地的风险管理提供参考。Abstract: The chromium (Cr) contamination in soils has posed a serious threat to human health and ecological environment. As the most popular remedial technique addressing Cr contaminated sites, solidification/stabilization can effectively decrease the toxicity and mobility of Cr in soils. Due to the complex and diverse environmental behavior of Cr, however, there are risks of pollution recurrence in post-remediation sites. This review highlighted the environmental behavior of Cr, such as oxidation/reduction, adsorption/desorption, and dissolution/precipitation in soil, as well as the migration and transformation associated with plants and microorganisms. Long-term monitoring data of contaminated sites were also summarized. The environmental fate and key influential factors of Cr in post-remediation sites, where solidification/stabilization was employed, are discussed. This review will provide the critical information for the risk management of post-remediation sites.
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表 1 Cr(VI)还原的常用反应体系
Table 1. The common system of Cr(VI) reduction
反应体系 还原类型 还原条件 环境介质 还原剂/
还原微生物还原效果 参考
文献材料体系 铁基材料 材料投加量2.5%,土壤中Cr(Ⅵ)质量分数85.8 mg·kg−1 土壤 零价铁 土壤中Cr(Ⅵ)质量分数降低92% [53] 摩尔比≥ 5∶1,土壤中Cr(Ⅵ)
质量分数94 mg·kg−1土壤 硫酸亚铁 土壤中Cr(Ⅵ)质量分数降低84% [54] pH = 6.0,Cr(Ⅵ)质量浓度
4.65 mg·L−1水溶液 硫化亚铁 1 h,Cr(Ⅵ)质量浓度降低99%以上 [55] 硫基材料 材料投加量5%,Cr(Ⅵ)浸出浓度664.0 mg·L−1 土壤 硫化钠 Cr(Ⅵ)浸出浓度降低99%以上 [56] pH = 7.6,H2S浓度
800 μmol·L−1,Cr(Ⅵ)
浓度40 μmol·L−1水溶液 硫化氢 pH = 7.6时,21 min内Cr(Ⅵ) 浓度降低到12.6 μmol·L−1 [58] 碳基材料 pH = 7.5和pH = 5.5,材料投加量5%,土壤中Cr(Ⅵ)质量分数100 mg·kg−1 土壤 生物炭 土壤中Cr(Ⅵ)质量分数分别降低74%和88% [60] pH = 5.8,固液比1g∶100 mL,Cr(Ⅵ)浓度1.1 mmol·L−1 水溶液 泥炭腐殖酸 2 d后Cr(Ⅵ)浓度降低100% [62] 生物体系 还原微生物 pH = 7.2,Cr(Ⅵ)质量浓度
20~100 mg·L−1水溶液 Aeromonas hydrophila ATCC 7966 60 h内Cr(Ⅵ)浓度达到平衡,Cr(Ⅵ)修复速率分别为0.200,0.175,0.125,0.090和
0.075 mg·(L−1·h−1)[64] pH = 7.0,Cr(Ⅵ)质量浓度
分别在10~70、80~300 、
500 mg·L−1水溶液 Stenotrophomonas maltophilia 各组Cr(Ⅵ)质量浓度分别降低100%,98%~ 99%和92% [65] 耦合体系 材料+
微生物材料投加量1.5%,土壤中Cr(Ⅵ)质量分数100 mg·kg−1,25 ℃,土壤湿度60% 土壤 纳米FeS@HA-Cr-resistant microflora 90 d后土壤中Cr(Ⅵ)质量分数下降99.16% [66] pH = 7.0,初始Cr(Ⅵ)浓度
0.1 mmol·L−1,进液Cr(Ⅵ)浓度
0.2 mmol·L−1水溶液 氢氧化铁/三氧化二铁-Shewanella alga strain BrY Cr(Ⅵ)最大还原速率为
5.5 μg·h−1[67] 表 2 EPA超级基金Cr污染场地修复后的长期监测数据[70]
Table 2. Long-term monitoring data of EPA Superfund Cr contaminated in post-remediation sites[70]
序号 场地名称 涉及污染物 修复措施 监测年份 地下水中
Cr是否
超标Cr质量浓度分析 1 Bennington Municipal Sanitary Landfill As、Hg、Cr、
有机物等表面覆盖阻隔、拦截沟、渗滤液收集及处理系统、沉积物清理 1999—2019 否 监测点位Cr质量浓度稍有波动,但未曾超标。 2 BFI Sanitary Landfill As、Cr、
有机物等表面覆盖阻隔、地下水拦截沟、气体收集及处理系统 1994—2019 是 Cr质量浓度基本均低于检测限,仅MW-9中Cr超标时有发生,监测质量浓度总体无明显变化趋势。 3 Elizabeth Mine As、Cr、
有机物等污染区覆盖阻隔,部分污染土固化处理;污染水域填土和覆土 2004— 2019 — 缺乏Cr相关长期监测数据。 4 Parker Sanitary Landfill As、Cr、
有机物等表面屏障、地下水处理系统、气体收集及处理系统、地下水及沉积物定期监测 1999-2019 否 地下水中Cr监测未超标。 5 Pownal Tannery As、Hg、Cr、
有机物等废弃物清挖、固化并进行原位覆盖阻隔,地下水及沉积物定期监测 1999—2019 否 地下水中Cr监测未超标。 6 Tansitor Electronics Inc. As、Cr、
有机物等制度控制,长期监测 1999—2019 — 缺乏Cr相关长期监测数据。 7 Saco Tannery Waste Pits As、Cr、
有机物等废物堆和排水区覆盖阻隔,补偿性湿地系统修复 1993—2019 是 地下水Cr基本均低于检测限,仅MW-114B质量浓度存在超标,监测质量浓度总体无明显变化趋势。 8 Hatheway & Patterson As、Cr、
有机物等拆除建筑物,As污染土原位固化/稳定化,二恶英污染土异位处理 2004-2019 否 地下水中Cr监测未超标。 9 Hocomonoco Pond As、Cr、
有机物等DNAPL收集处理系统,底泥清运,污染土固化。 1999—2019 — 缺乏Cr相关长期监测数据。 10 Nyanza Chemical Waste Dump As、Hg、Cr、
有机物等地下水收集处理系统,底泥清运,污染土固化/稳定化 1990—2019 — 缺乏Cr相关长期监测数据。 11 Silresim Chemical Corporation As、Hg、Cr、
有机物等阻隔装置,土壤真空/气相抽提,地下水处理设施(地下水抽提、气提、碳吸附、热氧化等) 1994—2019 否 地下水中Cr监测未超标。 12 Federal Facility: South Weymouth Naval Air Station As、Cr、
有机物等划为10区分开修复。以As、Cr污染的OU1填埋区为例,清理表土,铺设覆盖层,重建湿地,自然衰减监测 2004—2019 否 地下水中Cr监测未超标。 13 W.R. Grace & Co., Inc As、Cr、
有机物等污染土和底泥固化/稳定化、堆存并表面覆盖,地下水抽提以及自然衰减 1994-2019 否 地下水中Cr监测未超标。 14 Wells G&H, Woburn As、Hg、Cr、
有机物等原位土壤气相抽提,污泥清挖处置,地下水抽提处理,原位化学氧化 1994—2019 否 地下水中Cr测未超标。 15 Federal Facility: Pease Air Force Base As、Hg、Cr、
有机物等固废及底泥清挖异位处置,灌注土壤改良剂,地下水抽提处理及生物修复。土壤和地下水曝气(地下水位以下),土壤气相抽提(地下水位以上) 1994—2019 否 地下水中Cr监测未超标。底泥中位于Paol上游和中游的点位Cr质量浓度存在一次超标,推测与附近污染场地的地表径流相关。 16 Pine Street Canal As、Cr(Ⅵ)、
有机物等污染底泥覆盖阻隔,栖息地恢复以及长期监测 2001-2019 否 2007—2011,地下水中Cr监测未超标;2012—2016,Cr不继续作为关注污染物进行监测。 17 Town Garage/Radio Beacon Cr、
有机物等制度控制,长期监测 1994—2019 是 地下水Cr轻度超标,浓度偏高可能是采样扰动有关。采用低流速地下水采样后,重金属指标均未超标。 18 New Hampshire Plating As、Cr、
有机物等石灰和次氯酸钠处理排水系统,建筑物及废弃物清运,污染土化学稳定化 2004-2019 否 地下水中Cr监测未超标。 -
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