The contaminated land remediation industry in China has experienced explosive growth in recent years. However, traditional remediation strategies that typically require high energy and resource inputs are faced with major challenges under China's 2060 carbon neutrality goal. Here, we provide an environmental sustainability assessment of the remediation of a large petrochemical site, particularly from carbon emissions, using life cycle assessment and calculation of the net ecosystem carbon budget; the results showed that the two traditional remediation strategies had carbon emissions of 6.08 x 108 and 1.10 x 108 kg CO2 equivalent (CO2 eq) respectively, and nature-based solution (NbS) reduced carbon emissions to 1.80 x 106 kg CO2 eq, corresponding to 99.8% and 98.6% reductions, respectively. Furthermore, if considering the remediation of a total of 302 petrochemical facilities in China, the estimated carbon emissions were 5.53 x 1011 and 9.99 x 1010 kg CO2 eq based on the two traditional remediation strategies; however, net carbon storage in the NbS could be up to 5.58 x 108 kg CO2 eq if only 30% of the petrochemical-contaminated sites would adopt NbS strategies. Finally, challenges for adopting NbS strategies in China are discussed, and sustainable remediation framework and policy recommendation for implementing NbS are suggested. Our findings not only underscore the feasibility and effectiveness of NbS strategies but also provide valuable insights for sustainable management of contaminated sites in China.
Site-specific arsenic (As) bioaccessibility data can improve the accuracy of health risk assessments, but direct measurements are costly and time-consuming. Even when available, measured values such as the mean still yield remediation targets below natural background levels, limiting their practical use. Existing predictive models, including linear regressions and some machine learning (ML) approaches, often rely on artificially spiked or limited field-aged samples with high As concentrations, reducing their generalizability. A global dataset of 1458 records of As bioaccessibility in field-aged soils from studies since the 1990s were complied, covering a wide range of As concentrations (As-T) and soil properties. Gastric bioaccessibility showed a log-normal distribution with a mean of 23.4 %. Among eight ML models, the Random Forest (RF) model performed best (R² = 0.86, RMSE = 0.58). As-T explained 73.2 % of the variance, with significant relationships observed with Fe, Mn, organic carbon, and pH. Applied to a contaminated sintering site in southwest China, the RF-informed probabilistic risk assessment yielded a remediation target three times higher than current standards and reduced soil remediation volume and carbon emissions by 79.1 %. This study highlights the potential of ML to enhance risk assessment accuracy and support more sustainable site remediation strategies.
Health risks to workers involved in the active pit excavation of volatile organic compound (VOC)-contaminated soils have been overlooked, despite the prevalence of ex-situ remediation practices in China. This study developed a new VOC exposure in pit excavation (VEPE) model that comprehensively accounts for the release of gasphase VOCs in soil pores, surface volatilization of newly exposed agglomerates, and volatilization of newly exposed excavation pit bottom surfaces. Additionally, the model incorporates the concentration variation of soil contaminants, spatial heterogeneity of soil properties, and the variability and uncertainty of worker exposure using two-dimensional Monte Carlo simulation (2D MCS), highlighting the importance of controlling area of new exposure surfaces, soil saturation, and air exchange during the pit excavation to mitigate risks. The study evaluated worker-health-based risks during the excavation of a VOC-contaminated site in Beijing and revealed that the inhalation cancer risk for trichloroethylene (2.35 x 10(-6)) and its hazard quotient (143.92) exceed the acceptable levels (10(-6) and 1.0, respectively). The comparison of models demonstrated the theoretical advancements of the VEPE model over existing pit excavation models, while the field test comparison showed a significant improvement in the predication accuracy. This study addresses the under-researched area of worker safety in contaminated excavation sites. The findings have the potential to promote cleaner and more sustainable practices in ex-situ contaminated site remediation by providing valuable insights for implementing effective control measures to mitigate the emission of toxic VOCs, thereby reducing adverse social and environmental impacts.
Arsenic is a highly toxic soil contaminant, which is a major public concern. The universal health risk models and global efforts on deriving remedial goals for arsenic-contaminated soil have not yielded the desired or very satisfactory results. In this study, we developed a probabilistic risk-assessment method with a two-dimensional Monte Carlo simulation by integrating arsenic bioaccessibility uncertainty and human exposure variability. We found that arsenic bioavailability significantly varied in gastric (0.59-43.20%) and intestinal (0.72-44.22%) phases owing to arsenic fractions and total iron content. We showed that the mean carcinogenic risk at the 95th percentile was 7.64 x 10-5, exceeding the acceptable risk level (10-6), and the non-carcinogenic risk was 3.48, exceeding the acceptable risk level (1.0). Finally, we recommend 25.72 mg/kg as a remedial goal for the site based on this new approach. Overall, this study demonstrated that the improved method effectively mitigates the conservative nature of the existing regulatory approach. The improved approach helps prevent unnecessary remediation actions, supporting SDG 13 climate action by lowering pollutant and carbon emissions.
为反映实际场地源强或挥发通量的衰减对室内风险的影响,以某挥发性有机污染场地为例,在原有Jury模型基础上增加了建筑物底板及场地地层垂向异质性对传输通量的影响作用,比较了 J&E模型与Jury模型在预测挥发通量,室内空气浓度、健康风险评估结果的差异及影响因素.结果表明:J&E模型预测进入室内的苯通量恒定,与实际场地存在源衰减不符.Jury模型可反映源通量衰减、包气带土壤和建筑底板的阻滞对室内浓度及风险的影响;Jury模型中的暴露区间设定是影响风险水平的关键因素.源形成初期,即T1情景下,暴露期只有两个点位超出可接受风险水平;中期T2情景下,4个点位超出风险可接受水平,后期T3情景下,7个点位超出风险可接受水平,而J&E模型为恒定源,不同时期均为7个点位超标.总体而言,Jury模型考虑了污染源衰减及上方覆盖土壤的阻滞作用,相对J&E模型更为合理.
Traditional phase equilibrium models usually depend on simplified assumptions and empirical parameters, which are difficult to obtain during regular site investigations. As a result, they often under- or over-estimate soil vapor concentrations for assessing the risks of volatile organic compound (VOC)-contaminated sites. In this study, we develop several machine learning models to predict soil vapor concentrations using 2225 soil-soil vapor data pairs collected from seven contaminated sites in northern China. Compared to the classic dual equilibrium desorption model, the random forest (RF) model can provide more accurate predictions of soil vapor concentrations by at least 1-2 orders of magnitude. Among the employed covariates, soil concentration and organic carbon-water partition coefficient are two of the most significant explanatory covariates affecting soil vapor concentrations. Further examination of the developed RF model reveals the phase equilibrium behavior of VOCs in soil is that: the soil vapor concentration increases with soil concentration at different rates in the first two intervals but remains almost unchanged in the last interval; the solid-vapor partitioning interface may still exist at up to 15% mass water content in our simulations. These findings can help site investigators perform more accurate risk assessments at VOC-contaminated sites.
在某场地苯重点污染区布置10个钻孔,按规范采集检测了 63对土壤-土壤气样品,基于土壤和土壤气VOCs浓度分别刻画了场地污染并评估了风险.结果显示,土壤采样和土壤气采样两种方法揭露的污染垂向分布特征基本一致,10个钻孔中采集的土壤气样品均存在一定程度超标,超过土壤气筛选值1.242mg/m3的样品比例为35%,最大超标1000倍,但仅3个钻孔中采集的土壤样品存在超标,超过土壤筛选值1mg/kg的样品比例为5%,最大超标30倍.可见,仅检测土壤样品可能低估场地中VOCs的污染范围和程度,在以砂土为主的场地尤为明显.采用线性分配模型基于土壤中苯检出浓度预测的健康风险较基于实测土壤气中苯浓度预测的风险总体高约1个数量级,因为"老化"、"锁定"等环境行为导致实际污染场地中VOCs在土壤固-液-气间的分配并不完全遵循瞬间平衡分配原理,线性平衡分配模型预测的土壤气浓度显著高于实测值.此外,不考虑苯系物这类易生物降解的VOCs在传输过程中的生物降解过程可导致场地实际健康风险被高估至少2个数量级,评估结论会发生本质的变化.因此,我国应尽快启动基于土壤气的VOCs场地调查与风险评估技术方法的系统研究及相关标准规范的制定,为场地环境管理提供科学支撑.
The current regulatory site investigation employs the J&E model to predict vapor intrusion risk. However, the J&E model assumes that the source concentration is constant for a given exposure period, which is not consistent with the actual site source under depletion. In this study, we compared the differences between the J&E model (constant source), SD source depletion model, and RBCA source depletion model for predicting indoor concentration variation as well as the risk levels during the exposure period with a case study in Beijing. The results showed that the source and indoor air concentrations predicted by the SD and RBCA models showed exponential decreases, whereas those predicted by the J&E model maintained high concentrations throughout the exposure period, which greatly overestimated the risk. The RBCA predicted source depletion at the fastest rate, but the predicted indoor air concentrations were still lower than those of the SD model, which was related to the fact that the RBCA did not consider the effect of buildings on source depletion and did not follow mass conservation. Further, the sensitivity analysis showed that the pressure difference (dP) had the greatest influence on the source concentration in the SD model. For the calculated carcinogenic risk and hazard quotients, the J&E constant source model, the SD source depletion model, and the RBCA source depletion model were ranked in descending order. The results indicated that in general the J&E model was too conservative, the RBCA model may have underestimated risk, and the SD model was more suitable for quantifying vapor intrusion risk in reality.
Although many industrial heritage sites have been repurposed into attractive landscapes, the contamination and health risks from polycyclic aromatic hydrocarbons (PAHs) on industrial legacy surfaces remain unexplored. We collected 441wiping surface samples from 95 buildings and facilities at Beijing coking plant in China and found that the concentrations of 16 US EPA priority PAHs (sigma(16)PAHs) ranged from ND-982.16 and ND-4262.20 mg/m(2) on the surfaces of buildings and facilities, respectively. The main source of PAHs was the coking process, and spatial distribution of PAHs was consistent with sigma(16)PAHs in the soil. The carcinogenic risks of BaP, DBA, BbF, BaA, Ind of the facilities remained as industrial heritage relics, and those of Bap, DBA and BbF in the buildings with commercial uses exceeded the acceptable level (10(-6)). The hazard quotient of 9 PAHs was below the acceptable level (1.0). The remedial goals for BaP and DBA (0.11 mg/m(2)) and BbF, BaA and Ind (1.14 mg/m(2)) at the facility heritage relics were derived. Similarly, the RGs for the buildings with commercial uses of BaP, DBA and BbF were 0.16, 0.16, and 1.64 mg/m(2), respectively. Overall, we determined that carcinogenic PAHs on the surfaces of industrial legacy should be regulated for regeneration.
China issued the unified national soil screening levels (NSSLs) in 2018 to assist the regulation of contaminated sites, but the applicability of NSSLs was not thoroughly evaluated. Datasets from the National Qinghai-Tibet Plateau Scientific Data Center indicated great variability of soil organic matter (0.8-173 g/kg), soil water content (0.05-0.6), soil porosity (0.4-0.6), and soil bulk density (1.11-1.59 kg/m3). We analyzed the effects of soil properties on the derivation of SSLs by using Monte Carlo simulations. The soil factors mainly affected the inhalation exposure pathway of volatile organic compounds (VOCs). They had an effect of more than two orders of magnitude on SSLs for most selected VOCs, particularly with the parameters 0.35 > Henry's law constant > 0.1 and carbon-water distribution coefficient of >100. We compared NSSLs with the recommended SSLs assuming fifth percentile by using Monte Carlo simulations. In general, NSSLs were not sufficient to identify contaminated sites that require additional investigation in the south, central, and northwest regions but were too conservative in screening sites out that required no further action in the east and northeast regions. Our framework and findings may contribute to more scientific and effective soil quality management in other large countries.
Pharmaceutical and personal care products (PPCPs) are among the most frequently reported groups of emerging contaminants in groundwater worldwide. PPCPs in rivers may infiltrate into groundwater through hydraulic exchange and potentially threaten drinking water safety and human health. In the present study, the occurrence and distribution of nine PPCPs in riverbank groundwater and adjacent rivers (distance up to 113 m) were investigated at four sites with different lithological features and permeabilities of aquifers in a city in North China. Seven of nine PPCPs were detectable in groundwater, ranging from 90%). The concentrations and major compounds in river water varied with the sampling location and water system distribution, resulting in distinct compositions of PPCPs in the groundwater at each site along with different lithology and hydrological conditions. The spatial distribution of PPCPs in riverbank groundwater was affected by the hydraulic connection between the groundwater and river and the lithology of aquifers. Direct hydraulic connection of a fine sand aquifer to the adjacent river caused a decrease in PPCPs with increasing distance. The results also suggested that sandy gravel aquifers had a lower capacity to attenuate PPCPs compared to that of fine sand. Significant correlations between PPCP concentrations and thirteen physicochemical factors of groundwater were discovered, including nitrate, potassium, and manganese. Overall, this study provides important evidence on the role of lithology and hydrological conditions on the composition, distribution, and influential physicochemical factors of PPCPs in riverbank groundwater.
The partitioning of volatile organic compounds (VOCs) in soil multiphase system is a critical process for vapour intrusion, however, the importance of vapour-solid interface adsorption doesn't receive the due attention, which causes the exposure assessment too conservative particularly in arid conditions. This paper proposed a multiphase partitioning equilibrium (MPE) model establishing the quantitative relationship between VOCs and its various partitioning phases in soil, including solid-liquid interface adsorption phase, vapour phase and dissolved phase and vapour-solid interface adsorption phase. Taking benzene as the targeted pollutant, the model was found in good agreement with the experimental data while the errors were within one magnitude basically. The role of vapour-solid interface adsorption under different soil moisture conditions was also investigated by the model. The results reveals that a) soil moisture is the conspicuous controlling factor that affects the benzene partitioning in soil; b) vapour-solid interface adsorption dominates benzene uptake when soil relative saturation (RS) is under 20% among three typical soils; c) as adsorption by soil minerals (vapour-solid interface adsorption) is reduced by increasing amounts of humidity (RS > 20%), uptake by partitioning into the soil organic matter (OM) increasingly becomes a controlling factor; d) the common sense that vapour concentration of benzene is particularly high with low level of RS may not occur since the vapour-solid interface adsorption dominates benzene uptake in arid environment. The MPE model is suitable for prediction of VOCs partitioning and vapour exposure risk assessment of contaminated soil in arid area.
由于地下水文地质条件的非均质性、污染物环境行为的多样性、修复技术应用的局限性等原因,地下水修复过程存在较大的不确定性,导致出现修复时间和资源的消耗与修复预期不匹配等问题,对地下水修复效果评估和场地再开发利用带来压力.美国提出了地下水修复技术不可达性的概念,推行了技术不可达豁免政策,将技术不可达评估纳入地下水修复管理程序中,并提出适应性管理、低风险结案、长期监测等一系列管理要求,以保障场地修复后的健康风险和环境风险.我国尚未建立技术不可达情景的应对措施和技术体系,在复杂污染场地地下水修复中仍存在修复目标、修复周期、修复效果评估周期等各方面的挑战.本文围绕地下水修复的技术不可达性,借鉴美国污染场地管理经验,提出了修复技术不可达情景下的应对策略,包括建立修复过程跟踪管理技术体系、适时开展残留污染物风险评估、严格落实污染场地后期管理等建议,以期为保障修复后场地再开发安全利用提供理论依据和技术支撑.
我国现行技术导则在评估VOCs呼吸暴露途径健康风险时推荐Johnson-Ettinger(J&E)模型,该模型虽然简单易用,但在实际应用中存在过于保守的问题,采用双元平衡模型(dual equilibrium desorption, DED)对J&E模型进行校正后可以在一定程度上克服该问题.为准确评估实际场地中VOCs呼吸暴露风险,探索JE-DED模型在预测实际场地中VOCs呼吸暴露途径健康风险的适用性,选取苏州某污染场地面积约314 m2 的重污染区域开展三氯甲烷土壤气挥发通量研究进行精细化风险评估,并与基于土壤中三氯甲烷浓度采用J&E模型和JE-DED模型的计算结果进行比较.多手段风险评估结果显示,评价区域三氯甲烷呼吸暴露途径的人体致癌健康风险水平超过可接受水平1.00×10-6 ;就本场地而言,相对于基于土壤浓度风险评估,以基于实测土壤气挥发通量的风险评估结果来表征研究区域整体暴露风险水平更加稳定;研究区域土壤三氯甲烷浓度整体偏高,J&E和JE-DED模型计算的风险水平无明显差异;通过数据模拟发现,针对该场地,当三氯甲烷浓度<6 mg·kg-1时,能更好地发挥JE-DED模型的优势.该场地三氯甲烷健康风险评估结果表明,基于实测土壤气挥发通量能够一定程度上避免基于土壤浓度计算带来的偶然性结果;JE-DED模型在较低浓度时,才能发挥优势.
An alternative risk assessment strategy for mercury (Hg)-contaminated sites is proposed with bioaccessible fractions and soil Hg vapor (SHgV) concentrations. The new strategy avoids the conservatism of assessment rely on soil total Hg (THg) content and inaccuracy caused by predicted SHgV concentration. The exposure risk to Hg -contaminated soil associated with historical mining activities in Guizhou, China, was evaluated using the proposed strategy. The experimental results revealed that the average bioaccessibility in gastric, intestinal and lung phases was 10.39 % (2.09 % similar to 35.28 %), 1.28 % (0.23 % similar to 4.3 %), and 11.27 % (5.04 % similar to 20.71 %), respectively. Via the proposed strategy, the Hg risk for the oral ingestion pathway, represented as the hazard quotient (HQ), decreased from 1.57 to an acceptable level of 0.19 (< 1). The risk of SHgV inhalation sharply decreased from 1168 to 0.35 while the soil PM10 inhalation pathway did not exhibit significant variations. The dominant exposure pathways turned to oral intake and inhalation of SHgV by the strategy. The results indicated that the proposed assessment strategy can greatly improve the understanding of the exposure risk level at Hg -contaminated sites and provide a reasonable decision basis for decision makers.
Background : From the perspective of contaminated sites risk assessment, vapor-solid interface adsorption of volatile organic compounds (VOCs) in soil is thought to play a pivotal role because this greatly affects the release of VOCs into soil gas thus affecting the concentrations of intrusion and human exposure. Understanding the significance requires quantifying different forms of VOCs that occur in soil, but no relevant models have included the vapor-solid interface adsorption yet. Methods : This paper proposes the multiphase partitioning equilibrium (MPE) model that integrates vapor-solid adsorption phase for the first time. The MPE model establishes the quantitative relationship between the total VOC mass in soil and the mass in various partitioning phases. An equilibrium partitioning experiment was designed to verify the validity of the MPE model. Results : The error of the MPE model was basically within an order of magnitude. It also revealed that that the vapor-solid interface adsorption dominates benzene uptake in dry soil, but as reducing adsorption of soil minerals (vapor-solid interface adsorption) by increasing humidity, uptake by partitioning into the soil organic matter (OM) gradually dominates. Soil moisture was demonstrated the controlling factor that affects the partitioning. It was distinct that exposure concentration of benzene in indoor air rises from 0.0013 mg/m 3 to 0.0070 mg/m 3 when the sandy soil relative saturation increases an order of magnitude from 0.01. Conclusion : This study confirms the significance of VOCs partitioning in soil environment for human health exposure, in addition to frequently-mentioned exposure parameters and building parameters. The MPE model gives accurate mass/concentration prediction of VOCs phases in the soil system, and the relationship between exposure and soil moisture was proved.
复杂污染场地中土壤和地下水介质的非均质性、污染物形态归趋变化的复杂性是导致复杂污染场地调查、风险评估与修复过程存在较大不确定性的主要原因.基于侵入式采样和实验室样品分析等高成本调查技术无法理想反映复杂场地的真实污染分布,简单的定值风险评估结果则具有较大的不确定性,线性化场地管理技术体系不能适应复杂污染场地风险管理面临的不确定性挑战.结合国内外实践经验,本文提出"二精一优"的场地风险管理技术方法体系,即:①基于"有效数据理论"的定量测试与半定量实时监测技术相结合的精准调查技术;②基于污染物形态归趋规律,综合采用基于生物有效性、多证据和概率分析等多种手段的精细化风险评估技术;③动态调整优化的非线性场地风险管理技术框架.
挥发性有机物(Volatile Organic Compounds,VOCs)是场地中常见的污染物,其迁移扩散性强,对环境和人类健康造成威胁.本文梳理总结了近年来国内外在VOCs蒸气入侵行为理论及修复与风险控制技术方面的研究进展,阐述了一系列可用于VOCs污染场地修复与风险控制的相关技术,对不同技术的优缺点、适用范围和应用情况进行了归纳和评价,总结了选择风险控制技术需要考虑的因素,同时指出风险控制系统需要开展有效性、稳定性及长期性的效果评估,并提出如下建议:结合我国场地特点和建筑特征,进一步揭示VOCs蒸气入侵的传输机理和驱动机制;建立修复技术与风险控制技术相结合的VOCs污染场地风险管控技术模式;制定适合我国国情的VOCs蒸气入侵风险控制技术标准体系.
危险物质泄漏是导致场地土壤和地下水污染的常见原因,泄漏场地的应急响应与清理制度是污染场地风险管理制度的重要组成部分,及时开展危险物质泄漏场地的土壤和地下水污染应急响应与清理工作,可降低污染导致的健康与环境危害以及后期土壤和地下水修复成本.目前,许多国家已构建了应急响应、紧急清理和非紧急清理等基于场地污染事件严重性和紧迫性的差异化应对机制,对泄漏场地土壤和地下水污染控制发挥了重要作用,但我国尚未建立泄漏场地土壤和地下水污染应急响应与清理技术体系.该文通过梳理国外场地土壤和地下水污染应急响应与清理体系框架及关键技术,分析总结了国外泄漏场地污染应急响应与清理体系中以现场协调员为核心的多层级多部门协同机制、工作程序、调查评估方法、应急响应与清理模式、措施选择与行动备忘录制定原则等,从技术层面探讨了泄漏场地中污染的移除清理、阻控、封闭隔离与应急修复等关键技术.结合国内外典型案例分析,提出以下建议:①建立涵盖多层级、多部门的泄漏场地污染应急响应与清理协同机制;②制定和完善污染场地应急响应与清理的决策机制和技术标准体系;③建立高素质专业化的应急响应与清理协调指挥队伍;④鼓励开展快速高效应急响应与清理关键技术研发.
At sites impacted by volatile organic compounds (VOCs), vapor intrusion (VI) is the pathway with the greatest potential to result in actual human exposure. Since sites with VI were first widely publicized in late 1990s, the scientific understanding of VI has evolved considerably. The VI conceptual model has been extended beyond relatively simple scenarios to include nuances, such as biological and hydrogeological factors that may limit the potential for VI and alternative pathways, such as preferential pathways and direct building contact/infiltration that may enhance VI in some cases. Regulatory guidance documents typically recommend initial concentration- or distance-based screening to evaluate whether VI may be a concern, followed by a multiple-lines-of-evidence (MLE) investigation approach for sites that do not screen out. These recommendations for detailed evaluation of VI currently focus on monitoring of VOC concentrations in groundwater, soil gas, and indoor air and can be supplemented by other lines of evidence. In this Critical Review, we summarize key elements important to VI site characterization, provide the status and current understanding, and highlight data interpretation challenges, as well as innovative tools developed to help overcome the challenges. Although there have been significant advances in the understanding of VI in the past 20 years, limitations and knowledge gaps in screening, investigation methods, and modeling approaches still exist. Potential areas for further research include improved initial screening methods that account for the site-specific role of barriers, improved understanding of preferential pathways, and systematic study of buildings and infrastructure other than single-family residences.