Do disinfection byproducts in drinking water have an effect on human cancer risk worldwide? A meta‐analysis

In the present study, a meta‐analysis was carried out to clarify the association between disinfection byproducts (DBPs) in drinking water and human cancer risk worldwide. Kidney, colorectal, esophagus, urinary bladder, brain, breast, leukemia, lung, and rectum cancers were selected to perform this analysis. According to preferred reporting items for systematic review and meta‐analysis protocol (PRISMA) guidelines, the relevant studies were identified and selection criteria (inclusion and exclusion criteria) were applied. Next, effective subgroups in these studies (gender, type of drinking water source, and type of DBPs) were analyzed. The quality of the studies was evaluated using the Newcastle‐Ottawa Scale. In addition, this overall study included analyses of 16 case–control and 3 cohort studies. The overall odds ratio (OR) with 95% confidence intervals (CI) between DBPs and cancer risk was 1.01 (95% CI, 0.94–1.09). The summary ORs of cancer risk were 1.04 (95% CI, 0.89–1.19) for kidney; 0.98 (95% CI, 0.87–1.09) for colorectal; 1.07 (95% CI, 0.84–1.29) for esophagus; 0.93 (95% CI, 0.80–1.06) for pancreatic; 1.00 (95% CI, 0.83–1.18) for brain; 1.13 (95% CI, 0.99–1.26) for breast; 0.93 (95% CI, 0.72–1.13) for leukemia; and 1.18 (95% CI, 1–1.36) for lung cancers. The results of this meta‐analysis suggested that there is not a significant association between DBPs in water and cancer risk. In addition, subgroup analysis shows a positive association with colorectal and kidney cancer risk in men, as well as colon and breast cancers in females. Studies of both genders have shown a significant association between lung and pancreatic cancers. Moreover, this study finds a significant relationship between cancer rate and consumers of city water and bottled water sources. In analyzing different types of DBPs in water, chlorine and trichloromethane show a significant association in increasing cancer risk.     

长距离供水系统中消毒副产物分布特征及二次加氯的影响

供水管网覆盖区域大,导致出厂消毒剂量不足以维持管网末梢余氯量,需进行途中二次投氯.以H市供水管网为目标,通过均匀布点采样分析,考察二次加氯消毒型管网中消毒副产物(disinfection by-products,DBPs)的分布特征.结果表明,管网中检出DBPs包括三氯甲烷(TCM)、一溴二氯甲烷(BDCM)、二溴一氯甲烷(DBCM)、三溴甲烷(TBM)、二氯乙酸(DCAA)、三氯乙酸(TCAA)、二氯乙腈(DCAN)、溴氯乙腈(BCAN)和三氯硝基甲烷(TCNM)等,所检水样中DBPs浓度均低于《生活饮用水卫生标准》(GB 5749-2006)规定的标准限值.二次加氯前检出质量浓度(以平均值±偏差表示)分别为:(8.08±3.34)、(9.77±2.91)、(7.38±4.82)、(2.65±2.02)、(2.95±3.26)、(6.02±6.06)、(3.13±2.48)、(1.61±2.05)和(0.15±0.10)μg·L~(-1).二次加氯后检出质量浓度分别为:(10.30±4.55)、(11.73±3.60)、(8.23±5.22)、(2.95±2.45)、(3.29±3.60)、(8.15±7.58)、(3.31±2.61)、(1.33±2.04)和(0.12±0.06)μg·L~(-1).二次加氯后DBPs含量相较于出厂水至二次加氯点呈明显上升趋势,三卤甲烷(THMs)和卤乙酸(HAAs)分别比前段管网含量升高6.32%～26.60%和5.32%～42.71%.此外,原水水质和季节变化对DBPs的形成有一定影响,夏季DBPs的水平普遍高于春季或秋季.出厂水及管网水DBPs生成势分析表明,H市供水系统中DBPs可能存在超标风险,后续需考虑进一步优化处理工艺以保障供水水质.     

Molecular characterization of transformation and halogenation of natural organic matter during the UV/chlorine AOP using FT-ICR mass spectrometry

UV/chlorine process, as an emerging advanced oxidation process (AOP), was effective for removing micro-pollutants via various reactive radicals, but it also led to the changes of natural organic matter (NOM) and formation of disinfection byproducts (DBPs). By using negative ion electrospray ionization coupled with Fourier transform ion cyclotron resonance mass spectrometry (ESI FT-ICR MS), the transformation of Suwannee River NOM (SRNOM) and the formation of chlorinated DBPs (Cl-DBPs) in the UV/chlorine AOP and subsequent post-chlorination were tracked and compared with dark chlorination. In comparison to dark chlorination, the involvement of ClO^?, Cl^?, and HO^? in the UV/chlorine AOP promoted the transformation of NOM by removing the compounds owning higher aromaticity (AI_mod) value and DBE (double-bond equivalence)/C ratio and causing the decrease in the proportion of aromatic compounds. Meanwhile, more compounds which contained only C, H, O, N atoms (CHON) were observed after the UV/chlorine AOP compared with dark chlorination via photolysis of organic chloramines or radical reactions. A total of 833 compounds contained C, H, O, Cl atoms (CHOCl) were observed after the UV/chlorine AOP, higher than 789 CHOCl compounds in dark chlorination, and one-chlorine-containing components were the dominant species. The different products from chlorine substitution reactions (SR) and addition reactions (AR) suggested that SR often occurred in the precursors owning higher H/C ratio and AR often occurred in the precursors owning higher aromaticity. Post-chlorination further caused the cleavages of NOM structures into small molecular weight compounds, removed CHON compounds and enhanced the formation of Cl-DBPs. The results provide information about NOM transformation and Cl-DBPs formation at molecular levels in the UV/chlorine AOP.     

Nitrogenous and carbonaceous aerosols in PM2.5 and TSP during pre-monsoon: Characteristics and sources in the highly polluted mountain valley

This study reports for the first time a comprehensive analysis of nitrogenous and carbonaceous aerosols in simultaneously collected PM_2.5 and TSP during pre-monsoon (March–May 2018) from a highly polluted urban Kathmandu Valley (KV) of the Himalayan foothills. The mean mass concentration of PM_2.5 (129.8 µg/m³) was only ~25% of TSP mass (558.7 µg/ m³) indicating the dominance of coarser mode aerosols. However, the mean concentration as well as fractional contributions of water-soluble total nitrogen (WSTN) and carbonaceous species reveal their predominance in find-mode aerosols. The mean mass concentration of WSTN was 17.43±4.70 µg/m³ (14%) in PM_2.5 and 24.64±8.07 µg/m³ (5%) in TSP. Moreover, the fractional contribution of total carbonaceous aerosols (TCA) is much higher in PM_2.5 (~34%) than that in TSP (~20%). The relatively low OC/EC ratio in PM_2.5 (3.03 ± 1.47) and TSP (4.64 ± 1.73) suggests fossil fuel combustion as the major sources of carbonaceous aerosols with contributions from secondary organic aerosols. Five-day air mass back trajectories simulated with the HYSPLIT model, together with MODIS fire counts indicate the influence of local emissions as well as transported pollutants from the Indo-Gangetic Plain region to the south of the Himalayan foothills. Principal component analysis (PCA) also suggests a mixed contribution from other local anthropogenic, biomass burning, and crustal sources. Our results highlight that it is necessary to control local emissions as well as regional transport while designing mitigation measures to reduce the KV's air pollution.     

Transformation mechanism and fate of dissolved organic nitrogen (DON) in a full-scale drinking water treatment

Dissolved organic nitrogen (DON) has attracted much attention in drinking water treatment due to its potential to produce nitrogenous disinfection by-products (N-DBPs). This work was designed to explore the transformation and fate of DON and dissolved inorganic nitrogen (DIN) in drinking water treatment. The changes of DON and formation of N-DBPs were evaluated along the water treatment route (i.e., pre-ozonation and biological-contact oxidation, delivery pipes’ transportation, coagulation-sedimentation, sand filtration, post-ozonation, biological activated carbon, ultrafiltration and disinfection) of drinking water treatment plant (DWTP). The transformation mechanism of DON was comprehensively investigated by molecular weight fractionation, three-dimensional fluorescence, LC-OCD (Liquid Chromatography-Organic Carbon Detection), total free amino acids. A detailed comparison was made between concentrations and variations of DON and DIN affected by seasons in the drinking water treatment. Regardless of seasonal variation in raw water concentration, the DON removal trends between different treatment processes remain constant in the present study. Compared to other treatment processes, pre-ozonation and coagulation-sedimentation exhibited the dominant DON removal in different seasons, i.e., 11.13%-14.45% and 14.98%-22.49%, respectively. Contrary, biological-contact oxidation and biological activated carbon negatively impacted the DON removal, in which DON increased by 1.76%-6.49% in biological activated carbon. This may be due to the release of soluble microbial products (SMPs) from bacterial metabolism, which was further validated by the rise of biopolymers in LC-OCD.     

Effects of ultrasonication on the DBP formation and toxicity during chlorination of saline wastewater effluents

Chlorine disinfection of saline wastewater effluents rich in bromide and iodide forms relatively toxic brominated and iodinated disinfection byproducts (DBPs). Ultrasonication is a relatively new water treatment technology, and it is less sensitive to suspended solids in wastewaters. In this study, we examined the effects of ultrasonication (in terms of reactor type and combination mode with chlorination) on the DBP formation and toxicity in chlorinated primary and secondary saline wastewater effluents. Compared with the chlorinated wastewater effluent samples without ultrasonication, ultrasonic horn pretreatment of the wastewater effluent samples reduced the total organic halogen (TOX) levels in chlorination by ∼30%, but ultrasonic bath pretreatment of the wastewater samples did not significantly change the TOX levels in chlorination, which might be attributed to the higher energy utilization and decomposition extent of organic DBP precursors in the ultrasonic horn reactor. Moreover, the TOX levels in the chlorinated samples with ultrasonic horn pretreatment (USH–chlorination), simultaneous treatment (chlorination+USH) and subsequent treatment (chlorination–USH) were also significantly reduced, with the maximum TOX reductions occurring in the samples with ultrasonic horn pretreatment. A toxicity index was calculated by weighting and summing the levels of total organic chlorine, total organic bromine and total organic iodine in each treated sample. The calculated toxicity index values of the chlorinated wastewater effluent samples followed a descending rank order of “chlorination” > “chlorination+USH” > “chlorination–USH” > “USH–chlorination”, with the lowest toxicity occurring in the samples with ultrasonic horn pretreatment. Then, a developmental toxicity bioassay was conducted for each treated sample. The measured toxicity index values of the chlorinated wastewater samples followed the same descending rank order.     

臭氧与氯联合消毒对钱塘江水源水DBPs形成及溴取代的影响

本文研究了在pH 6～8、反应时间2～72 h、反应温度10～30℃条件下,钱塘江水源水在臭氧-氯消毒联合作用下,三卤甲烷(THMs)、二卤乙酸(DHAAs)、三卤乙酸(THAAs)、二卤乙腈(HANs)、三卤硝基甲烷(THNMs)等5类消毒副产物(DBPs)的形成和溴取代特征.结果显示,臭氧-氯消毒下DBPs的形成与氯消毒有较多相似之处:①大部分DBPs形成量均随着温度的升高、时间的延长而增加,相应的溴取代因子(BSFs)则随着时间的延长、温度的上升而呈下降趋势;②氯代DHANs倾向于在酸性条件下形成多,而溴代DHANs则倾向于在碱性条件下形成多;③不管是氯消毒还是臭氧-氯消毒,也不管是哪种消毒条件,5类DBPs的BSF值顺序均为BSF_(HNMs)BSF_(DHANs) BSF_(THAAs)BSF_(THMs)≈BSF_(DHAAs).但与氯消毒不同的是,臭氧-氯消毒下THMs、DHAAs、THAAs、HANs的形成产量更低,而THNMs的产量则更高;而且与氯消毒相比,臭氧-氯消毒普遍增加了DBPs的溴取代程度,也改变了溴离子在不同DBPs之间的分配,即减少了THMs、DHAAs、THAAs、DHANs对溴的利用率,但大幅增加了HNMs的溴利用率.鉴于溴代HNMs的极高毒性,因此对于钱塘江水源水,臭氧-氯消毒要注意HNMs带来的健康风险.     

自来水常规和深度处理工艺中挥发性有机物的变化规律

针对连云港市3个自来水厂不同的消毒处理工艺,研究了常规和深度处理对原水中挥发性有机物(VOCs)的处理效果和工艺过程中VOCs的形成规律.在所采集的水样中,67种目标VOCs有3类共30种被检出,其中羰基化合物、卤代烃和苯系物的检出浓度范围分别是0.04~61.27、0.02~35.61和0.07~2.33μg·L-1.研究表明,常规氯消毒工艺能有效去除原水中的苯系物类化合物,但会产生三卤甲烷(THMs)等消毒副产物;臭氧-生物活性炭深度处理工艺能有效降低预氯化过程中THMs的生成量,但会产生如羰基化合物等风险污染物.管网中深度处理产生的羰基化合物在余氯作用下转化形成THMs.管网水中检出的VOCs除巴豆醛的致癌风险在9.3×10-5~2.2×10-4之间,略高于US EPA的控制阈值(10-6~10-4)外,其他化合物的健康风险都处于较低水平.     

Fe/Cu催化还原降解饮用水中溴氯乙腈的性能研究

为了降低饮用水在氯消毒过程中产生的消毒副产物(DBPs)溴氯乙腈(BCAN)对人体带来的健康危害,采用Fe/Cu催化还原的方法降解饮用水中低浓度的BCAN,考察了BCAN的降解效果和其影响因素,探讨了其降解机制及动力学规律.结果表明,Fe/Cu具有更强的还原降解BCAN的能力,与零价铁相比,Fe/Cu(质量比为10∶1)的降解效率是其1.5倍.随着Fe/Cu投加量的增加,BCAN的去除率有明显的提高,对于初始浓度为20μg·L-1的BCAN溶液,当Fe/Cu(质量比为10∶1)投加量由5g·L-1增加到10 g·L-1,反应150 min后,去除率由51.1%增加到89.5%.BCAN降解效率随着温度的升高逐渐提高,BCAN初始浓度的变化对Fe/Cu去除BCAN的去除效果影响不大,Fe/Cu降解BCAN符合一级反应动力学规律.     

太湖、钱塘江取水口底泥及周边土壤有机物形成消毒副产物的特征研究

底泥、土壤均是水体有机物的重要来源,但目前相关消毒副产物(DBPs)形成方面的研究偏少.本研究以长三角重要水源地太湖、钱塘江取水口的底泥和周边土壤的浸出液为研究对象,探索氯、臭氧+氯、氯胺、臭氧+氯胺4种消毒方式下,三卤甲烷(THMs)、卤代酮(HKs)、卤乙腈(HANs)、卤代硝基甲烷(HNMs)的形成情况.结果表明,太湖、钱塘江取水口的底泥、周边土壤有机物的芳香度均很低(SUVA254(即比紫外吸光值)2),与腐殖质(Sigma)相比,底泥、土壤有机物不是氯消毒中THMs的重要前驱物,但却是HANs特别是HNMs的重要前驱物.相比氯消毒,氯胺消毒能大幅降低土壤、底泥有机物THMs、HKs、HANs、HNMs的生成量,而且也可抑制含溴DBPs的形成.臭氧预处理大幅提高了氯、氯胺消毒中HKs、HNMs的产量,但对THMs、HANs则不一定.太湖、钱塘江的土壤、底泥存在一定的溴污染,但不管是哪种消毒方式,均是HNMs的溴嵌入因子最大.