Arsenic biotransformation in industrial wastewater treatment residue: Effect of co-existing Shewanella sp. ANA-3 and MR-1

Shewanella sp. ANA-3 with the respiratory arsenate reductase (ArrAB) and MR-1 with ferric reduction ability always coexist in the presence of high arsenic (As)-containing waste residue. However, their synergistic impacts on As transformation and mobility remain unclear. To identify which bacterium, ANA-3 or MR-1, dominates As mobility in the coexisting environment, we explored the As biotransformation in the industrial waste residue in the presence of Shewanella sp. ANA-3 and MR-1. The incubation results show that As(III) was the main soluble species, and strain ANA-3 dominated As mobilization. The impact of ANA-3 was weakened by MR-1, probably due to the survival competition between these two bacteria. The results of micro X-ray fluorescence and X-ray photoelectron spectroscopy analyses further reveal the pathway for ANA-3 to enhance As mobility. Strain ANA-3 almost reduced 100% surface-bound Fe(III), and consequently led to As(V) release. The dissolved As(V) was then reduced to As(III) by ANA-3. The results of this study help to understand the fate of arsenic in the subsurface and highlight the importance of the safe disposal of high As-containing industrial waste.     

Co-occurrence of genes for antibiotic resistance and arsenic biotransformation in paddy soils

Paddy soils are potential hotspots of combined contamination with arsenic (As) and antibiotics, which may induce co-selection of antibiotic resistance genes (ARGs) and As biotransformation genes (ABGs), resulting in dissemination of antimicrobial resistance and modification in As biogeochemical cycling. So far, little information is available for these co-selection processes and specific patterns between ABGs and ARGs in paddy soils. Here, the 16S rRNA amplicon sequencing and high-throughput quantitative PCR and network analysis were employed to investigate the dynamic response of ABGs and ARGs to As stress and manure application. The results showed that As stress increased the abundance of ARGs and mobile genetic elements (MGEs), resulting in dissemination risk of antimicrobial resistance. Manure amendment increased the abundance of ABGs, enhanced As mobilization and methylation in paddy soil, posing risk to food safety. The frequency of the co-occurrence between ABGs and ARGs, the host bacteria carrying both ARGs and ABGs were increased by As or manure treatment, and remarkably boosted in soils amended with both As and manure. Multidrug resistance genes were found to have the preference to be co-selected with ABGs, which was one of the dominant co-occurring ARGs in all treatments, and manure amendment increased the frequency of Macrolide-Lincosamide-Streptogramin B resistance (MLSB) to co-occur with ABGs. Bacillus and Clostridium of Firmicutes are the dominant host bacteria carrying both ABGs and ARGs in paddy soils. This study would extend our understanding on the co-selection between genes for antibiotics and metals, also unveil the hidden environmental effects of combined pollution.     

The role of phosphorus in the metabolism of arsenate by a freshwater green alga, Chlorella vulgaris

A freshwater microalga, Chlorella vulgaris, was grown in the presence of varying phosphate concentrations( 10–500 μg/L P) and environmentally realistic concentrations of arsenate(As(Ⅴ))(5–50 μg/L As). Arsenic speciation in the culture medium and total cellular arsenic were measured using AEC-ICP-MS and ICP-DRC-MS, respectively, to determine arsenic biotransformation and uptake in the various phosphorus scenarios. At high phosphate concentration in the culture medium, 100 μg/L P, the uptake and biotransformation of As(Ⅴ) was minimal and dimethylarsonate(DMAs(Ⅴ)) was the dominant metabolite excreted by C. vulgaris, albeit at relatively low concentrations. At common environmental P concentrations, 0–50 μg/L P, the uptake and biotransformation of As(Ⅴ) increased. At these higher As-uptake levels, arsenite(As(Ⅲ)) was the predominant metabolite excreted from the cell. The concentrations of As(Ⅲ) in these low P conditions were much higher than the concentrations of methylated arsenicals observed at the various P concentrations studied. The switchover threshold between the(small) methylation and(large) reduction of As(Ⅴ) occurred around a cellular As concentration of 1 fg/cell. The observed nearly quantitative conversion of As(Ⅴ) to As(Ⅲ) under low phosphate conditions indicates the importance of As(Ⅴ) bio-reduction at common freshwater P concentrations. These findings on the influence of phosphorus on arsenic uptake, accumulation and excretion are discussed in relation to previously published research. The impact that the two scenarios of As(Ⅴ) metabolism, As(Ⅲ) excretion at high As(Ⅴ)-uptake and methylarsenical excretion at low As(Ⅴ)-uptake, have on freshwater arsenic speciation is discussed.     

Bioaccumulation and human health risk assessment of trace metals in the freshwater mussel Cristaria plicata in Dongting Lake, China

Trace metal contamination in water and bioaccumulation in aquatic organisms are human health risks of increasing concern. However, the bioaccumulation of trace metals in the organs of the mussel Cristaria plicata in Dongting Lake, China and the human health risks of mussel consumption are largely unknown. We investigated the concentrations of 15 trace metals and metalloids in surface water, sediments, and C. plicata organs (foot, gill, mantle, and visceral mass) and quantified the bioaccumulation and human health risk of these trace metals in specimens collected from Dongting Lake. The concentrations of most metals in surface water exceeded previously published background values. In contrast, the concentrations of most metals in sediments showed a decreasing trend. Overall, the metal concentrations in the gill and visceral masses of C. plicata were higher than those in the foot and mantle, and higher bioaccumulation capacities were observed for essential metals than for nonessential metals. The mean concentrations of the trace elements Zn, Pb, Cd, As, Cu, and Cr in C. plicata foot samples were lower than the threshold values established by international and Chinese organizations. The estimated daily intake (EDI) values of the essential metal Mn in C. plicata foot was higher than the recommended tolerable daily intake (TDI) values for juveniles. Only Mn for juveniles and As for both juveniles and adults may pose noncarcinogenic health risks through foot consumption. The hazard index (HI) values for adults and juveniles were higher than 1, suggesting significant risks of noncarcinogenic effects to humans by exposure to multiple metals.     

Combined pollution of arsenic and Polymyxin B enhanced arsenic toxicity and enriched ARG abundance in soil and earthworm gut microbiotas

Polymyxin B (PMB) is considered as the last line of antibiotic defense available to humans. The environmental effects of the combined pollution with PMB and heavy metals and their interaction mechanisms are unclear. We explored the effects of the combined pollution with PMB and arsenic (As) on the microbial composition of the soil and in the earthworm gut, as well as the spread and transmission of antibiotic resistance genes (ARGs). The results showed that, compared with As alone, the combined addition of PMB and As could significantly increase the bioaccumulation factor and toxicity of As in earthworm tissues by 12.1% and 16.0%, respectively. PMB treatment could significantly increase the abundance of Actinobacteria in the earthworm gut (from 35.6% to 45.2%), and As stress could significantly increase the abundance of Proteobacteria (from 19.8% to 56.9%). PMB and As stress both could significantly increase the abundance of ARGs and mobile genetic elements (MGEs), which were positively correlated, indicating that ARGs might be horizontally transferred. The inactivation of antibiotics was the main resistance mechanism that microbes use to resist PMB and As stress. Network analysis showed that PMB and As might have antagonistic effects through competition with multi-drug resistant ARGs. The combined pollution by PMB and As significantly promoted the relative abundance of microbes carrying multi-drug resistant ARGs and MGEs, thereby increasing the risk of transmission of ARGs. This research advances the understanding of the interaction mechanism between antibiotics and heavy metals and provides new theoretical guidance for the environmental risk assessment and combined pollution management.     

Bioaccumulation and changes of trace metals over the last two decades in marine organisms from Guangdong coastal regions, South China

Trace metal(Cr, Ni, Cu, Zn, Cd and Pb) exposures, distribution and bioaccumulation were investigated in marine organisms from Guangdong coastal regions, South China. The results showed that all of the selected metals were observed in marine organisms with a predomination of Cu and Zn. The metal exposure levels exhibited obvious variations between species with the decreasing order of crab > shellfish > shrimp > fish. The higher metals enrichment seen in shellfish and crab species primari...     

Occurrence and fate of chlorinated methylsiloxanes in surrounding aqueous systems of Shengli oilfield, China

Mono-chlorinated products of cyclic volatile methylsiloxanes (cVMS), i.e., Monochlormet-hylheptamethylcyclotetrasiloxane [D3D(CH₂Cl)], monochlormethylnonamethylcyclopenta-siloxane [D4D(CH₂Cl)], and monochlormethylundemethylcyclohexasiloxane [D5D(CH₂Cl)], were detected in water [<LOQ (Limit of quantitation) -86.3 ng/L, df (detection frequency) = 23%-38%, n=112] and sediment samples [<LOQ-504 ng/g dw (dry weight), df = 33%-38%, n=112] from 16 lakes located in Shengli oilfield of China, and had apparent increasing trends (31%-34% per annum) in sediments during Year 2014-2020. Simulated experiments showed that chloro-cVMS in sediment-water system had approximately 1.7-2.0 times slower elimination rates than parent cVMS. More specifically, compared with those of parent cVMS, volatilization (86-2558 days) and hydrolysis (135-549 days) half-lives of chloro-cVMS were respectively 1.3-2.0 and 1.8-2.1 times longer. In two species of freshwater mussels (n=1050) collected from six lakes, concentrations of chloro-cVMS ranged from 9.8-998 ng/g dw in Anodonta woodiana and 8.4-970 ng/g dw in Corbicula fluminea. Compared with parent cVMS, chloro-cVMS had 1.1-1.5 times larger biota-sediment accumulation factors (2.1-3.0) and 1.1-1.7 times longer half-lives (13-42 days). Their stronger persistence in sediment and bioaccumulation in freshwater mussels suggested that environmental emission, distribution and risks of chloro-cVMS deserve further attention.     

Temporal variation and sharing of antibiotic resistance genes between water and wild fish gut in a peri-urban river

Antibiotic resistance genes (ARGs) as emergence contaminations have spread widely in the water environment. Wild fish may be recipients and communicators of ARGs in the water environment, however, the distribution and transmission of ARGs in the wild fish and relevant water environment were rarely reported. Here, we have profiled ARGs and bacterial communities in wild freshwater fish and relevant water in a peri-urban river using high-throughput qPCR and 16S rRNA gene sequence. A total of 80 and 220 unique ARG subtypes were identified in fish and water samples. Fish and water both showed significant ARG seasonal variations (P < 0.05). The highest absolute abundance of ARGs in fish and water occurred in summer (1.32 × 10⁹ copies per g, on average) and autumn (9.04 × 10⁶ copies per mL), respectively. In addition, the bipartite network analysis showed that 9 ARGs and 1 mobile genetic element continuously shared in fish and water. Furthermore, bacteria shared in fish and water were found to significantly correlate with shard ARGs. The findings demonstrate that bacteria and ARGs in fish and water could interconnect and ARGs might transfer between fish and water using bacteria as a spreading medium.     

Distribution and chemical speciation of arsenic in different sized atmospheric particulate matters

The distribution and chemical speciation of arsenic (As) in different sized atmospheric particulate matters (PMs), including total suspended particles (TSP), PM₁₀, and PM_2.5, collected from Baoding, China were analyzed. The average total mass concentrations of As in TSP, PM₁₀, and PM_2.5 were 31.5, 35.3, and 54.1 µg/g, respectively, with an order of PM_2.5 >PM ₁₀ > TSP, revealing that As is prone to accumulate on fine particles. Due to the divergent toxicities of different As species, speciation analysis of As in PMs is further conducted. Most of previous studies mainly focused on inorganic arsenite (iAs^III), inorganic arsenate (iAs^V), monomethylarsonate (MMA), and dimethylarsinate (DMA) in PMs, while the identification and sensitive quantification of trimethylarsine oxide (TMAO) were rarely reported. In this study, a high-performance liquid chromatography coupled to inductively coupled plasma mass spectrometry system was optimized for As speciation including TMAO in PMs. An anion exchange column was used to separate MMA, DMA and iAs^V, while a cation exchange column to separate TMAO and iAs^III. Results showed that iAs^V was the dominate component in all the samples, corresponding to a portion of 79.2% ± 9.3% of the total extractable species, while iAs^III, TMAO and DMA made up the remaining 21%. Our study demonstrated that iAs^III accounted for about 14.4% ± 11.4% of the total extracted species, with an average concentration of 1.7 ± 1.6 ng/m³. It is worth noting that TMAO was widely present in the samples (84 out of 97 samples), which supported the assumption that TMAO was ubiquitous in atmospheric particles.     

Simple and rapid determination of dioxin in fish and sea food using a highly sensitive reporter cell line, CBG 2.8D

Food, especially animal origin food is the main source of polychlorinated dibenzo-p-dioxins and dibenzofurans (PCDD/Fs), and dioxin-like polychlorinated biphenyls (dl-PCBs) for human exposure. So, a simple, rapid and cheap bioassay method is needed for determination of dioxins in food samples. In this study, we used a new highly sensitive reporter cell line to determine the concentration of dioxins in 33 fish and seafood samples. The samples were extracted by shaking with water/isopropanol (1:1 v/v) and hexane and cleaned-up by a multi layered silica gel column and an alumina column, then analyzed using CBG 2.8D cell line. We compared the results obtained from the CBG 2.8D cell assay to those obtained from conventional High-Resolution Gas Chromatography–High Resolution Mass Spectrometry (HRGC–HRMS) analysis. Good correlations were observed between these two methods (r²=0.93). While the slope of regression line was 1.76, the bioanalytical equivalent (BEQ) values were 1.76 folds higher than WHO-TEQ values and the conversion coefficient was 0.568 (the reciprocal of 1.76). In conclusion, CBG 2.8D cell assay was an applicable method to determine dioxins levels in fish and sea food samples.     

Polycyclic aromatic hydrocarbons in benthos of the northern Bering Sea Shelf and Chukchi Sea Shelf

Eighteen polycyclic aromatic hydrocarbons(PAHs) were detected in benthos collected onboard the ‘Snow Dragon’ in the Northern Bering Sea Shelf and Chukchi Sea Shelf during the 6 th Chinese National Arctic Research Expedition(CHINARE 2014). 18 PAHs for all biota samples ranged from 34.2 to 128.1 ng/g dry weight(dw), with the highest concentration observed in fish muscle( Boreogadus saida) samples close to St. Lawrence Island. The PAH composition pattern was dominated by the presence of lighter 3 r...     

Evaluation of joint toxicity of heavy metals and herbicide mixtures in soils to earthworms (Eisenia fetida)

It is widely acknowledged that a simplified and robust approach to evaluating thecombined effects of chemical mixtures is critical for ecological risk assessment(ERA) of contaminated soil. The earthworm( Eisenia fetida) was used as a model to study the combined effects of polymetallic contamination and the herbicide siduron in field soil using a microcosm experiment. The responses of multiple biomarkers, including the activities of catalase(CAT), superoxide dismutase(SOD), glutathione reductase(...     

Understanding the risks of mercury sulfide nanoparticles in the environment: Formation, presence, and environmental behaviors

Mercury (Hg) could be microbially methylated to the bioaccumulative neurotoxin methylmercury (MeHg), raising health concerns. Understanding the methylation of various Hg species is thus critical in predicting the MeHg risk. Among the known Hg species, mercury sulfide (HgS) is the largest Hg reservoir in the lithosphere and has long been considered to be highly inert. However, with advances in the analytical methods of nanoparticles, HgS nanoparticles (HgS NPs) have recently been detected in various environmental matrices or organisms. Furthermore, pioneering laboratory studies have reported the high bioavailability of HgS NPs. The formation, presence, and transformation (e.g., methylation) of HgS NPs are intricately related to several environmental factors, especially dissolved organic matter (DOM). The complexity of the behavior of HgS NPs and the heterogeneity of DOM prevent us from comprehensively understanding and predicting the risk of HgS NPs. To reveal the role of HgS NPs in Hg biogeochemical cycling, research needs should focus on the following aspects: the formation pathways, the presence, and the environmental behaviors of HgS NPs impacted by the dominant influential factor of DOM. We thus summarized the latest progress in these aspects and proposed future research priorities, e.g., developing the detection techniques of HgS NPs and probing HgS NPs in various matrices, further exploring the interactions between DOM and HgS NPs. Besides, as most of the previous studies were conducted in laboratories, our current knowledge should be further refreshed through field observations, which would help to gain better insights into predicting the Hg risks in natural environment.     

Burden levels of polychlorinated dibenzo-p-dioxins, dibenzofurans, and polychlorinated biphenyls in typical edible meat animals

The concentrations and distributions of polychlorinated dibenzo-p-dioxins (PCDDs), polychlorinated dibenzofurans (PCDFs), and polychlorinated biphenyls (PCBs) in the whole blood and meat of eight typical edible animals (chicken, donkey, horse, cattle, rabbit, sheep, duck, and pig) were illustrated. Total concentrations of polychlorinated dibenzo-p-dioxins and dibenzofurans (PCDD/Fs) and PCBs (on a basis of liquid volume) in animal bloods were 142-484 pg/L and 46-62 ng/L, respectively. Total concentrations of PCDD/Fs and PCBs (on a basis of dry weight (dw) and lipid weight (lw)) in animal meat samples were 0.47-1090 pg/g dw (0.47-4513 pg/g lw) and 7.2-23 ng/g dw (10-776 ng/g lw), respectively. TEQs for both PCDD/Fs and PCBs in animal blood and meat samples were (67 ± 27) pg/L and (5.3 ± 14) pg/g dw (24 ± 56 pg/g lw), respectively. Besides, the dietary intakes of PCDD/Fs and PCBs were also estimated. Chicken and pig contributed more TEQs than other animals. Chicken contributed the most (95%) with high toxicity, followed by pig (3.4%) with high consumption. The dietary intake of chicken might pose risks to consumers who prefer to eat chicken products, who should comprehensively consider the essential nutrients and contaminants in food during dietary intake.     

Assessing microbial and chemical exposure risks of Giardia in indoor swimming pool water disinfected by chlorine

Swimming pools adopt chlorination to ensure microbial safety. Giardia has attracted attention in swimming pool water because of its occurrence, pathogenicity, and chlorine resistance. To control Giardia concentrations in pool water and reduce the microbial risk, higher chlorine doses are required during disinfection. Unfortunately, this process produces carcinogenic disinfection byproducts that increase the risk of chemical exposure. Therefore, quantitatively evaluating the comparative microbial...     

Different effects of foliar application of silica sol on arsenic translocation in rice under low and high arsenite stress

Foliar application of Si can generally reduce As translocation from roots to shoots in rice; however, it does not always work, particularly under high As stress. Here, the effects of foliar application of nanoscale silica sol on As accumulation in rice were investigated under low (2 μmol/L) and high (8 μmol/L) arsenite stress. The results revealed that foliar Si application significantly decreased the As concentration in shoots under low arsenite stress, but showed different effects under high arsenite stress after 7 days of incubation. The reduction in root-to-shoot As translocation under the 2As+Si treatment was related to the down-regulation of OsLsi1 and OsLsi2 expression and up-regulation of OsABCC1 expression in roots. In the 8As+Si treatment, the expressions of OsLsi1, OsLsi2, and OsABCC1 were significantly promoted, which resulted in substantially higher As accumulation in both the roots and shoots. In the roots, As predominantly accumulated in the symplasts (90.6%–98.3%), in which the majority of As was sequestered in vacuoles (79.0%–94.0%) under both levels of arsenite stress. Compared with that of the 8As treatment, the 8As+Si treatment significantly increased the As concentration in cell walls, but showed no difference in the vacuolar As concentration, which remained constant at approximately 69.1–71.7 mg/kg during days 4–7. It appeared that the capacity of root cells to sequester As in the vacuoles had a threshold, and the excess As tended to accumulate in the cell walls and transfer to the shoots via apoplasts under high arsenite stress. This study provides a better understanding of the different effects of foliar Si application on As accumulation in rice from the view of arsenite-related gene expression and As subcellular distribution in roots.     

A SPE-HPLC-MS/MS method for the simultaneous determination of prioritised pharmaceuticals and EDCs with high environmental risk potential in freshwater

This work describes the development, optimisation and validation of an analytical method for the rapid determination of 17 priority pharmaceutical compounds and endocrine disrupting chemicals (EDCs). Rather than studying compounds from the same therapeutic class, the analyses aimed to determine target compounds with the highest risk potential (with particular regard to Scotland), providing a tool for further monitoring in different water matrices. Prioritisation was based on a systematic environmental risk assessment approach, using consumption data; wastewater treatment removal efficiency; environmental occurrence; toxicological effects; and pre-existing regulatory indicators. This process highlighted 17 compounds across various therapeutic classes, which were then quantified, at environmentally relevant concentrations, by a single analytical methodology. Analytical determination was achieved using a single-step solid phase extraction (SPE) procedure followed by high-performance liquid chromatography with tandem mass spectrometry (HPLC-MS/MS). The fully optimised method performed well for the majority of target compounds, with recoveries >71% for 15 of 17 analytes. The limits of quantification for most target analytes (14 of 17) ranged from 0.07 ng/L to 1.88 ng/L in river waters. The utility of this method was then demonstrated using real water samples associated with a rural hospital/setting. Eight compounds were targeted and detected, with the highest levels found for the analgesic, paracetamol (at up to 105,910 ng/L in the hospital discharge). This method offers a robust tool to monitor high priority pharmaceutical and EDC levels in various aqueous sample matrices.     

The exposure risks associated with pathogens and antibiotic resistance genes in bioaerosol from municipal landfill and surrounding area

Pathogenic microbes with antibiotic resistance can thrive on municipal solid waste as nutrients and be aerosolized and transported to vicinities during waste disposal processes. However, the characterization of pathogenic bioaerosols and assessment of their exposure risks are lacking. Herein, particle size, concentration, activity, antibiotic resistance, and pathogenicity of airborne microorganisms were assessed in different sectors of a typical landfill. Results showed that active sector in downwind direction has the highest bioaerosol level (1234 CFU/m³), while residential area has the highest activity (14.82 mg/L). Botanical deodorizer from mist cannon can effectively remove bioaerosol. Most bioaerosols can be inhaled into respiratory system till bronchi with sizes ranging from 2.1−3.3 and 3.3−4.7 µm. Pathogenic bacteria (Bacilli, Bacillus, and Burkholderia-Paraburkholderia) and allergenic fungi (Aspergillus, Cladosporium, and Curvularia) prevailed in landfill. Although high abundance of microbial volatile organic compounds (mVOCs) producing bioaerosols were detected, these mVOCs contributed little to odor issues in landfill. Notably, surrounding areas have higher levels of antibiotic-resistance genes (ARGs) than inner landfill with tetC, acrB, acrF, mdtF, and bacA as dominant ones. Most ARGs were significantly correlated with bacterial community, while environmental parameters mainly influenced fungal prevalence. These findings can assist in reducing and preventing respiratory allergy or infection risks in occupational environments relating to waste management.