Management of per- and polyfluoroalkyl substances (PFAS)-laden wastewater sludge in Maine: Perspectives on a wicked problem.

This article discusses the challenges and potential solutions for managing wastewater sludge that contains per- and polyfluoroalkyl substances (PFAS), using the experience in Maine as a guide toward addressing the issue nationally. Traditional wastewater treatment, designed to remove excess organic waste and nutrients, does not eliminate persistent toxic pollutants like PFAS, instead partitioning the chemicals between discharged effluent and the remaining solids in sludge. PFAS chemistry, the molecular size, the alkyl chain length, fluorine saturation, the charge of the head group, and the composition of the surrounding matrix influence PFAS partitioning between soil and water. Land application of sludge, incineration, and storage in a landfill are the traditional management options. Land application of Class B sludge on agricultural fields in Maine peaked in the 1990s, totaling over 2 × 106 cu yd over a 40-year period and has contaminated certain food crops and animal forage, posing a threat to the food supply and the environment. Additional Class A EQ (Exceptional Quality) composted sludge was also applied to Maine farmland. The State of Maine banned the land application of wastewater sludge in August 2022. Most sludge was sent to the state-owned Juniper Ridge Landfill, which accepted 94 270 tons of dewatered sludge in 2022, a 14% increase over 2019. Between 2019 and 2022, the sum of perfluorooctane sulfonate (PFOS) and perfluorooctanoic acid (PFOA) concentrations in sludge sent to the landfill ranged from 1.2 to 104.9 ng/g dw. In 2022, the landfill generated 71.6 × 106 l of leachate. The concentration of sum of six PFAS in the leachate increased sixfold between 2021 and 2022, reaching 2 441 ng/l. The retention of PFAS within solid-waste landfills and the potential for long-term release of PFAS through liners into groundwater require ongoing monitoring. Thermal treatment, incineration, or pyrolysis can theoretically mineralize PFAS at high temperatures, yet the strong C-F bond and reactivity of fluorine require extreme temperatures for complete mineralization. Future alternatives may include interim options such as preconditioning PFAS with nonpolar solvents prior to immobilization in landfills, removing PFAS from leachate, and interrupting the cycle of PFAS moving from landfill, via leachate, to wastewater treatment, and then back to the landfill via sludge. Long-term solutions may involve destructive technologies such as electron beam irradiation, electrochemical advanced oxidation, or hydrothermal liquefaction. The article highlights the need for innovative and sustainable solutions for managing PFAS-contaminated wastewater sludge.

Linking drivers of plant per- and polyfluoroalkyl substance (PFAS) uptake to agricultural land management decisions.

Widespread contamination of the per- and polyfluoroalkyl substance (PFAS) in agricultural areas is largely attributed to the application of sewage sludge in which the PFAS can be concentrated. This creates a pathway for these contaminants to enter the food chain and, by extension, causes human health and economic concerns. One barrier to managing land with PFAS contamination is the variation in reported plant uptake levels across studies. A review of the literature suggests that the variation in plant uptake is influenced by a host of factors including the composition of PFAS chemicals, soil conditions, and plant physiology. Factors include (1) the chemical components of the PFAS such as the end group and chain length; (2) drivers of soil sorption such as the presence of soil organic matter (SOM), multivalent cation concentration, pH, soil type, and micropore volume; and (3) crop physiological features such as fine root area, percentage of mature roots, and leaf blade area. The wide range of driving factors highlights a need for research to elucidate these mechanisms through additional experiments as well as collect more data to support refined models capable of predicting PFAS uptake in a range of cropping systems. A conceptual framework presented here links drivers of plant PFAS uptake found in the literature to phytomanagement approaches such as modified agriculture or phytoremediation to provide decision support to land managers.

Evidence of compost contamination with per- and polyfluoroalkyl substances (PFAS) from "compostable" food serviceware.

Per- and polyfluoroalkyl substances (PFAS) have been used to waterproof and greaseproof food serviceware for decades. Health concerns about these compounds have drawn attention to the potential for contamination of the food system. Finished compost (n = 3) made from manure and food serviceware labeled "compostable" generated at a large fair was found to contain 12 or 13 of the 28 PFAS compounds sampled for, in concentrations ranging from 1.1 to 183 µg/kg (Σ28PFAS range = 209-455 µg/kg). Of note, perfluorooctanoic acid, a known carcinogen, was found at concentrations between 47.2 and 55.5 µg/kg. In contrast, fresh manure contained only perfluoroctanesulfonic acid at 3.7 µg/kg, and separated food waste from the fair composted with grass clippings and livestock bedding had no detectable PFAS in 2022, and Σ28PFAS = 9.6 µg/kg in 2019. Including compostable serviceware in compost likely contaminates the finished compost and threatens surrounding groundwater and surface waters, in addition to increasing potential crop uptake.

Water temperature and disease alters bacterial diversity and cultivability from American lobster (Homarus americanus) shells.

The American lobster, Homarus americanus, is an economically valuable and ecologically important crustacean along the North Atlantic coast of North America. Populations in southern locations have declined in recent decades due to increasing ocean temperatures and disease, and these circumstances are progressing northward. We monitored 57 adult female lobsters, healthy and shell diseased, under three seasonal temperature cycles for a year, to track shell bacterial communities using culturing and 16S rRNA gene sequencing, progression of epizootic shell disease using visual assessment, and antimicrobial activity of hemolymph. The richness of bacterial taxa present, evenness of abundance, and community similarity between lobsters was affected by water temperature at the time of sampling, water temperature over time based on seasonal temperature regimes, shell disease severity, and molt stage. Several bacteria were prevalent on healthy lobster shells but missing or less abundant on diseased shells, although some bacteria were found on all shells regardless of health status.

Many Questions Remain Unanswered About the Role of Microbial Transmission in Epizootic Shell Disease in American Lobsters (Homarus americanus).

Despite decades of research on lobster species' biology, ecology, and microbiology, there are still unresolved questions about the microbial communities which associate in or on lobsters under healthy or diseased states, microbial acquisition, as well as microbial transmission between lobsters and between lobsters and their environment. There is an untapped opportunity for metagenomics, metatranscriptomics, and metabolomics to be added to the existing wealth of knowledge to more precisely track disease transmission, etiology, and host-microbe dynamics. Moreover, we need to gain this knowledge of wild lobster microbiomes before climate change alters environmental and host-microbial communities more than it likely already has, throwing a socioeconomically critical industry into disarray. As with so many animal species, the effects of climate change often manifest as changes in movement, and in this perspective piece, we consider the movement of the American lobster (Homarus americanus), Atlantic Ocean currents, and the microorganisms associated with either.

Composition and contamination of source separated food waste from different sources and regulatory environments.

Food waste recycling is needed to create a more sustainable, circular food system; however, the process must be carefully managed to avoid the introduction and build-up of contaminants. We collected and screened source-separated food waste for five classes of contaminants (physical contaminants, heavy metals, halogenated organics, pathogens and antibiotic resistance genes) from two regulatory environments (voluntary vs mandated food separation) to quantify contamination. Physical contamination was frequently found; 57% of samples contained non-compostable waste. Most heavy metals were not detected, and although copper and zinc were present in most samples, they were always below the most stringent global standards for compost. Some samples had detectable halogenated organics, including perfluoroalkyl substances (PFAS), which is cause for concern because some of these accumulate in the food chain. PFBA was detected in 60%, PFHxS in 8% and PFNA in 4% of samples tested. The pathogen Salmonella was present in 3% (2/71) and L. monocytogenes in 11% (8/71) of samples. Shiga toxin-producing E. coli was not detected. Next generation sequencing showed the presence of several genera that contain foodborne pathogens, most commonly Yersinia. Antibiotic resistance genes tet(M) and blaTEM were present in 96% and 97% of samples respectively, however the last-resort colistin resistance gene mcr-1 was not detected. Overall contamination in our source-separated samples was low, with the exception of some antibiotic resistance genes, however our processing method might have underestimated packaging-associated contamination. Regulatory environment did not affect contamination, but carbon, nitrogen phosphorus, calcium, copper, tet (M), and physical contamination varied by source type.

Effect of air nanobubbles on oxygen transfer, oxygen uptake, and diversity of aerobic microbial consortium in activated sludge reactors.

Nanobubbles have the potential to curtail the loss of oxygen during activated sludge aeration due to their extensive surface areas and lack of buoyance in solution. In this study, nanobubble aeration was explored as a novel approach to enhance aerobic activated sludge treatment and benchmarked against coarse bubble aeration at the lab scale. Nanobubble aerated activated sludge reactors achieved greater dissolved oxygen levels at faster rates. Higher soluble chemical oxygen demand removal by 10% was observed when compared to coarse bubble aeration with the same amount of air. The activated sludge produced compact sludge yielding easier waste sludge for subsequent sludge handling. The samples showed fewer filamentous bacteria with a lower relative abundance of floc forming Corynebacterium, Pseudomonas, and Zoogloea in the sludge. The microbiome of the nanobubble-treated activated sludge showed significant shifts in the abundance of community members at the genus level and significantly lower alpha and beta diversities.

Bacterial transfer from Pristionchus entomophagus nematodes to the invasive ant Myrmica rubra and the potential for colony mortality in coastal Maine.

The necromenic nematode Pristionchus entomophagus has been frequently found in nests of the invasive European ant Myrmica rubra in coastal Maine, United States, and may contribute to ant mortality and collapse of colonies by transferring environmental bacteria. Paenibacillus and several other bacterial species were found in the digestive tracts of nematodes harvested from collapsed ant colonies. Serratia marcescens, Serratia nematodiphila, and Pseudomonas fluorescens were collected from the hemolymph of nematode-infected wax moth (Galleria mellonella) larvae. Virulence against waxworms varied by the site of origin of the nematodes. In adult nematodes, bacteria were highly concentrated in the digestive tract with none observed on the cuticle. In contrast, juveniles had more on the cuticle than in the digestive tract. Host species was the primary factor affecting bacterial community profiles, but Spiroplasma sp. and Serratia marcescens sequences were shared across ants, nematodes, and nematode-exposed G. mellonella larvae.

A review of chemical and microbial contamination in food: What are the threats to a circular food system?

A circular food system is one in which food waste is processed to recover plant nutrients and returned to the soil to enable the production of more food, rather than being diverted to landfill or incineration. The approach may be used to reduce energy and water use in food production and contribute to the sustainability of the system. Anaerobic digestion and composting are common food waste treatment technologies used to stabilize waste and produce residual materials that can replenish the soil, thus contributing to a circular food system. This approach can only be deemed safe and feasible, however, if food waste is uncontaminated or any contaminants are destroyed during treatment. This review brings together information on several contaminant classes at different stages of the food supply chain, their possible sources, and their fates during composting and digestion. The main aim is to identify factors that could impede the transition towards a safe, reliable and efficient circular food system. We investigated heavy metals, halogenated organic compounds, foodborne pathogens and antibiotic resistance genes (ARGs) in the food system and their fates during digestion and composting. Production and processing stages were identified as major entry points for these classes of contaminants. Heavy metals and foodborne pathogens pose less risk in a circular system than halogenated organics or antibiotic resistance. Given the diversity of properties among halogenated organic compounds, there is conflicting evidence about their fate during treatment. There are relatively few studies on the fate of ARGs during treatment, and these have produced variable results, indicating a need for more research to clarify their fate in the final products. Repeated land application of contaminated food waste residuals can increase the risk of accumulation and jeopardize the safety of a circular food system. Thus, careful management of the system and research into the fate of the contaminants during treatment is needed.

Snowmelt periods as hot moments for soil N dynamics: a case study in Maine, USA.

The vernal transition represents the seasonal transition to spring, occurring as temperatures rise at the end of winter. With rapid snowmelt, microbial community turnover, and accelerated nutrient cycling, this is a critical but relatively under-studied period of ecosystem function. We conducted a study over two consecutive winters (2015-2016) at the Bear Brook Watershed in Maine to examine how changing winter conditions (warming winters, reduced snow accumulation) altered soil nitrogen availability and stream N export during winter and the vernal transition, and how these patterns were influenced by ecosystem N status (N-enriched vs. N-limited). Of the two study years, 2016 had a warmer winter with substantially less snow accumulation and a discontinuous snowpack-and as a result, had a longer vernal transition and a snowpack that thawed before the vernal transition began. Across both years, snowmelt triggered a transition, signaled by increased ammonium concentrations in soil, decreased soil nitrate concentrations due to flushing by meltwater, and increased stream nitrate exports. Despite the contrasting winter conditions, both years showed similar patterns in N availability and export, differing only in the timing of these transitions. The vernal transition has conventionally been considered a critical period for biogeochemical cycling, because the associated snowmelt event triggers physicochemical and biochemical changes in soil systems. This was consistent with our results in 2015, but our data for 2016 show that this may not always hold true, and instead, that warmer, low-snow winters may demonstrate a temporal asynchrony between snowmelt and the vernal transition. We also show that ecosystem N status is a strong driver of the seasonal N pattern, and the interaction of N status and changing climate must be further investigated to understand ecosystem function under our current predicted trajectory of warming winters, declining snowfall, and winter thaw events.

Microbial metabolisms in a 2.5-km-deep ecosystem created by hydraulic fracturing in shales.

Hydraulic fracturing is the industry standard for extracting hydrocarbons from shale formations. Attention has been paid to the economic benefits and environmental impacts of this process, yet the biogeochemical changes induced in the deep subsurface are poorly understood. Recent single-gene investigations revealed that halotolerant microbial communities were enriched after hydraulic fracturing. Here, the reconstruction of 31 unique genomes coupled to metabolite data from the Marcellus and Utica shales revealed that many of the persisting organisms play roles in methylamine cycling, ultimately supporting methanogenesis in the deep biosphere. Fermentation of injected chemical additives also sustains long-term microbial persistence, while thiosulfate reduction could produce sulfide, contributing to reservoir souring and infrastructure corrosion. Extensive links between viruses and microbial hosts demonstrate active viral predation, which may contribute to the release of labile cellular constituents into the extracellular environment. Our analyses show that hydraulic fracturing provides the organismal and chemical inputs for colonization and persistence in the deep terrestrial subsurface.

Temporal changes in microbial ecology and geochemistry in produced water from hydraulically fractured Marcellus shale gas wells.

Microorganisms play several important roles in unconventional gas recovery, from biodegradation of hydrocarbons to souring of wells and corrosion of equipment. During and after the hydraulic fracturing process, microorganisms are subjected to harsh physicochemical conditions within the kilometer-deep hydrocarbon-bearing shale, including high pressures, elevated temperatures, exposure to chemical additives and biocides, and brine-level salinities. A portion of the injected fluid returns to the surface and may be reused in other fracturing operations, a process that can enrich for certain taxa. This study tracked microbial community dynamics using pyrotag sequencing of 16S rRNA genes in water samples from three hydraulically fractured Marcellus shale wells in Pennsylvania, USA over a 328-day period. There was a reduction in microbial richness and diversity after fracturing, with the lowest diversity at 49 days. Thirty-one taxa dominated injected, flowback, and produced water communities, which took on distinct signatures as injected carbon and electron acceptors were attenuated within the shale. The majority (>90%) of the community in flowback and produced fluids was related to halotolerant bacteria associated with fermentation, hydrocarbon oxidation, and sulfur-cycling metabolisms, including heterotrophic genera Halolactibacillus, Vibrio, Marinobacter, Halanaerobium, and Halomonas, and autotrophs belonging to Arcobacter. Sequences related to halotolerant methanogenic genera Methanohalophilus and Methanolobus were detected at low abundance (<2%) in produced waters several months after hydraulic fracturing. Five taxa were strong indicators of later produced fluids. These results provide insight into the temporal trajectory of subsurface microbial communities after "fracking" and have important implications for the enrichment of microbes potentially detrimental to well infrastructure and natural gas fouling during this process.

Polybrominated diphenyl ethers in fish and wastewater samples from an area of the Penobscot River in central Maine.

Polybrominated diphenyl ethers (PBDEs) are one class of flame retardants commonly used in textiles, foams and plastics. They are similar in behavior to the well-studied polychlorinated biphenyls and growing evidence suggests they are widespread global environmental pollutants that are capable of bioaccumulation. Fish tissue samples were collected from sites along the Penobscot River in central Maine. The total concentration of tetra- to hepta-PBDEs in these samples were calculated and generally increased from upstream to downstream locations ranging from 800 to 1810 ng/g lipid at the northernmost site to 5750-29000 ng/g at the downstream sampling site. BDE-47, 99 and 100 were the predominant congeners found in the fish tissue. Wastewater treatment plants (WWTPs) are one of the potential sources of these compounds to the environment through effluent discharge and landspreading of biosolids. Influent, effluent, activated sludge and dewatered biosolids were collected and analyzed for PBDE congeners from a WWTP at Orono, Maine. PBDE congeners were detectable in effluent samples at concentrations from 0.31 to 0.90 microg/l, in the activated sludge at 1.32-3.8 microg/l and in the influent at 4.2-4.3 microg/l, but the majority of the material was concentrated in the biosolids. Total concentration in the biosolids was 2320-3530 microg/kg dry weight.

Correlations between arsenic in Maine groundwater and microbial populations as determined by fluorescence in situ hybridization.

Arsenic is known to cause serious health effects when consumed in drinking water. In the state of Maine, approximately half of the population relies on private groundwater wells for their drinking water. Of those wells, as many as 13% may contain arsenic levels above the current EPA maximum contaminant level of 10 microgl(-1). Microorganisms can potentially contribute to arsenic release into groundwater through several mechanisms. Some can reduce arsenate to arsenite, which is more toxic and may be more mobile. Sulfurospirillum species NP4, which was isolated from well water, respires arsenate and could act in this way. Microorganisms can also act indirectly by reducing bedrock surface coatings, such as iron oxyhydroxides, that adsorb arsenic in the groundwater environment. The genus Geobacter contains many species that are capable of iron reduction that could play a role in the indirect release of arsenic into groundwater. Water samples from Northport, ME and the Branch Lake region of Ellsworth, ME, which both have elevated groundwater arsenic levels, have been probed using fluorescence in situ hybridization (FISH), to determine the percentage of the population that is NP4 and the percentage that are Geobacter species. Geobacter abundance correlates well with the total arsenic concentration indicating that indirect mechanisms could be important in releasing arsenic. NP4 appears to be reducing arsenate since its prevalence correlates well with arsenite, the end product of arsenate respiration.

Uptake of mercury by thiol-grafted chitosan gel beads.

This study describes the synthesis and characterization of thiol-grafted chitosan beads for use as mercury (Hg) adsorbents. Chitosan flakes were dissolved and formed into spherical beads using a phase inversion technique, then crosslinked to improve their porosity and chemical stability. Cysteine was grafted onto the beads in order to improve the adsorption affinity of Hg to the beads. The beads possessed an average diameter of 3.2 mm, porosity of 0.9, specific surface area of approximately 100 m2/g, average pore size of approximately 120 angstroms, and specific gravity of 2.0. Equilibrium and kinetic uptake experiments were conducted to study the uptake of Hg by the beads. The adsorption capacity was approximately 8.0 mmol-Hg/g-dry beads at pH 7, and decreased with decreasing pH. Hg adsorption kinetics was modeled as radial pore diffusion into a spherical bead with nonlinear adsorption. Use of the nonlinear Freundlich isotherm in the diffusion equation allowed modeling of the uptake kinetics with a single tortuosity factor of 1.5 +/- 0.3 as the fitting parameter for all initial Hg concentrations, chitosan loadings, and agitation rates. At agitation rates of 50 and 75 rpm, where uptake rate was reduced significantly due to the boundary layer effect, the mass transfer coefficient at the outside boundary was also used as a fitting parameter to model the kinetic data. At agitation rates higher than 150 rpm, pore diffusion was the rate-limiting step. The beads exhibited a high initial uptake rate followed by a slower uptake rate suggesting pore diffusion as the rate-determining step especially at high agitation rates. Higher uptake rates observed in this study compared to those in a previous study of chitosan-based crab shells indicate that dissolution and gel formation increase the porosity and pore accessibility of chitosan.

Kinetics of cadmium uptake by chitosan-based crab shells.

Crushed crab shells were chemically treated to transform the chitin present into chitosan. Three particle sizes with average diameters of 0.65, 1.43 and 3.38 mm, average pore diameters ranging from approximately 300 to 540 A, and a specific surface area of approximately 30 m2/g were obtained. Batch experiments were performed to study the uptake equilibrium and kinetics of cadmium by chitosan. Adsorption equilibrium followed a Freundlich relationship and was found to be independent of particle size indicating that adsorption takes place largely in the pore space. A high initial rate of cadmium uptake was followed by a slower uptake rate suggesting intraparticle diffusion as the rate-limiting step. The kinetic uptake data were successfully modeled using a pore diffusion model incorporating nonlinear adsorption. The effect of boundary layer resistance was modeled through inclusion of a mass transfer expression at the outside boundary. Two fitting parameters, the tortuosity factor (tau) and the mass transfer coefficient at the outside boundary (k(c)) were used. These parameters were unique for all solute and sorbent concentrations. The tortuosity factors varied from 1.5 for large particles to 5.1 for small particles. The mass transfer coefficient varied from 2 x 10(-7) m/s at 50 rpm to 2 x 10(-3) m/s at 200 rpm. At agitation rates below 100 rpm, boundary layer resistance reduced the uptake rate significantly. Its very high sorption capacity and relatively low production cost make chitosan an attractive sorbent for the removal of heavy metals from waste streams.