skip to main content


Title: Raw material recovery from hydraulic fracturing residual solid waste with implications for sustainability and radioactive waste disposal
Unconventional oil and gas residual solid wastes are generally disposed in municipal waste landfills (RCRA Subtitle D), but they contain valuable raw materials such as proppant sands. A novel process for recovering raw materials from hydraulic fracturing residual waste is presented. Specifically, a novel hydroacoustic cavitation system, combined with physical separation devices, can create a distinct stream of highly concentrated sand, and another distinct stream of clay from the residual solid waste by the dispersive energy of cavitation conjoined with ultrasonics, ozone and hydrogen peroxide. This combination cleaned the sand grains, by removing previously aggregated clays and residues from the sand surfaces. When these unit operations were followed by a hydrocyclone and spiral, the solids could be separated by particle size, yielding primarily cleaned sand in one flow stream; clays and fine particles in another; and silts in yet a third stream. Consequently, the separation of particle sizes also affected radium distribution – the sand grains had low radium activities, as lows as 0.207 Bq g −1 (5.6 pCi g −1 ). In contrast, the clays had elevated radium activities, as high as 1.85–3.7 Bq g −1 (50–100 pCi g −1 ) – and much of this radium was affiliated with organics and salts that could be separated from the clays. We propose that the reclaimed sand could be reused as hydraulic fracturing proppant. The separation of sand from silt and clay could reduce the volume and radium masses of wastes that are disposed in landfills. This could represent a significant savings to facilities handling oil and gas waste, as much as $100 000–300 000 per year. Disposing the radium-enriched salts and organics downhole will mitigate radium release to the surface. Additionally, the reclaimed sand could have market value, and this could represent as much as a third of the cost savings. Tests that employed the toxicity characteristic leaching protocol (TCLP) on these separated solids streams determined that this novel treatment diminished the risk of radium mobility for the reclaimed sand, clays or disposed material, rendering them better suited for landfilling.  more » « less
Award ID(s):
1640634
NSF-PAR ID:
10093912
Author(s) / Creator(s):
; ; ; ; ;
Date Published:
Journal Name:
Environmental Science: Processes & Impacts
Volume:
21
Issue:
2
ISSN:
2050-7887
Page Range / eLocation ID:
308 to 323
Format(s):
Medium: X
Sponsoring Org:
National Science Foundation
More Like this
  1. High concentrations of barium (Ba), strontium (Sr) and radium (Ra) are present in both the liquid and suspended solid portions of wastewater produced from hydraulic fracturing. These high concentrations often require special treatment in which the solid and liquid portions are separated and then independently treated prior to disposal. The solids are typically disposed in landfills while the liquids are further treated, recycled for future hydraulic fracturing, or disposed via injection wells. Finding optimal treatment methods of both the solid and the liquid fractions requires a thorough understanding of potential Ra mobility from both the raw suspended solids and mineral precipitates formed during treatment. Using a sequential extraction procedure, we found that, without treatment, more than 50% of Ra-226 in the suspended solids was associated with soluble salts and readily exchangeable fractions. When the liquid portion of the wastewater was treated by mixing with acid mine drainage (AMD), which contained high sulfate concentrations, approximately 80–97% of the total Ra-226 in the mixture solution is found in the insoluble sulfate fraction of the precipitate. The activity of Ra-226 sequestered in the precipitated solid sulfate fractions is positively correlated with the Sr/Ba ratio of the wastewater-AMD solution. We discuss implications of these findings for effective long-term management of elevated radium in both solid and liquid wastes. 
    more » « less
  2. Food waste (FW), a major part of the US waste stream, causes greenhouse gases within landfills, but there is an opportunity to divert FW to anaerobic digestion (AD) facilities that produce biogas and digestate fertilizer. The composition of FW inputs to AD determines the value of these products. This study provides insight into the effect of waste composition on the quality of AD products by first characterizing the biogas and digestate quality of anaerobically digested FW from four diets (paleolithic, ketogenic, vegetarian, and omnivorous), and then estimating the difference in biogas produced from codigested FW and brewery waste (BW). Waste feedstock mixtures were incubated in lab-scale bioreactors for 21 days with live inoculum. Biogas quality was monitored for 21–30 days in four trials. Samples were analyzed using a gas chromatograph for detection of methane (CH4) and carbon dioxide (CO2). The composition of the waste inputs had a significant impact on the quality of biogas but not on the quality of the digestate, which has implications for the value of post-AD fertilizer products. Wastes with higher proportions of proteins and fats enhanced biogas quality, unlike wastes that were rich in soluble carbohydrates. Codigestion of omnivorous food waste with carbon-rich agricultural wastes (AW) improved biogas quality, but biogas produced from BW does not necessarily improve with increasing amounts of AW in codigestion. 
    more » « less
  3. null (Ed.)
    Municipal solid waste (MSW) landfills near a metropolitan area are renewable energy resources to produce heat and methane that can generate electricity. However, it is difficult to use those sources productively because disposed MSW in landfills are spatially and temporally heterogeneous. Regarding the prediction of the sources, the analysis of in situ MSW properties is an alternative way to reduce the uncertainty and to understand complex processes undergoing in the landfill effectively. A hydraulic profiling tool (HPT) and membrane interface probe (MIP) test measures the continuous profile of MSW properties with depth, including hydraulic pressure, temperature, electrical conductivity (EC), and the relative concentration of methane at the field. In this study, we conducted a series of the tests to investigate the MSW characteristics of active and closed landfills. MIP results showed that the methane existed closer to right below the top cover in the active landfill and several peak concentrations at different layers of the closed landfill. As the depth and age of the waste increased, the hydraulic pressure increased for both landfills. The average EC results showed that the electrical conductivity decreased with the landfill age. The results of hydraulic properties, temperature, and EC obtained from active and closed sites could be used to estimate the waste age and help designing energy recovery systems. 
    more » « less
  4. Abstract

    Environmental contamination by plastic waste is a growing threat to the environment and human health. Unfortunately, most post‐consumer plastics are still disposed of in landfills, even plastics that could be easily recycled via simple chemical processes. This disconnect between technology and implementation is partly due to the economic barrier posed by multi‐step processes that convert plastic waste into commodity goods. There is an urgent need for green methods to convert plastic waste directly into marketable commodities via simple processes. Herein we report a simple, single‐stage process to chemically recycle poly(ethylene terephthalate) (PET) to yield composites having thermal and mechanical properties that are competitive with commercial structural materials like Portland cement. In this protocol, a mixture of PET and geraniol are heated with elemental sulfur. In this process, transesterification between geraniol and PET with concomitant thiocracking of the PET backbone leads to the formation of a highly‐crosslinked sulfur–PET–geraniol (SPG) network composite. The composite exhibited compressive strength (23.1 MPa) greater than that required for Portland cement to be used in building foundations. This new, single‐stage chemical recycling strategy thus employs a bio‐olefin and waste sulfur to convert PET waste into a durable composite that could serve as a sustainable alternative to traditional cements.

     
    more » « less
  5. Site description. This data package consists of data obtained from sampling surface soil (the 0-7.6 cm depth profile) in black mangrove (Avicennia germinans) dominated forest and black needlerush (Juncus roemerianus) saltmarsh along the Gulf of Mexico coastline in peninsular west-central Florida, USA. This location has a subtropical climate with mean daily temperatures ranging from 15.4 °C in January to 27.8 °C in August, and annual precipitation of 1336 mm. Precipitation falls as rain primarily between June and September. Tides are semi-diurnal, with 0.57 m median amplitudes during the year preceding sampling (U.S. NOAA National Ocean Service, Clearwater Beach, Florida, station 8726724). Sea-level rise is 4.0 ± 0.6 mm per year (1973-2020 trend, mean ± 95 % confidence interval, NOAA NOS Clearwater Beach station). The A. germinans mangrove zone is either adjacent to water or fringed on the seaward side by a narrow band of red mangrove (Rhizophora mangle). A near-monoculture of J. roemerianus is often adjacent to and immediately landward of the A. germinans zone. The transition from the mangrove to the J. roemerianus zone is variable in our study area. An abrupt edge between closed-canopy mangrove and J. roemerianus monoculture may extend for up to several hundred meters in some locations, while other stretches of ecotone present a gradual transition where smaller, widely spaced trees are interspersed into the herbaceous marsh. Juncus roemerianus then extends landward to a high marsh patchwork of succulent halophytes (including Salicornia bigellovi, Sesuvium sp., and Batis maritima), scattered dwarf mangrove, and salt pans, followed in turn by upland vegetation that includes Pinus sp. and Serenoa repens. Field design and sample collection. We established three study sites spaced at approximately 5 km intervals along the western coastline of the central Florida peninsula. The sites consisted of the Salt Springs (28.3298°, -82.7274°), Energy Marine Center (28.2903°, -82.7278°), and Green Key (28.2530°, -82.7496°) sites on the Gulf of Mexico coastline in Pasco County, Florida, USA. At each site, we established three plot pairs, each consisting of one saltmarsh plot and one mangrove plot. Plots were 50 m^2 in size. Plots pairs within a site were separated by 230-1070 m, and the mangrove and saltmarsh plots composing a pair were 70-170 m apart. All plot pairs consisted of directly adjacent patches of mangrove forest and J. roemerianus saltmarsh, with the mangrove forests exhibiting a closed canopy and a tree architecture (height 4-6 m, crown width 1.5-3 m). Mangrove plots were located at approximately the midpoint between the seaward edge (water-mangrove interface) and landward edge (mangrove-marsh interface) of the mangrove zone. Saltmarsh plots were located 20-25 m away from any mangrove trees and into the J. roemerianus zone (i.e., landward from the mangrove-marsh interface). Plot pairs were coarsely similar in geomorphic setting, as all were located on the Gulf of Mexico coastline, rather than within major sheltering formations like Tampa Bay, and all plot pairs fit the tide-dominated domain of the Woodroffe classification (Woodroffe, 2002, "Coasts: Form, Process and Evolution", Cambridge University Press), given their conspicuous semi-diurnal tides. There was nevertheless some geomorphic variation, as some plot pairs were directly open to the Gulf of Mexico while others sat behind keys and spits or along small tidal creeks. Our use of a plot-pair approach is intended to control for this geomorphic variation. Plot center elevations (cm above mean sea level, NAVD 88) were estimated by overlaying the plot locations determined with a global positioning system (Garmin GPS 60, Olathe, KS, USA) on a LiDAR-derived bare-earth digital elevation model (Dewberry, Inc., 2019). The digital elevation model had a vertical accuracy of ± 10 cm (95 % CI) and a horizontal accuracy of ± 116 cm (95 % CI). Soil samples were collected via coring at low tide in June 2011. From each plot, we collected a composite soil sample consisting of three discrete 5.1 cm diameter soil cores taken at equidistant points to 7.6 cm depth. Cores were taken by tapping a sleeve into the soil until its top was flush with the soil surface, sliding a hand under the core, and lifting it up. Cores were then capped and transferred on ice to our laboratory at the University of South Florida (Tampa, Florida, USA), where they were combined in plastic zipper bags, and homogenized by hand into plot-level composite samples on the day they were collected. A damp soil subsample was immediately taken from each composite sample to initiate 1 y incubations for determination of active C and N (see below). The remainder of each composite sample was then placed in a drying oven (60 °C) for 1 week with frequent mixing of the soil to prevent aggregation and liberate water. Organic wetland soils are sometimes dried at 70 °C, however high drying temperatures can volatilize non-water liquids and oxidize and decompose organic matter, so 50 °C is also a common drying temperature for organic soils (Gardner 1986, "Methods of Soil Analysis: Part 1", Soil Science Society of America); we accordingly chose 60 °C as a compromise between sufficient water removal and avoidance of non-water mass loss. Bulk density was determined as soil dry mass per core volume (adding back the dry mass equivalent of the damp subsample removed prior to drying). Dried subsamples were obtained for determination of soil organic matter (SOM), mineral texture composition, and extractable and total carbon (C) and nitrogen (N) within the following week. Sample analyses. A dried subsample was apportioned from each composite sample to determine SOM as mass loss on ignition at 550 °C for 4 h. After organic matter was removed from soil via ignition, mineral particle size composition was determined using a combination of wet sieving and density separation in 49 mM (3 %) sodium hexametaphosphate ((NaPO_3)_6) following procedures in Kettler et al. (2001, Soil Science Society of America Journal 65, 849-852). The percentage of dry soil mass composed of silt and clay particles (hereafter, fines) was calculated as the mass lost from dispersed mineral soil after sieving (0.053 mm mesh sieve). Fines could have been slightly underestimated if any clay particles were burned off during the preceding ignition of soil. An additional subsample was taken from each composite sample to determine extractable N and organic C concentrations via 0.5 M potassium sulfate (K_2SO_4) extractions. We combined soil and extractant (ratio of 1 g dry soil:5 mL extractant) in plastic bottles, reciprocally shook the slurry for 1 h at 120 rpm, and then gravity filtered it through Fisher G6 (1.6 μm pore size) glass fiber filters, followed by colorimetric detection of nitrite (NO_2^-) + nitrate (NO_3^-) and ammonium (NH_4^+) in the filtrate (Hood Nowotny et al., 2010,Soil Science Society of America Journal 74, 1018-1027) using a microplate spectrophotometer (Biotek Epoch, Winooski, VT, USA). Filtrate was also analyzed for dissolved organic C (referred to hereafter as extractable organic C) and total dissolved N via combustion and oxidation followed by detection of the evolved CO_2 and N oxide gases on a Formacs HT TOC/TN analyzer (Skalar, Breda, The Netherlands). Extractable organic N was then computed as total dissolved N in filtrate minus extractable mineral N (itself the sum of extractable NH_4-N and NO_2-N + NO_3-N). We determined soil total C and N from dried, milled subsamples subjected to elemental analysis (ECS 4010, Costech, Inc., Valencia, CA, USA) at the University of South Florida Stable Isotope Laboratory. Median concentration of inorganic C in unvegetated surface soil at our sites is 0.5 % of soil mass (Anderson, 2019, Univ. of South Florida M.S. thesis via methods in Wang et al., 2011, Environmental Monitoring and Assessment 174, 241-257). Inorganic C concentrations are likely even lower in our samples from under vegetation, where organic matter would dilute the contribution of inorganic C to soil mass. Nevertheless, the presence of a small inorganic C pool in our soils may be counted in the total C values we report. Extractable organic C is necessarily of organic C origin given the method (sparging with HCl) used in detection. Active C and N represent the fractions of organic C and N that are mineralizable by soil microorganisms under aerobic conditions in long-term soil incubations. To quantify active C and N, 60 g of field-moist soil were apportioned from each composite sample, placed in a filtration apparatus, and incubated in the dark at 25 °C and field capacity moisture for 365 d (as in Lewis et al., 2014, Ecosphere 5, art59). Moisture levels were maintained by frequently weighing incubated soil and wetting them up to target mass. Daily CO_2 flux was quantified on 29 occasions at 0.5-3 week intervals during the incubation period (with shorter intervals earlier in the incubation), and these per day flux rates were integrated over the 365 d period to compute an estimate of active C. Observations of per day flux were made by sealing samples overnight in airtight chambers fitted with septa and quantifying headspace CO_2 accumulation by injecting headspace samples (obtained through the septa via needle and syringe) into an infrared gas analyzer (PP Systems EGM 4, Amesbury, MA, USA). To estimate active N, each incubated sample was leached with a C and N free, 35 psu solution containing micronutrients (Nadelhoffer, 1990, Soil Science Society of America Journal 54, 411-415) on 19 occasions at increasing 1-6 week intervals during the 365 d incubation, and then extracted in 0.5 M K_2SO_4 at the end of the incubation in order to remove any residual mineral N. Active N was then quantified as the total mass of mineral N leached and extracted. Mineral N in leached and extracted solutions was detected as NH_4-N and NO_2-N + NO_3-N via colorimetry as above. This incubation technique precludes new C and N inputs and persistently leaches mineral N, forcing microorganisms to meet demand by mineralizing existing pools, and thereby directly assays the potential activity of soil organic C and N pools present at the time of soil sampling. Because this analysis commences with disrupting soil physical structure, it is biased toward higher estimates of active fractions. Calculations. Non-mobile C and N fractions were computed as total C and N concentrations minus the extractable and active fractions of each element. This data package reports surface-soil constituents (moisture, fines, SOM, and C and N pools and fractions) in both gravimetric units (mass constituent / mass soil) and areal units (mass constituent / soil surface area integrated through 7.6 cm soil depth, the depth of sampling). Areal concentrations were computed as X × D × 7.6, where X is the gravimetric concentration of a soil constituent, D is soil bulk density (g dry soil / cm^3), and 7.6 is the sampling depth in cm. 
    more » « less