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Review

Produced Water Treatment and Valorization: A Techno-Economical Review

by
Ramon Sanchez-Rosario
and
Zacariah L. Hildenbrand
*
Department of Chemistry and Biochemistry, The University of Texas at El Paso, 500 W. University Ave, El Paso, TX 79968, USA
*
Author to whom correspondence should be addressed.
Energies 2022, 15(13), 4619; https://doi.org/10.3390/en15134619
Submission received: 4 May 2022 / Revised: 9 June 2022 / Accepted: 21 June 2022 / Published: 24 June 2022
(This article belongs to the Special Issue Environmental Analysis, Monitoring, and Optimization of Unconventional Oil and Gas Extraction)
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Abstract

:
In recent years, environmental concerns have urged companies in the energy sector to modify their industrial activities to facilitate greater environmental stewardship. For example, the practice of unconventional oil and gas extraction has drawn the ire of regulators and various environmental groups due to its reliance on millions of barrels of fresh water—which is generally drawn from natural sources and public water supplies—for hydraulic fracturing well stimulation. Additionally, this process generates two substantial waste streams, which are collectively characterized as flowback and produced water. Whereas flowback water is comprised of various chemical additives that are used during hydraulic fracturing; produced water is a complex mixture of microbiota, inorganic and organic constituents derived from the petroliferous strata. This review will discuss the obstacles of managing and treating flowback and produced waters, concentrating on the hardest constituents to remove by current technologies and their effect on the environment if left untreated. Additionally, this work will address the opportunities associated with repurposing produced water for various applications as an alternative to subsurface injection, which has a number of environmental concerns. This review also uses lithium to evaluate the feasibility of extracting valuable metals from produced water using commercially available technologies.

1. Introduction

Flowback-produced water (FP) is a waste fluid associated with hydraulic fracturing in unconventional oil and gas development (UOG). Initially, FP reflects the composition of the hydraulic fracturing fluid, which is referred as flowback water (FBW). After the initial months of well production, the waste fluid is predominantly representative of the formation and is known as produced water (PW) [1]. PW is primarily ancient groundwater which has been reacting with minerals, gases, and organic matter in the subsurface for thousands to millions of years and contains most naturally occurring elements. The composition of FP is highly variable with respect to inorganic, organic, and biological constituents. In fact, several studies have revealed that the relative abundance of certain elements and organic compounds found in FP is a reflection of where the respective production well is located as well as the geological formation from which the fluid is derived [2,3,4,5]. Nevertheless, extremely high levels of sodium (Na) and chlorine (Cl) ions are distinctive characteristics of these brines. For example, studies have reported concentrations of 54,000 and 138,000 parts per million (ppm) in Permian Basin [6]. Naturally occurring radioactive materials (NORM) are within the inorganic species found in FP [7] in addition to iron (Fe), magnesium (Mg), strontium (Sr), calcium (Ca) and several other metal and nonmetal monoatomic and/or polyatomic species [8,9,10,11]. Some studies have reported significant concentrations of radium isotopes [11,12] as well as trace levels of radionuclides of cesium, lead, plutonium, polonium, strontium, thorium and uranium in FP [13,14].
The organic constituents found in FP can be classified in three major categories: aliphatics, aromatics and drilling additives [15]. Aliphatics involve small-chain hydrocarbons (found in petroleum), alkylethoxylates [16], long-chain fatty acids and heterocyclic compounds [17]. Alkyl halides and amines have also been reported [18]. Examples of the aromatics in FP include polycyclic aromatic hydrocarbons (PAHs), xylenes, phenols and alkyl benzenes [16,17,18,19]. Additionally, a wide range of other unknown volatile or semivolatile compounds can be present in PW [20,21].
Chemical additives can be further divided into three major types: alcohols, biocides and surfactants. Chen and Carter have suggested that the most common alcohols present in wells are ethanol, isopropanol, methanol and propargyl alcohol [22]. Other reported alcohols are phenols, ethylene glycol, and ethoxylated and tertbutyl alcohol, which serve as solvents and surfactants and also inhibit corrosion in tubing and equipment [23]. Chen and Carter also stated that “almost all of the added alcohols are considered to be toxic chemicals”. Additionally, biocides are added in hydraulic fracturing fluid to control the proliferation of bacteria in the formation of interest. These chaotropic agents function by reacting with some functional groups in membrane proteins and damaging cell walls, by disulfide bond cleavage and by inhibiting metabolic processes in microorganisms [24]. Some commonly used biocides include glutaraldehyde, quaternary ammonium compounds (QACs), sodium hypochlorite, tetrakishydroxymethylprosphonium sulfate (THPS), various brominated compounds, Tributyltetradecylphosphonium chloride dibromonitrilopropionamide and a combination of 2-methyl-3(2H)-isothiazolone and 5-chloro-2-methyl-3(2H)-isothiazolone. The biodegradability of these compounds varies from rapidly biodegradable (i.e., THPS) to environmentally persistent (i.e., QACs) [17,22,23,25,26]. Lastly, surfactants control the viscosity of fracturing liquids and increase fluid recovery. As many as 84 examples of these have been found in HF fluids [26]. For instance, some common surfactants include alcohol ethoxylates (AEOs), alkylphenol ethoxylates (APEOs), ethoxylated alcohols and phenols, cocamide compounds, sodium lauryl sulfate and dimethyl dihydrogenated tallow ammonium chloride (DHTDMA) [22,23,25].
The biogeochemical richness of PW can often provide an optimal environment for the proliferation of a vast range of microorganisms. Examples of these range from strictly aerobic to anaerobic microbes, including sulfate-reducing bacteria (SRB), iron-oxidizing bacteria (IRB), acid-producing bacteria (APB), sulfur-oxidizing bacteria (SOB) and extremophiles. The presence of SRB (e.g., desulfomicrobium, desulfovibrio, desulfohalubium, desulfobacter) may lead to souring of natural gas, whereas IRB (e.g., desulfuromusa, pelobacter, malonomonas, desulfuromonas) cause corrosion in metal infrastructure [27,28]. APB (e.g., halanaerobium) generate metabolites that could affect the integrity of grout and the casing of wells [29]. A recent study indicated that SOB (e.g., Acidithiobacillus caldus, A. thiooxidans and A. albertensis) promote corrosion in carbon steel by triggering the oxidation of sulfur compounds to sulfate and ultimately generating sulfuric acid [27]. Lastly, extremophiles can withstand extreme conditions, such as very high or low pH or temperature, high salinity, and oil-bearing strata, making them especially persistent. In a previous study, biocide resistance was exhibited in microorganisms such as Arcobacter sp. and Pseudomonas balearica [30]. Other undesired bacteria found in PW include Marinobacterium sp., which—under aerobic conditions—can metabolize aliphatic and aromatic compounds for energy harvesting [31], as well as the fungus Syncephalastrum racemosum, which degrades hydrocarbons in soil [32]. Also present in these brines is the gas-souring Shewanella [33]. By contrast, Thermoanaerobacter exhibits anticorrosive properties through the reduction of thiosulfate to elemental sulfur [34], which might be of benefit to the oil and gas industry.
Numerous analytical techniques are required to comprehensively characterize the chemical profile of FP. For example, gas chromatography coupled with mass spectrometry (GC-MS) and liquid chromatography–mass spectrometry (LC-MS) is utilized to detect and quantify the presence of volatile and semi-volatile organic compounds. Additionally, LC-MS is applied for untargeted analysis of constituents yet to be identified. Inductively coupled plasma-optical emission spectrometry (ICP-OES) and/or inductively coupled plasma mass spectrometry (ICP-MS) facilitate the analysis of metal and nonmetal ions [5]. In particular, ion chromatography (IC) is the “go-to” method for pertinent anions (i.e., chloride, sulfate, sulfide, nitrate, bromide). Methods for the characterization and quantitation of microbial constituents include aerobic and anaerobic plate count (i.e., selective, and nonselective media), Gram staining, microscopy, and molecular methods (i.e., immunological- and nucleic-acid-based techniques). Common molecular methods include polymerase chain reaction (PCR) and DNA sequencing [35]. Analysis of protein profiles by matrix-assisted laser desorption ionization–time-of-flight-mass spectrometry (MALDI-TOF-MS) is a relatively recent innovation that facilitates the rapid identification of microorganisms compared to traditional methods [32]. Lastly, bulk water quality parameters, such as total dissolved solids, total suspended solids, turbidity, organic and inorganic carbon content, pH and oxidation reduction potential (ORP), are predominantly quantified through the use of sensors, titration and gravimetric methods [20,36]. The use of these analytical techniques in concert provides considerable insight into the complex composition of FP, which is essential in developing and designing an effective treatment regimen.
Traditionally, large FP volumes are managed via disposal into the subsurface through saltwater disposal wells (SWDs). This consists of transporting the waste fluid (i.e., trucking or pipelines) to a designed site, where the fluid is pumped and sequestered into deep geologic formations [37]. However, this practice comes with a series of environmental concerns. For example, spills during the transport of FP to disposal sites can lead to groundwater and surface water contamination. In 2017, a study modelled different spillage scenarios with varying soil types, spill intensities and depth of ground water, concluding that benzene and toluene—toxicity-inducing compounds—are the primary contaminants of concern [38]. Another study from 2019 reported an increase in bromide, radium, strontium, lithium and boron downstream from a spill site in comparison to upstream, which translated into a reduction in the growth of fish and the survival of mussels [39]. Additionally, spill events can vary the concentration of ions and increase the total dissolved solids (TDS) in nearby areas and natural water streams, respectively [40]. Overall, these are just a few examples of the various threats to environment associated with the disposal of FP. Another key aspect to consider is water management.
During the period from 2009 to 2017, a total of 11.43 billion barrels of water were used for HF in the US, with the Permian Basin increasing its water intake by 1.26 billion barrels since 2009. According to Scanlon et al., this represents 0.1% of the US water withdrawal in 2015 [41]. In 2017, Permian Basin reported an annual PW volume (106) of 1,663.21 barrels (bbl) as well as a water demand for HF of (106) 1,322.26 bbl. By 2017, the Permian Basin had an increment in PW volume approximately 20 times higher compared to 2011 [41,42]. In view of this, the Permian region is a prime candidate to substantially benefit from recycling PW, as it will reduce the demand of high volumes of fresh water, favoring the main urban centers Lubbock and Midland-Odessa, with a total population of 466,200 individuals (2010) [43]. In fact, far more FP is being produced than the required for HF, this could be a major opportunity for the agricultural sector. For instance, from 2000–2014, 91% of total water used in this area was destined for irrigation, followed by 6% for municipal use and 2% for industry and livestock [43]. Another significant concern for residents in shale regions is the increasing seismic events. Induced seismicity is a risk when injection is performed into deep bedrock formations, as it may lubricate pre-existing geological faults and provoke fault slips [44]. In 2020, Benson et al. concluded that extracting and injecting fluids affects the natural seismicity of a given area. Furthermore, subsurface injection has a particular association with earthquakes because it drives critically stressed faults to failure by increasing pore pressure [45]. In recent years, seismicity rates have increased 12-fold since 2008 in West Texas [46]. Moreover, documented cases of induced earthquakes have been observed in Canada, the United Kingdom, and China as well, with events of up to 5.7 on the Richter scale [47]. For these reasons, the state of New Mexico no longer grants permits for disposals as a preventative action that aims to decrease the occurrence of seismicity in the area. Nevertheless, seismologists have difficulties in determining exactly whether the earthquakes are naturally occurring, if they are caused by the hydraulic fracturing processes or if they result from post-injection of wastewater.
Taken as a whole, the potential treatment and reuse of FP for HF would significantly reduce the reliance on freshwater resource in shale energy regions, particularly in the Bakken and Permian Basins, thus alleviating water stress in nearby communities and retaining large volumes of water in the water cycle. Assuming that FP is treated to an appropriate standard, a growing number of applications are available, such as agricultural and surface water discharge, domestic usage and aquifer recharge. Ultimately, the frequency of injection-well-induced earthquakes could be greatly attenuated by the utilization of treated FP.
Current technologies applied in FP treatment include membrane and media filtration, chemical oxidation and thermal and ion exchange methods. Typical setbacks for these methods are membrane clogging, corrosion, high cost of chemicals, need of pre-treatment and post-treatment, and solid separation [4]. Utilizing novel technologies in the treatment of FP could reduce the negative impacts associated with SWDs, while making UOG operations more sustainable and offering potential ancillary economic opportunities. For example, one option for the industrial sector is the extraction of precious and semiprecious metals that are in high demand, such as cobalt, nickel and particularly lithium. The mining and extraction of precious metals found in FP represents a relatively unexplored opportunity for the energy sector. This article reviews the current state of produced water characterization techniques and treatment technologies. First, we discuss the efficacies of various treatment modalities commonly used to remediate FP, including established and emerging technologies, and how they are utilized to remove various classes of biogeochemical constituents found in FP. Secondarily, we cover the costs of treatment and the options for extracting metals from FP using Li extraction technologies and their associated costs as an example.

2. Challenges Associated with Produced Water Management

2.1. Technologies Utilized in Produced Water Treament

The major concern in treating FP for reuse, apart from the cost of treatment, is the removal of pertinent constituents (see Table 1) that can negatively affect the production of a given oil/gas well. For example, elevated levels Sr, Ca, Mg and Ba can contribute to the formation of insoluble scales in production tubing, which can attenuate production rates [48]. Elevated levels of sulfate can also contribute to scaling, as well as provide a substrate for sulfate-reducing bacteria (SRB) to proliferate. Ultimately, this could lead to the corrosion of tubing and, as a consequence, environmental contamination along with the clogging of the wellbore, the degradation of hydrocarbons and the souring of natural gas [16,17,25,32,49]. Additionally, significant concentrations of B and Fe (>10 mg/L) limit effectiveness of cross-linkers polymerization in fracturing fluid [16,50]. Lastly, elevated values of TOC, Na, Ca, Fe and phosphate reduce the viscosity of gel-based fracturing fluids [48], which can have negative implications for production well stimulation.
The biogeochemical complexity of produced water requires the implementation of multiple treatment modalities to effectively remove all the contaminants from microorganisms and heavy metals to organic particulates and NORMs. The most widely utilized procedures can be categorized as such: chemical oxidation, adsorption, membrane filtration, electrocoagulation and distillations:
  • Chemical oxidation facilitates the flocculation of volatile and semi-volatile organics, the precipitation of inorganic compounds, and the eradication of bacteria. Additionally, the use of oxidizing agents leads to the volatilization and remediation of undesirable odors and colors, respectively. The oxidizing agents most commonly used in FP treatment include ozone, hydrogen peroxide, chlorinated compounds and permanganate [4]. Advanced oxidation processes (AOPs) comprise a set of chemical treatments that remove organic matter by reaction and subsequent degradation with a hydroxyl (OH) group. Furthermore, AOPs are thought to be environmentally sustainable for chemical oxygen demand (COD) degradation [13]. Recent advances in this technology involve the addition of nanoparticles to enhance the removal of major organics from fracking wastewater [51].
Table
Table 1. Inorganic constituents and other parameters of fracturing waste waters from Bakken Shale and Permian Basin, the regulated concentration ranges for reuse in well stimulation [15] and in agricultural and consumption use [52,53]. * represents the reported average of three measurements in the study.
Table 1. Inorganic constituents and other parameters of fracturing waste waters from Bakken Shale and Permian Basin, the regulated concentration ranges for reuse in well stimulation [15] and in agricultural and consumption use [52,53]. * represents the reported average of three measurements in the study.
Bakken Shale Range
(mg/L) [13,40,54,55,56,57]		Permian Basin
Range
(mg/L) [6,58,59]		Well Stimulation
(mg/L) [15]		Agricultural Use
(mg/L)
(EPA)		Drinking Water
(mg/L)
(FAO & EPA)
METAL
Magnesium (Mg)1530–37901630–19502000
Iron (Fe)0.70–30.201110.005.000.30
Manganese (Mn)5.20–17.2011.00–53.00 0.200.05
Aluminium (Al)<LOQ–8.30 5.000.05–0.20
Calcium (Ca)13,140–41,16010,000–15,0002000
Sodium (Na)89,100–189,00048,000–54,000 69.00
Potassium (K)3510–9530570–1100
Barium (Ba)6.40–26.300.00–16.0020.00 2.00
Strontium (Sr)709–2450730.0–820.0
Cobalt (Co)0.030–0.20N/A 0.050
Nickel (Ni)<LOQ–3.800.020 0.200.07
Lithium (Li)34.50–89.7018.80 2.50
Chromium (Cr) 0.100.10
Radium 226 (Ra)527.1–1211 pCi/L 5.000 pCi/L
Uranium (U) 30.00 µg/L
Copper (Cu)4.60–16.90 0.201.00
Zinc (Zn)2.50–10.10 2.005.00
Arsenic (As) 1.1 0.100.01
Beryllium (Be) 0.100.004
Lead (Pb)0.00–3.50 5.000.015
Silver (Ag) 0.10
Molybdenum (Mo) 0.01
Cadmium (Cd)0.001–0.031 0.010.005
Vanadium (V)0.60–1.00 0.10
Thallium (Tl)0.00–0.20 0.002
Antimony (Sb) 0.006
Rubidium (Rb)0.30–12.90
Mercury (Hg) 0.002
NON-METAL
Chloride (Cl−)21,728–136,220111,000–138,00030,000–50,00092.00250.0
Bromide (Br−)91.6–5581370–1650
Silicon (Si) 3235.00
Fluoride (F−) 1.004.00
Boron (B)25.0–260.1 10.000.70
Selenium (Se)0.10–1.00 0.020.05
POLYATOMIC IONS
Sulfate SO42−)0.000–293.0515–743500 250
Bicarbonate (HCO3−)35.00–856.092–16030091.50
Nitrite (NO2−) 1.00
Nitrate (NO3−) 5.00010.00
Phosphate (PO43)584 *
Ammonium (NH4+)44.8–2520655
Cyanide (CN−) 0.200
OTHER PARAMETERS
pH4.1–7.27.306.0–8.06.5–8.46.5–8.5
TDS128,300–388,600174,213–212,984 450500
TSS7040 *6850–21,820500
Total nitrogen
TOC311 *86.25–184.21
Alkalinity (CaCO3)0–562.82345
Turbidity (NTU)1353.4
DOC80 *63.45–145.71
Conductivity (mS/cm) 201.2
Nonvolatile dissolved organic carbon (NVDOC)1.13–3.31
Total Hardness(mg/L CaCO3)31,000–59,000
Chemical Oxygen demand (COD)20,000–79,000
2.
Adsorption is applied for the sequestration of organics and metal contaminants. However, it is more of a polishing step for other preceding treatment modalities instead of being a sole separation technique on its own. It is important to note that the adsorption efficiency of various media is mediated by salinity. Activated carbon media are effective for organic contaminants, whereas, activated zeolite is an effective adsorbent for the removal of scaling ions such as Ca2+ and Mg2+ [60] that are generally present in elevated concentrations in FP (see Table 1). Other possible absorbents include alumina and organoclays [4]. In recent studies, Sun et al. achieved the removal of several metal pollutants; for instance, Cu(ll), As(V), Cr (Vl), Cr(ll) and Zn(ll) on Fe-impregnated biochar, a carbon-rich fine-grained pyrolysis residue [61].
3.
Membrane filtration consists of the separation of a fluid from dissolved substances by a porous surface. This includes reverse osmosis (RO), microfiltration (MF), nanofiltration (NF), ultrafiltration (UF) and forward osmosis (FO). RO removes solids by the application of hydraulic pressure to move water molecules through a semi-permeable membrane; MF allows the physical separation of suspended solids and turbidity depletion via the retention of particles larger than the micropores in the membranes. UF reduces odor, organic matter and color with pore membranes on the order of microns. NF offers selective particle rejection based on size and charge, which lessens multivalent ions, and FO lowers TDS in high-saline brines, benefiting from osmotic pressure and transporting water molecules through a semipermeable membrane from the less-concentrated feed to the highly concentrated solution [62]. Some modalities could be applied as treatment technologies on their own, such as MF and UF; others are steps in a more complex separation process. The obstacles to overcome include the membrane fooling/clogging due to interactions with VOCs in NF/RO, fouling caused by high Fe concentration in MF/UF, and scaling in RO [4,13,63,64] as well as RO’s limitation to ionic strengths lower than that of sea water (approx. 40,000 ppm) [65].
4.
Electrocoagulation (EC) promotes the precipitation of metals in the form of hydroxides by the addition of direct current through a metal electrode. This has been shown to be efficient and economically feasible for wastewater [66]. Previous studies have demonstrated high removals of turbidity, COD, oils and greases by EC. For example, Kausley et al. reported efficacy in the removal of total organic carbon (TOC) and scaling-causing ions, particularly Ca2+, Mg2+, CO32− and HCO3-, from synthetic PW and PW [66,67]. The precipitation of metal cations in the form of hydroxides could be further exploited to make the treatment of FP more economically viable to the industrial sector through the generation and commercialization of Cu2+, Mn2+, Zn2+, Al3+, Fe3+, Ni2+, Mg2+, Ca2+, Na+ and several other metal hydroxides. Moreover, HCl could be produced by hydrolysis of Cl2 gas generated during the process [67,68,69,70]. (Greater details will be discussed in subsequent sections of this review).
5.
Distillation is a thermal process in which solid particles are separated from liquid matrix by boiling point differences. One of the promising variations for brine desalination is multistage flash distillation (MSF). In MSF, the saline solution is converted into a vapor state and then goes through successive units in which the solution evaporates and condensates. In each unit, a fraction of the original feed remains as a highly concentrated brine (see Figure 1) [62]. The technique produces high-quality fresh water [71] and is efficient in the treatment of brackish/sea water. Nevertheless, for future applications in PW treatment, it is suggested to pretreat the inlet water with chemical softeners, filtrations and/or ion exchange technologies to avoid scaling and fouling, as well as to upgrade the infrastructure material to stainless steel to prevent corrosion [62]. The latter increases capital costs. Additionally, the salts produced by this treatment modality can serve as a feedstock for electrocatalytic processes to produce acids (HCl) and caustic agents (NaOH).
Many ongoing efforts for the treatment of FP incorporate separation and desalination [72]. Similarly, a common practice is the utilization of powdered activated carbon (PAC) for the depletion of dissolved organic carbon (DOC), turbidity and organic components. Other operations include softening hardness ions by the addition of caustic soda [54], demineralization through membrane distillation [73] and removal of organic components by coagulation followed by ultrafiltration [74]. Furthermore, biologically active membranes help remove organics and salinity [13]. The use of these techniques in tandem is generally required to remediate FP to a reusable and/or recyclable standard.
The commercial methods implemented in desalination of seawater, typically membrane-based and thermal-based [62], fail to meet the requirements for processing wastewater from UOG. However, the elevated values of TDS (>50,000) in FP can lead to difficult scenarios when treating the approximately 250 million barrels produced globally each day [75]. For example, the FP in the Permian Basin has TDS values three to five times higher when compared to those of seawater (see Table 1) [76]. Common challenges include corrosion, fouling and scaling of the membrane when precipitation conditions are met [77].
Forward osmosis allows the separation of water from dissolved solids by employing a semipermeable membrane and the difference in osmotic pressure as driving force. In contrast to RO, it is believed to be more appropriate for high-TDS matrices, such as FP [78]. Additionally, FO is a cost-competitive and reliable alternative for wastewater treatment [79] that exhibits great potential in removing heavy metal ions, including Cr2O72−, HAsO42−, Pb2+, Cd2+, Cu2+ and Hg2+ [80].
A previous study suggested that reusing PW in the energy sector is a better option than surface discharge due to safety concerns. Alternatively, its authors suggested thermal distillation (TD) as the appropriate treatment modality [42]. Regardless of being one of the most utilized operations for saline water recycling, TD’s energy consumption must be addressed when treating PW since scaling may lead to a to insulation of heat exchangers and, consequently, inefficient heat transfer. Again, the elevated price of anticorrosion materials to build this facility should be considered, since high costs affect the feasibility at an industrial scale. Similarly, osmotic properties constrain the application of membrane technologies in highly saline brines [62].
Recent advances in membrane technology, as well as integration of existing procedures, show promising results in processing high-TDS watersIn 2018, Sardari et al. demonstrated that electrocoagulation (EC) pre-treatment followed by direct contact membrane (DCMD) was effective in recovering up to 57% from a sample with a TDS of 135 g/L. However, they suggested a reduction in the sedimentation time for practical applications [81]. Furthermore, pretreatment with antiscalants such as 1-hydroxyethylidene-1,1-diphosphonic acid (HEDP) increased the performance of carbon-nanotube-immobilized membranes in membrane distillation (MD) [82]. Additionally, Ahmad et al. (2020) proposed a hybrid technology that incorporates assisted reverse osmosis (ARO), microfiltration and reverse osmosis—introduced as MF-ARO-RO—for which individual operations enhanced the ability to withstand different salinity effects and profiles. Although the addition of ARO to the MF-RO system represented an increase in the total cost, it was presented as the cheapest alternative for high-salinity FP [83].
Recent studies developed a combined membrane system consisting of an electrodialysis chamber followed by nanofiltration and membrane distillation (ED-NF-MD), represented in Figure 2. The system facilitated zero liquid discharge and allowed a water recovery of up to 99.8% with no need for chemical antiscalants [84]. Regardless of being a laboratory-scale experiment, the novel method has underlying potential in high-TDS waters treatment at industrial scale.
To summarize, the utilization of different adsorbents and novel materials to prevent scaling and corrosion, as well as the tandem use of existing commercially available technologies, can facilitate the effective treatment of FP. Enhancement in the performance of the more sophisticated methods can be achieved by pretreatment with the well-known membrane filtrations.

2.2. Costs Associated with Produced Water Treatment

As previously mentioned, the efficacy of FP treatment is inherently important when determining the terminal destination for the treated water. However, the more influential aspect of assessing the feasibility and sustainability of FP reuse and/or recycling is operational cost. The cost of deep-well injections ranges from approximately USD $0.25/bbl in private wells to approx. USD $0.50 to 2.50/bbl in commercial wells [85]. Adding the price of transportation to disposal sites (approx. USD $0.03/bbl/mile) may increase the cost significantly depending on the location of the storage [86]. In fact, transportation costs can range from USD $2.00–20.00/bbl [87]. Moreover, these values are expected to become higher due to distances of disposal sites possibly increasing. Additionally, permitting SWDs is becoming more contentious because of earthquake issues could increase costs. On the other hand, FP can also be transported via pipeline at an approximate cost of USD $0.25/bbl (personal correspondence with water treatment provider), yet this requires considerable infrastructure that is generally not established in most shale energy basins. Typical treatment costs range from USD $3.00 to $30.00/bbl, including storage and transport [88]. Recently, MD modalities were studied for reuse waste waters of HF operations, resulting in costs ranging from USD $0.11 to $0.90/bbl of treated fluid [89]. Operational costs of RO and FO typically stand at USD ~$1.00/bbl. Providing an initial cost for the acquisition of these membranes is challenging due to their performance dependency on influent TDS levels and throughput requirements. In Table 2, the annual cost for FP disposal in Permian and Bakken is compared to treatment costs, assuming treatment take place in situ based on mobile treatment modalities.

3. Opportunities in Produced Water Management

3.1. Technologies/Processes, and Their Respective Costs, Used to Extract Precious Metals

The recovery of elements with added values (Li, K, Sr, Mg, Mn, etc.) from FP represent a great advantage for the energy sector. The rapidly increasing demand for precious metals such as Li is challenging, however, as the reservoirs of Li are limited worldwide. Various industries, including batteries, pharmaceuticals and ceramics, need Li for their operations [54]. Global efforts are pursuing the acquisition of Li from seawater [90,91], although compared to FP, the concentration in seawater is orders of magnitudes lower. Alternatively, several other metals and critical minerals are also found in FP, including Co and Ni (refer to Table 1), which are also relevant for the manufacturing of batteries. Based on the annual production of FP in the Bakken and Permian Basin Region, a comparison in the economics of extractable metals is provided in Table 3.
Previous studies involved the nano-sized zerovalent iron (n-ZVI) catalytic oxidation and adsorption for the recovery of elements such as Sr, Mg, Na, Al, Ca, K and P, as well as the degradation of organic matter in FP. The cost associated with these operations is approximately USD 1355.80 per barrel per hour [51]. In other studies, the analysis of the costs for FP desalination in the Marcellus Shale applying direct contact membrane distillation (DCMD) resulted in USD $35.87/bbl. Moreover, there is opportunity to decrease the costs to as low as USD $4.66/bbl of water fed if the waste heat is recycled into the treatment [92]. Additionally, Zendejas et al. compared chemical coagulation and electrocoagulation for the treatment of FP for reuse in the Permian Basin, estimating costs of USD $2.33/bbl and $2.77/bbl of treated water (Zendejas et al., 2020). Lastly, a combined osmosis system consisting of FO, RO and NF presented a total water management cost of USD $2.32/bbl of pit water [86].
Table
Table 3. Quantities and values of extractable metals from Permian Basin and Bakken.
Table 3. Quantities and values of extractable metals from Permian Basin and Bakken.
ElementIndustry/Terminal UsesPrice (USD/kg) [93]Total Extractable Mass in FP, kg (Bakken) *Value of Extractable Metals in Millions, M
(Bakken)		Total Extractable Mass in FP, kg (Permian) *Value of Extractable Metals in Millions, M
(Permian)
NaSodium salts production$2.57–3.437.59 ×109$22,776.391.35 × 1010$40,453.20
LiBatteries$81.40–85.603.39 × 106$283.124.97 × 106$415.06
KFertilizer/saltproduction$12.10–13.603.56 × 108$4574.502.21 × 108$2836.95
SrFirework$6.50–6.708.62 × 107$569.012.05 × 108$1352.41
CaCement fabrication/reducing agent$2.21–2.351.48 × 109$3379.853.31 × 109$7535.40
MgAlloying agent$2.30 1.45 × 108$334.044.73 × 108$1088.53
MnSteel making$1.806.12 × 105$1.108.46 × 106$15.23
CoBatteries$32.8 6.28 × 103$0.210$0.00
NiBatteries $13.901.04 × 105$1.445.29 × 103$0.07
BGlass and ceramics$3.687.78 × 106$28.630$0.00
* Calculations based on amount of FP generated per annum (54.6 × 109 L for Bakken and 264.4 × 109 L for Permian) multiplied by the average ion concentration, as illustrated in Table 1.
The feasibility of mining precious metals relies on: (1) the location of the play; (2) the cost of the treatment modality; (3) the market price of the element. In particular, the Permian Basin has levels of K of 1100 mg/L (see Table 1), and the combined osmosis system has a cost of USD $2.32/bbl. The recovery of 1 kg of K would require the treatment of approximately 5.72 bbl of FP (USD $13.34); as shown in Table 3, the market price for K is USD ~$12.10/kg, which shows that it is not economically viable to extract K from the Permian region. Similarly, the expenditures for the acquisition of Li and Sr are USD $776.27 and $17.80, respectively. Meanwhile, the cost of K extraction in Bakken utilizing the previous analogy is USD $1.53 for 1 kg of K, which could be further sold for USD $12.10, producing a significant profit margin. The cost of recovery of Sr in Bakken is approximately USD $5.96, which also makes it viable. Additional costs involving possible purification steps should be considered. According to the USGS National Mineral Information Center, the domestic production of salt satisfies 85.11% of the reported salt consumption in the US (excluding Puerto Rico) [94]. The estimated extractable value for sodium chloride in the Permian Basin alone represents approximately 73% of the salt demand in 2021. Other outlets for these byproducts are to be explored.
The challenges associated with treating FP, along with the variety of modalities available for this purpose, steer the efforts into a combined technologies approach as shown in Figure 3. This FP valorization process integrates: (1) an oxidation step; (2) chemical coagulation/precipitation; (3) filtration; (4) a membrane system; (5) electrocoagulation. The first three steps achieve the removal of microorganisms and part of the organic matter found in FP. The membrane system target the ions, and the EC polishes the metal for its recovery. The utilization of embedded membranes aids in the removal of persistent ions such as B. The resulting treated water could be used for crop irrigation or to replenish natural sources, or it could be recycled in UOG operations depending on the attained parameters and the requirements set by FAO, EPA or the oil and gas industry.

3.2. Feasibility of Extracting Precious Metals in Certain Shale Energy Basins

The U.S. Geological Survey (USGS) is a national agency that collects data of natural resource conditions. The USGS provides a database with information about the abundance of certain elements typically present in FP, their origin and other bulk parameters [95]. According to the database, metals like Na, K, Mg, Ca and Sr are common in most shales at elevated concentrations. However, there is limited information about ions with more industrial relevance, such as Co, Ni and Li. More studies are needed in the characterization of FP to establish a better foundation when dabbling into this field. The feasibility of metal extraction relies on a minimum threshold of ion concentration. In Table 4, these values are shown for certain elements along with viable locations for their extraction. The threshold calculations are based on the concentrations reported for Permian Basin (refer to Table 1) and a treatment cost of USD $2.32 per bbl of FP.
As previously mentioned, the interest in finding alternative sources of lithium has triggered a race in the study of various technologies for Li extraction from brines. As shown in Figure 4, these techniques range from typical solvent extractions to novel chemically modified surfaces for adsorption.
The conventional solar evaporation method is a very cost-effective procedure; however, the extensive land area required hinders its application, as does the limited selectivity for a particular ion of interest. Whilst solvent extraction and phosphate precipitation facilitate the recovery of lithium, the environmental concerns, costs and coprecipitation steer the industrial efforts toward less polluting options. Some adsorptive materials containing aluminum and titanium each offered promising results for Li extraction. However, the dependence on pH must be overcome, as must the challenges in the desorption mechanism of Li from the Al surface and the competition of cations on titanium-based adsorbents [96]. As for manganese based materials, the conversion from laboratory- to industrial-scale and the limited understanding of the adsorption/desorption process represent a challenge [97]. Nanofiltration and ion exchange technologies have been utilized in industrial scenarios for the removal of ions with great results. Nevertheless, metal extraction requires a combination of resins at different stages if not targeted to a particular metal. Additionally, matrices such as FP require further separation processes, compromising the feasibility on an industrial scale. Recently, encouraging results proposed a highly selective polymer for the efficient extraction of lithium in presence of other ions, such as Na and K. More importantly, Li can be easily released by increasing temperature; this is particularly interesting for possible industrial applications [98].
Energies 15 04619 g004 550
Figure 4. Available technologies for extracting Li from brines. Description of the mechanism of extraction for Li of the several commercial technologies and their developers [99].
Figure 4. Available technologies for extracting Li from brines. Description of the mechanism of extraction for Li of the several commercial technologies and their developers [99].
Energies 15 04619 g004
The “E3 Metals Corp” agency operates within the Leduc Formation in Alberta, Canada. They are able to recover >90% of Li from oilfield brines with Li concentrations of 74.6 mg/L in the form of hydrated lithium hydroxide (LiOH∙H2O), with an annual production capacity of 20,000 mt. The reported capital expenditure (CapEx) for this infrastructure is USD $602,000 MM, and the operation expenditure (OpEx) is USD $73,200 MM [100]. The magnitude of the initial investment for the construction of a similar structure in the United States frustrates the acquisition of these treatment sites in the shales. As a possible solution, a centralized facility should be considered to which the FP from the regional shales could be transported and treated via pipelines or trucks, resulting in a minimized economic impact that this strenuous investment may cause to the UOG industry.

4. Conclusions

The reuse of treated FP will relieve the water stress caused by HF in arid regions such as the Permian Basin. Due to more FP being produced than is required for injection, recycling in agriculture is an attractive option for this excess, as most of the water consumption in the Permian region is dedicated to irrigation. Remaining challenges in FP sanitation include the complete characterization of FP, the high cost of the materials used to build facilities and the lack of methods for removing difficult ions such as boron. Whilst a variety of technologies are available for the treatment of highly saline brines, the appropriate strategy should be a combination of sequential steps. Although promising a sustainable solution, the high CapEx associated with the development of a facility with these requirements is not economically favorable. The intensive capital cost of such investment demands joint efforts from the involved industries for the construction of a centralized treatment facility that facilitates the purification of water as well as the extraction of these valuable metals (Figure 4). The recuperation of Li is possible in Permian, Palo Duro, the Gulf Coast, Williston, Appalachia and many other regions, as is the recovery of Sr, Ca, Mg, Na and K. In this sense, based on the numerous studies available and the growing demand by the energy sector, lithium should be the candidate for the development of this pilot strategy. A drawback to treating FP down to reuse standards is the generation of extremely salty brines/sludge. Although found in low concentrations in the Permian Basin, the accumulation of radionuclides in these brines can generate low-level nuclear waste. Furthermore, assuming all the produced water is treated in both Bakken and Permian Basin, the sum of extractable salt will represent approximately 116% of the domestic consumption in 2021 with these plays alone (USGS, 2022). Other outlets for these surplus materials have yet to be explored.

Author Contributions

Conceptualization, Z.L.H. methodology, R.S.-R.; software, R.S.-R.; validation, R.S.-R. and Z.L.H.; formal analysis, R.S.-R.; investigation, R.S.-R.; resources, R.S.-R.; data curation, R.S.-R.; writing—original draft preparation, R.S.-R.; writing—review and editing, Z.L.H.; visualization, R.S.-R.; supervision, Z.L.H.; project administration, Z.L.H. All authors have read and agreed to the published version of the manuscript.

Funding

This research received no external funding.

Acknowledgments

We wish to thank Mark Engle for his time and consideration critiquing this review.

Conflicts of Interest

The authors declare no conflict of interest.

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Figure 1. Schematics for multistage flash distillation (MSF). Extracted from Panagopoulos et al., 2019 [62].
Figure 1. Schematics for multistage flash distillation (MSF). Extracted from Panagopoulos et al., 2019 [62].
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Figure 2. Diagram of the integrated ED-NF-MD system. CM: cation exchange membrane; AM: anion exchange membrane; ED: electrodialysis; NF: nanofiltration; VMD: vacuum membrane distillation. Reproduced with permission from Zhao et al., 2020 [84].
Figure 2. Diagram of the integrated ED-NF-MD system. CM: cation exchange membrane; AM: anion exchange membrane; ED: electrodialysis; NF: nanofiltration; VMD: vacuum membrane distillation. Reproduced with permission from Zhao et al., 2020 [84].
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Figure 3. Schematic of the valorization process for FP. Step-by-step methodologies are applied to extract precious metals from FP, adding an aggregated value to this waste.
Figure 3. Schematic of the valorization process for FP. Step-by-step methodologies are applied to extract precious metals from FP, adding an aggregated value to this waste.
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Table
Table 2. Annual cost for disposal and treatment of FP in Permian Basin and Bakken Shale, assuming both are performed on-site. * Based on USD $0.03/bbl/mile trucking cost and an average distance of 20 miles from the source to the nearest disposal site.
Table 2. Annual cost for disposal and treatment of FP in Permian Basin and Bakken Shale, assuming both are performed on-site. * Based on USD $0.03/bbl/mile trucking cost and an average distance of 20 miles from the source to the nearest disposal site.
UnitBakken RegionPermian RegionReference
Saltwater Disposal (SWD) cost
Disposal volumebbl/year3.43 × 1081.6 × 109[41,42]
Transportation Cost *USD/bbl$0.60$0.60[86]
Well Injection CostUSD/bbl$0.5$0.5[43]
Well disposal CostUSD/year$171,730,000$831,605,000
Water management Cost—Scenario 1USD/year$377.30 M$1.76 B
Treatment and reuse
Chemical oxidationUSD/bbl$0.20$0.20(Correspondence w/water treatment company)
Chemical precipitation & nanofiltrationUSD/bbl$0.24$0.24(Correspondence w/water treatment company)
Water management Cost—Scenario 2USD/year$150.92 M$704.00 M
Table
Table 4. Metal thresholds and abundance. Minimum concentration of metals required for feasible extractions and their abundance. Calculations are based on treatment costs of USD 2.32/bbl, further isolation processes not included.
Table 4. Metal thresholds and abundance. Minimum concentration of metals required for feasible extractions and their abundance. Calculations are based on treatment costs of USD 2.32/bbl, further isolation processes not included.
MetalMinimum Concentration (mg/L)FormationBasinState
Na5678.58Multiple
Ca6603.60Multiple
Mg6345.20Multiple
K1206.11Multiple
Li179.29Marcellus ShAppalachianPA
Helderberg Ls
Cambrian
Oriskany Ss
Onondaga Ls
DakotaPowder RiverWyoming
Parkman
SmackoverGulf coastArkansas
Smackover limeArkla
MississippianLas Animas ArchColorado
SmackoverGulf CoastMississippi
RatcliffeWillistonMontana
Dwyer Charles
Duperow
UnknownPermianNew Mexico
Oriskany SsAppalachianNew York
MadisonWillistonNorth Dakota
DuperowWilliston
Grenora CharlesWilliston
Madison CharlesWilliston
RivalWilliston
Devonian DuperowWilliston
CanyonPermianTexas
SmackoverEast Texas
UnknownAmarillo Arch
UnknownPalo Duro
UnknownAnadarko
EdwardsGulf coast
MioceneGulf coast
Sr2245.22Multiple
Mn8107.75N/A
Co444.94N/A
Ni1050.59N/A
B3965.75N/A
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Sanchez-Rosario, R.; Hildenbrand, Z.L. Produced Water Treatment and Valorization: A Techno-Economical Review. Energies 2022, 15, 4619. https://doi.org/10.3390/en15134619

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Sanchez-Rosario R, Hildenbrand ZL. Produced Water Treatment and Valorization: A Techno-Economical Review. Energies. 2022; 15(13):4619. https://doi.org/10.3390/en15134619

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Sanchez-Rosario, Ramon, and Zacariah L. Hildenbrand. 2022. "Produced Water Treatment and Valorization: A Techno-Economical Review" Energies 15, no. 13: 4619. https://doi.org/10.3390/en15134619

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