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Review

Cite This: Environ. Sci. Technol. Lett. 2018, 5, 467−475 pubs.acs.org/journal/estlcu

High-Pressure Reverse Osmosis for Energy-Efficient Hypersaline

Brine Desalination: Current Status, Design Considerations, and
Research Needs
Douglas M. Davenport, Akshay Deshmukh, Jay R. Werber, and Menachem Elimelech*
Department of Chemical and Environmental Engineering, Yale University, New Haven, Connecticut 06520-8286, United States
*
S Supporting Information
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ABSTRACT: Water scarcity, expected to become more widespread in the

coming years, demands renewed attention to freshwater protection and
management. Critical to this effort are the minimization of freshwater
withdrawals and elimination of wastewater discharge, both of which can be
achieved via zero liquid discharge (ZLD), an aggressive wastewater management
Downloaded via 95.154.221.91 on October 2, 2021 at 12:30:28 (UTC).

approach. Because of the high energetic cost of thermal desalination, ZLD is

particularly challenging for high-salinity wastewaters. In this review, we discuss
the potential of high-pressure reverse osmosis (HPRO) (i.e., reverse osmosis
operated at a hydraulic pressure greater than ∼100 bar) to efficiently desalinate
hypersaline brines. We first discuss the inherent energy efficiency of membrane processes compared to that of conventional
thermal processes for brine desalination. We then highlight the opportunity of HPRO to reduce energy requirements for
desalination of key high-salinity industrial wastewaters. The current state of membrane materials and processes for hypersaline
brine desalination is also discussed, emphasizing several process design considerations unique to HPRO. Lastly, we discuss the
most pressing research needs for the development of HPRO, notably the development of membranes and modules suitable for
high pressures as well as fundamental studies of compaction and transport under HPRO conditions.

■ INTRODUCTION
Recent estimates suggest 1.2 billion people live in areas of
physical water scarcity.1 Effective water resource management
is critical to ensure the widespread availability of freshwater in
the coming decades.2 Two specific concerns are the treatment
and disposal of wastewater and the utilization of previously
untapped water sources. Management of wastewater from
industrial sources is particularly challenging as it can be highly
saline, vary temporally in volume and composition, and contain
complex mixtures of contaminant species.3 The beneficial reuse
of industrial wastewaters mitigates unsafe disposal by
eliminating wastewater discharge, while simultaneously de-
creasing freshwater withdrawals.4,5 A major challenge for the
reuse of high-salinity wastewaters, however, is the high
energetic cost of brine desalination.6 In the case of inland
desalination, brine disposal costs often render the desalination
of brackish groundwater economically unfeasible.7 Low-cost
brine management is critically needed to enable the utilization
of inland brackish groundwater and prevent the unsafe
discharge of saline industrial wastewaters.
Because of the energy requirements for high-salinity
wastewater desalination, the preferred brine management
option, when it is both safe and effective to do so, is to
dispose or reuse the waste stream without extensive treatment.
For example, brine solutions (also called the retentate or
reject) produced from seawater reverse osmosis (SWRO)
processes can be safely discharged to the ocean without
extensive treatment.8 In the oil and gas industry, produced
water undergoes relatively moderate treatment via dissolved air
flotation, chemical precipitation, or advanced oxidation to
remove oil and grease and reduce organic content.9 Produced
water treated in this fashion is often discharged to the ocean at
offshore locations, albeit with some environmental concerns.10
At inland sites, treated produced water can be reused in
hydraulic fracturing fluid.9,11
When safe discharge or reuse is not possible, brines are
commonly disposed of via deep well injection or treated using
evaporation ponds prior to the disposal of solids in
landfills.9,11−13 These processes, however, have serious
environmental limitations. For instance, some geologic
formations, such as those surrounding the Marcellus shale
fields in the United States, are unsuitable for wastewater
disposal via deep well injection because of the high potential to
contaminate groundwater.14 Furthermore, deep well injection
has been linked to groundwater contamination in other areas
as well as increased seismic activity.13 Volume minimization
using evaporation ponds is similarly problematic as it poses a
threat to groundwater and birdlife, requires large areas of land,
and is effective in only warm, arid climates.15,16 The challenges
associated with brine management often result in exorbitant
disposal costs, which can even lead to otherwise promising
brackish water resources remaining untapped as sources for
potable water.7 To avoid expensive brine disposal, an
Received: May 26, 2018
Revised: June 22, 2018
Accepted: June 29, 2018
Published: June 29, 2018

© 2018 American Chemical Society 467 DOI: 10.1021/acs.estlett.8b00274

Environ. Sci. Technol. Lett. 2018, 5, 467−475
Environmental Science & Technology Letters
increasing level of attention is being given to brine
concentration and zero liquid discharge (ZLD) practices, in
which waste is disposed of in solid form.17
A critical step in the ZLD process chain is desalination,
wherein water is recovered from a saline waste stream.
Desalination can be achieved by membrane-based processes,
such as reverse osmosis (RO) and electrodialysis, or phase-
change-based (designated here as “thermal”) processes,
including multi-effect distillation (MED), multi-stage flash
(MSF), and mechanical vapor compression (MVC).18 RO
utilizes hydraulic pressure, in excess of solution osmotic
pressure, to drive the transport of water across a semi-
permeable membrane while retaining most solutes.19 A
combination of membrane and thermal processes are often
used to achieve ZLD for saline wastewaters.20 First, RO
concentrates wastewater to approximately 70000 mg L−1 total
dissolved solids (TDS), which has an osmotic pressure, π, of
∼59 bar. At higher salinities, thermal technologies are used to
concentrate brine streams to approximately 250000 mg L−1 (π
≈ 290 bar), the typical inlet concentration for crystallizers in
ZLD.17 Thermal-based brine crystallizers then concentrate the
waste stream above its solubility limit (e.g., 357000 mg L−1 for
NaCl) to extract solid salts for disposal.17
Because of its superior energy efficiency, RO has displaced
thermal processes in recent decades for the major applications
of seawater and brackish water desalination for drinking water
production.21 As such, membrane materials and processes have
been optimized to treat feedwaters with salinities equal to or
less than that of seawater (typically ∼35000 mg L−1; π ≈ 28
bar). Consequently, the maximum operating pressure for RO is
typically around 80 bar,22 suitable for overcoming the retentate
osmotic pressure of seawater treated to 50% recovery (∼70000
mg L−1; π ≈ 59 bar). Because of hydraulic-pressure limitations
of RO, hypersaline brines, here defined as solutions with a
TDS concentration of >70000 mg L −1, are primarily
desalinated via thermal processes.17 These processes, however,
are energy- and cost-intensive, which limits the implementa-
tion of brine wastewater desalination prior to disposal.
In this review, we critically discuss the application of high-
pressure RO (HPRO), defined here as RO operating above
∼100 bar, to the treatment of hypersaline brines. We start by
considering the large volumes of industrial brines that could
require desalination and the energy requirements of HPRO
versus other processes. We largely consider two pressure limits
for HPRO: (i) 150 bar as roughly double the current operating
limit and (ii) 300 bar to enable retentate concentrations of
250000 mg L−1, the inlet concentration for brine crystallizers.
We then discuss the current state of HPRO and the process
design requirements for its effective application. We conclude
with a discussion of the research needs that must be addressed
to enable viable HPRO processes.
■
ENERGY EFFICIENCY OF MEMBRANE
DESALINATION
Desalinating highly saline waste streams is inherently energy-
intensive. The minimum specific energy consumption
(SECmin) of desalination (i.e., the energy required by a
thermodynamically reversible process per unit volume of
product water) depends on the salinity of the feed stream, cF,
and the water recovery ratio, R, the proportion of water
recovered from the feed stream:23,24
468
Review
RĜ (c P) + (1 − R )Ĝ (c R ) − Ĝ (c F)
SECmin =
R (1)
where Ĝ is the specific Gibbs free energy as a function of
composition at a fixed temperature and a fixed pressure and cP
and cR are the solute concentrations in the product and
retentate streams, respectively. Assuming complete solute
rejection, cP = 0 and cR = cF/(1 − R). Because of its salinity
dependence, SECmin is high for hypersaline brines (5.3 kWh
m−3 for 125000 mg L−1 at 50% recovery) as compared to those
of more dilute solutions (1.1 kWh m−3 for 35000 mg L−1 at
50% recovery). In addition, the desalination energy efficiency,
η, is defined as the useful specific desalination work performed
by the system (i.e., SECmin) divided by its specific energy
consumption (SEC): η = SECmin/SEC.
Membrane-based desalination processes such as RO and
electrodialysis, which do not require a phase change to separate
water from dissolved solutes, can achieve energy efficiencies of
>40%, particularly with multi-stage systems.24−26 In contrast,
phase-change-based or thermal desalination processes, such as
MED, MSF, and MVC, are inherently less efficient, with typical
η values of <20%.24,27 The energetic performance of thermal
processes is strongly dependent on the recovery of the latent
heat of vaporization, ΔvH. Given that ΔvH, >630 kWh m−3 for
saline waters, is two orders of magnitude larger than the typical
SECmin, imperfect heat recovery severely limits the energy
efficiency of all thermal desalination processes.27
To directly compare membrane-based and thermal-based
desalination (Figure 1A), we can quantitatively analyze the
energetics of relevant processes. Typical SEC values and feed
concentrations are shown in Figure 1B for conventional
(largely thermal) desalination technologies,17,27 in addition to
SEC calculated for HPRO. The SEC of HPRO is modeled
assuming a terminal hydraulic pressure (ΔPt) that is 5 bar
above the osmotic pressure of the retentate (πR).26,28,29 More
detailed insights can be gained by modeling different processes
for the same inlet and outlet streams. In particular, a feed
solution of 70000 mg L−1 NaCl is concentrated to 250000 mg
L−1 via HPRO-based, MVC-based, and hybrid HPRO−MVC
desalination systems (Figure 1A). MVC is chosen as a
representative thermal process because of its highly effective
heat recovery. Its SEC is calculated assuming isentropic (i.e.,
adiabatic and reversible) vapor compression with a terminal
temperature difference (ΔTt) of 5 °C above the boiling point
elevation of the retentate (δR).24,30,31 In the two-stage HPRO
and MVC models, water recovery in each stage is optimized to
minimize SEC. In the hybrid HPRO−MVC model, the HPRO
stage is limited to a maximum hydraulic pressure of 150 bar.
Further details of SEC calculations are given in the Supporting
Information.
Panels C and D of Figure 1 show the SEC and energy
efficiency of each process, which illustrates the drastic 3-fold
energy savings made possible using HPRO rather than a
thermal desalination process such as MVC. For example,
concentration of a 70000 mg L−1 hypersaline feed to 250000
mg L−1 would require 24 kWh m−3 with two-stage MVC (15%
energy efficiency) and only 7.3 kWh m−3 (47% energy
efficiency) with two-stage HPRO. For context, the RO stage
in a typical SWRO process can operate as low as 1.8 kWh m−3
(59% energy efficiency).25 Achieving a retentate concentration
of 250000 mg L−1 with HPRO would require approximately
300 bar of hydraulic pressure, a challenging target from
membrane materials and module design perspectives. For this
DOI: 10.1021/acs.estlett.8b00274
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Environmental Science & Technology Letters Review

Figure 1. (A) Brine desalination process schematics. Three different process configurations are shown for the concentration of a 70 g L−1 NaCl
solution to 250 g L−1. (B) Specific energy consumption (SEC) of various desalination processes. The typical feed concentration range and energy
consumption are shown for conventional RO and thermal brine concentrators.17,27 The expected SEC calculated for high-pressure reverse osmosis
(HPRO), at pressures of ≤150 and ≤300 bar, is also shown. (C) Specific energy consumption and (D) energy efficiency for HPRO and mechanical
vapor compression (MVC) brine desalination processes. The energy consumption requirements of five membrane-based and thermal-based
process configurations are analyzed for the desalination of 70 g L−1 NaCl at increasing retentate concentrations (i.e., water recovery). The energy
efficiency, η, is the ratio of the minimum energy of desalination for a given brine salinity and recovery, SECmin, to the SEC for each process. Shown
here are one- and two-stage processes for both HPRO and MVC. A hybrid HPRO−MVC process is also shown where an HPRO stage is employed
at a maximum applied pressure of ≤150 bar followed by an MVC stage. The water recovery ratio of each stage is optimized to reduce specific
energy consumption for each two-stage process. Further details about the calculations are provided in the Supporting Information.

reason, a hybrid process is modeled in which HPRO is limited
to a maximum pressure of 150 bar, after which the retentate is
further concentrated by MVC. At a retentate concentration of
250000 mg L−1, the hybrid process SEC is 12 kWh m−3,
representing a 2-fold reduction compared to that of two-stage
MVC. Below a retentate osmotic pressure of 150 bar, the SEC
of the hybrid HPRO−MVC process is identical to the SEC of
one-stage HPRO, as the optimal water recovery ratio of its first
stage (HPRO) is almost equal to its final recovery. As the
retentate osmotic pressure increases beyond 150 bar, the water
recovery of the second stage (MVC) begins to increase,
leading to an increase in SEC. It is important to note that the
HPRO−MVC hybrid is a two-stage process and thus the brine
flow rate entering the less efficient MVC stage is significantly
lower than the initial flow rate (approximately 50% lower for
the conditions modeled). Consequently, the energetic
performance of the hybrid HPRO−MVC process should be
assessed relative to two-stage HPRO and two-stage MVC,
rather than one-stage HPRO.
regulations. In many circumstances, regulatory, financial, and
environmental restrictions motivate brine concentration and
volume reduction.17 The coal-to-chemicals industry in China,
for example, requires ZLD for all new facilities.32 Additionally,
the financial cost of brine disposal from inland desalination
facilities motivates brine volume minimization.7 In addition,
strict disposal regulations for landfill leachate in the United
States and effluent from the textile industry in India necessitate
brine volume reduction to minimize environmental impacts
and health risks, despite the financial and energetic cost of
brine desalination.33,34
Figure 2A shows the global desalination capacity that is
currently installed or under construction for brine feedwaters
with a salinity of ≥50000 mg L−1 TDS.35 At present, these
brine desalination processes utilize conventional thermal
separation processes (e.g., MVC, MED, or MSF) or conven-
tional RO.35 Of the nearly 16000 desalination plants online or
under construction in the GWI/IDA Desalting Inventory, only
110 treat brine feedwaters.35 In practice, the high cost of brine

■
POTENTIAL IMPACT OF HPRO
A variety of industrial sources generate hypersaline brine
wastewaters. Table 1 shows several brines of particular concern
because of their large volume, concentration, or strict disposal
469
desalination limits hypersaline wastewater desalination before
disposal. Therefore, the total volume of hypersaline wastewater
present in each industry is surely much greater. In the United
States, the Environmental Protection Agency cites the high
financial cost of brine desalination as the reason it does not
require evaporative brine concentration of flue gas desulfuriza-
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Environ. Sci. Technol. Lett. 2018, 5, 467−475
Environmental Science & Technology Letters Review

Table 1. Characteristics of Significant Brine Sources, Current Practices, and Disposal Regulations
representative flow typical TDS
brine wastewater rate (mg L−1) current disposal practice regulations regarding disposal
oil and gas produced water United States:11 13000−2100009 offshore: direct ocean discharge11 United States: regulations vary region-
8.7 million m3 day−1 onshore: deep well injection (where possible), ally based on permits9,11
reuse for hydraulic fracturing, evaporation Pennsylvania: discharge monthly
ponds9,11 average TDS of <500 mg L−173

brackish groundwater desali- United States:35,56 5000−5500056 surface or sewer discharge, United States: regulations vary region-
nation retentate 1.6 million m3 day−1 deep well injection (where possible)74 ally based on permits74

flue gas desulfurization United States:36 16000−5000036,75 settling ponds, chemical precipitation and United States: monthly average TDS of
(FGD) wastewater 1.2 million m3 day−1 surface discharge, zero liquid discharge36,76 <24 mg L−1 (effective starting No-
vember 2020)77,78

landfill leachate United States:79 0−5000079 zero liquid discharge via land application or United States: strict discharge regula-
230000 m3 day−1 recirculation to the landfill79 tions on 9 to 14 parameters not
including TDS33

coal-to-chemicals wastewater China:32 2000−1600017 zero liquid discharge32 China: zero liquid discharge required
320000 m3 day−1 for new plants17,32

textile industry wastewater estimates not available 1500−3000080 zero liquid discharge81 or chemical and India: TDS of <2100 mg L−1 for inland
biological treatment prior to surface discharge82 discharge34

Figure 2. (A) Global installed desalination capacity for brine feedwaters with total dissolved solids (TDS) concentrations of ≥50000 mg L−1.35 For
each industry, hollow bars represent the capacity desalinated by membrane-based processes and solid bars the brine capacity desalinated by thermal
processes. (B) Energy consumption of brine desalination. The left-most portion of the figure shows the daily energy consumption required to
desalinate the total quantity of brine wastewaters currently treated in each industry. The right-most portion of the figure shows a hypothetical
scenario in which the total volume of each saline wastewater presented in Table 1 must be concentrated to 250000 mg L−1 prior to disposal. In each
case, the energy consumption shown is that to concentrate the saline wastewaters to 70000 mg L−1 using a two-stage RO system followed by either
a two-stage HPRO or two-stage MVC process to concentrate the brine to 250000 mg L−1. Hollow bars represent the HPRO process scheme and
solid bars MVC. The corresponding percentage of the daily U.S. national electricity generation (NEG) is also shown.37 Additional calculation
details are provided in the Supporting Information.

tion (FGD) wastewater.36 If cost-effective technologies were
available, it is possible regulations would require brine
desalination prior to disposal.
At present, thermal technologies account for 54% of the
global brine desalination capacity.35 The remaining 46% is
treated using RO, but information about water recoveries and
operating pressures is unavailable. To understand the energetic
cost of treating these waste streams, we estimated the energy
(Figure 2B) needed to concentrate the total quantity of brine
wastewaters currently desalinated in each industry to 250000
mg L−1 (initial volumes and concentrations are provided in
Table S1). In these calculations, two-stage RO concentrates
wastewater up to 70000 mg L−1 followed by two-stage HPRO
or two-stage MVC. The energy required to desalinate each
stream is shown alongside the proportion this represents of the
average daily U.S. national electricity generation (NEG).37 In
each scenario, MVC would require approximately 2−3 times
more energy than HPRO. In the power industry, for example,
470
approximately 1 million kWh day−1 (the equivalent of ∼34000
U.S. homes)37 would be saved using HPRO as compared to
MVC.
Because of the lack of widespread brine desalination, a
hypothetical scenario (Figure 2B) is imagined to estimate the
potential energy savings of HPRO compared to MVC for each
wastewater in Table 1. In this scenario, regulations require all
saline wastewaters to be concentrated to 250000 mg L−1 prior
to disposal (i.e., approaching ZLD). The potential energy
savings are most notable for large-volume applications like
produced water, where MVC would require 130 million kWh
day−1, representing 1.2% of the daily U.S. NEG.37 In contrast,
HPRO would utilize 85 million kWh day−1 less than MVC,
albeit still requiring 0.4% of the daily U.S. NEG. 37
Consequently, despite HPRO being 2−3-fold more efficient
than MVC, its high thermodynamic minimum energy will
mean considerable quantities of energy would be required for
HPRO. As such, work should be done to model the financial
DOI: 10.1021/acs.estlett.8b00274
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Environmental Science & Technology Letters
costs and human health and environmental impacts of
hypersaline wastewater management38 to identify applications
best suited for HPRO.
■ CURRENT STATE OF MEMBRANE BRINE
DESALINATION
A few commercially available membranes rated above 80 bar
currently exist. Most notable is the Pall Disc Tube (DT)
Module System, which has been used for landfill leachate
treatment.39 DT modules are plate-and-frame configuration
with large feed channels designed to reduce fouling from highly
contaminated leachate streams. As a result, they have a small
active membrane area (9 m2 per element)40 compared to that
of high-pressure membranes with a spiral wound module
design (27 m 2 per element). 41 Several DT module
configurations are available with a range of maximum pressure
during filtration from 70 to 150 bar.40 Average water output,
however, is fairly low at 3 m3 day−1 per module for the
treatment of landfill leachate or other wastewaters.40
Membranes were also designed by Toray in the early 2000s
for operation up to 100 bar to achieve 60% recovery SWRO.42
Nonetheless, at present, the maximum operating pressure for
currently available Toray RO membranes is 83 bar.43
Additionally, Dow recently started manufacturing a specialty
line of RO elements rated at operating pressures up to 120
bar.41,44 The largest of these spiral wound elements (8 in.
diameter) is rated to generate permeate flow rates of 24.2 m3
day−1, albeit when treating 32000 mg L−1 NaCl to 8% recovery
at 55 bar (standard SWRO test conditions).41 The achievable
permeate flow rate during high-pressure operation is unclear.
To circumvent the need for high hydraulic pressures,
alternative “osmotically assisted” RO process configurations
that theoretically could use conventional (∼70 bar) pressures
have recently been proposed.45,46 These hypothetical processes
would use a saline solution at the membrane permeate side to
reduce the osmotic pressure difference across the membrane
and thus the required applied hydraulic pressure.45,46 Several
stages would be used to sequentially decrease the feed and
permeate osmotic pressures, until finally conventional RO can
be used to produce pure water. While these osmotically
assisted RO processes could theoretically avoid high-pressure
operation, their performance is inherently limited by internal
concentration polarization (ICP) in the membrane support
layer. As previous studies on forward osmosis have shown, ICP
decreases the solute concentration at the permeate-side
membrane−solution interface, drastically reducing the trans-
membrane driving force for water permeation and thus limiting
water flux.47,48
Designing membranes for osmotically assisted RO to
mitigate ICP will be very challenging. An intrinsic trade-off
exists between ICP reduction and mechanical integrity: the
membrane properties that decrease ICP (small support layer
thickness and high porosity) will decrease the pressure
tolerance of the membrane. The use of pressure-retarded
osmosis (PRO) membranes has been proposed to balance
these contradictory needs;45 however, recent work has shown
dramatic deformation of PRO membranes to take place at an
applied pressure of 55 bar, the maximum pressure achieved
prior to failure.49 In addition to ICP, increased capital costs
from staging and high frictional pressure drops in the permeate
channels49 would also hinder the proposed processes.
471
Review
■ HPRO PROCESS DESIGN CONSIDERATIONS
The design and operation of conventional RO processes are
well-established for brackish water RO and SWRO. However,
at high pressures and salinities, HPRO will likely require
unique design considerations. In this section, we discuss
several aspects of HPRO process design that must be
addressed for the development of membrane-based hypersaline
brine desalination.
Concentration polarization (CP) in the feed channel during
RO increases the osmotic pressure at the membrane surface,
πm, thus increasing the pressure needed to effect flux. Using
film theory and the van’t Hoff approximation, the CP modulus
can be defined as19
iJ y
= expjjjj w zzzz
πm − πp
kk{
πb − π p (2)
where πb and πp are the osmotic pressures in the bulk feed and
permeate solutions, respectively, Jw is the water flux, and k is
the mass transfer coefficient. If we neglect the permeate
osmotic pressure (πp = 0 assuming complete solute rejection)
and changes in mass transfer coefficient, which will be affected
to some extent by salinity (Figure S1), the πm/πb ratio is
constant for a given water flux, meaning that the relative
increase in osmotic pressure should be similar for different feed
solutions. Conversely, the absolute increase in osmotic
pressure from CP is correspondingly greater for high-salinity
feeds. For example, a modest CP modulus of 1.15 increases the
feed osmotic pressure of flowback water (modeled as 157000
mg L−1 TDS)50 by 26 bar, approximately the osmotic pressure
of seawater.
We performed module-scale modeling to assess the impact
of CP for one- and two-stage HPRO processes (Figure 3A).
When comparing 35000, 70000, and 125000 mg L−1 feeds
(each at 50% recovery), we find that water fluxes are
surprisingly similar. This result is partially a function of
conventional direct-pass RO operation where the hydraulic
pressure driving force is roughly the same throughout the
module: the increased driving force at the head of the module
for hypersaline feeds roughly balances the impact of increased
CP. To improve process efficiency, interstage design (i.e.,
placing higher-rejection, low-flux membrane elements at the
head of the module) may be useful for balancing water flux
along the module length (Figure S2).51 While this analysis
considers only a few cases, it appears that SWRO-like water
fluxes (10−15 L m−2 h−1) should theoretically be attainable for
HPRO, despite the increased CP stemming from the high feed
osmotic pressures.
Although CP is expected to impact water flux relatively little
in HPRO, it may critically influence inorganic scaling. In RO,
sparingly soluble salts near their solubility limit can precipitate
because of CP or increased retentate concentrations as water
recovery increases.52 Scaling could be a performance-limiting
phenomenon in HPRO processes, particularly at high water
recoveries (e.g., ZLD). Common scale-forming species,
including Ca2+, Mg2+, CO32−, SO42−, Ba2+, Sr2+, and silica,53,54
are present in many hypersaline brine wastewaters. FGD
effluent, for example, has average concentrations of gypsum
precursors Ca2+ and SO42− of 2000 and 13000 mg L−1,
respectively.36 If FGD effluent (33000 mg L−1 TDS)36 was
concentrated to 250000 mg L−1 TDS (87% recovery), Ca2+
and SO42− concentrations would be 15000 and 100000 mg
L−1, respectively, far above the 2400 mg L−1 solubility limit of
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Environmental Science & Technology Letters Review

Figure 3. (A) Average water flux calculated from module-scale membrane process modeling. The average water flux for one- and two-stage HPRO
processes at 50% water recovery is shown for different terminal hydraulic pressures, ΔPt (i.e., applied pressure in excess of the retentate osmotic
pressure). Osmotic pressures of the exiting retentate solution are also shown. Mass transfer coefficients are calculated using Sherwood−Reynolds−
Schmidt correlations and a water permeability coefficient, A, of 1 L m−2 h−1 bar−1 is assumed. (B) Specific membrane area for common module
designs. The specific membrane area is shown as a function of characteristic length along with the permeate production rate for a typical 8 in.
diameter, 40 in. long module operating at a water flux of 10 L m−2 h−1. The characteristic length shown here is the feed channel height for typical
spiral wound68 and plate-and-frame modules.69 For hollow fiber modules, the characteristic length is the average distance between fibers for typical
module packing densities.19 In the schematics, dark blue denotes the feed stream, light blue the permeate, black the membrane active layer, and
gray the membrane support layer, and the characteristic length, a, is colored white. (C) Compression pressure for nonporous hollow fibers. The
compression pressure is calculated using the von Mises criterion as a function of the fiber radii ratio.66 Shown here are dense, nonporous materials,
which will have a compressive yield strength greater than that of porous hollow fiber membranes. The materials shown are polytetrafluoroethylene
(PTFE), cellulose acetate (CA), polyvinyl chloride (PVC), polysulfone (PSf), polyimide (PI), A36 Steel, and Kevlar 49. The compressive yield
strength, σ, is listed for each material.70−72

gypsum.55 In addition, antiscalants that are commonly used to
prevent scaling in conventional RO53 have been ineffective at
high ionic strengths.56 Pretreatment processes are commonly
employed to remove foulants in conventional RO desalination
processes.22 Similarly, pretreatment to remove scale-forming
species may be necessary to achieve high water recoveries in
HPRO.
An important consideration for HPRO is the large volumes
of hypersaline brines that exist globally. To meet this need,
HPRO technologies should have a large specific membrane
waters up to 70000 mg L−1 due to capital cost concerns. At
higher concentrations (i.e., HPRO), energy costs would likely
incentivize two-stage processes, which would substantially
reduce energy requirements compared to those of a one-stage
process, as shown in Figure 1C. Additional configurations are
also possible such as batch and semibatch RO (also called
closed-circuit RO), which use retentate recycle streams.26
Energetic modeling has shown these processes could achieve
similar energy consumption as two- or three-stage RO, without
physical staging.26

area (i.e., membrane surface area per unit volume of membrane
module) to desalinate large-volume brines in compact facilities.
Figure 3B shows the specific membrane surface areas for
several common module design configurations. While hollow
fibers would provide the largest specific areas, their employ-
ment in RO is affected by high bore-side pressure drops and
poorly defined shell-side fluid flow.19 In contrast, spiral wound
modules are commonly used for conventional RO, and because
SWRO-like water fluxes are expected for HPRO (Figure 3A),
they are potentially an optimal HPRO module design. The
design of modules and pressure vessels suitable for HPRO
should be relatively simple using high-strength materials or
more robust designs. Costs may increase for auxiliary system
components and piping that must withstand high pressure and
resist corrosion when exposed to hypersaline brines. The most
challenging module design consideration is likely gluing
membrane sheets together to form an envelope that can
withstand high pressure, although this can likely be achieved
using high-strength adhesives. Permeate spacers should also be
designed for HPRO to minimize membrane deformation into
spacer voids without large increases in frictional pressure
losses.
From a process design standpoint, high salinities in HPRO
will incentivize unconventional configurations to decrease
energy consumption. Conventional RO process designs (e.g.,
one-stage RO) are likely the best options to concentrate feed
472
■
RESEARCH NEEDS FOR HPRO
Conventional RO is a mature technology with high-performing
materials, well-understood transport phenomena, and robust
process designs.25 However, much is unknown about the
behavior of membrane materials and processes under HPRO
conditions. In this section, we highlight the primary research
needs for the development and large-scale implementation of
HPRO.
One of the greatest unknown aspects of HPRO is the
fundamental effect of membrane compaction (i.e., physical
deformation) on membrane performance at high pressure. At
present, only a few studies have assessed RO above 100 bar,
with maximum tested pressures of 200 bar.57,58 These studies
observed decreased water permeability at high pressure and
attributed it to compaction, although compaction was not
directly observed. Indeed, even at conventional RO pressures,
much remains unknown about the nature of compaction.
Laboratory-scale studies commonly attribute declining water
permeability to compaction; however, recent work indicates
fouling may be the primary cause.59 Compaction is best
studied in ultrafiltration (UF) processes, where it has a strong
dependence on membrane composition and morphology.60−63
Decreased water permeability has been correlated to changes
in overall thickness,63 and some results speculate it is primarily
DOI: 10.1021/acs.estlett.8b00274
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Environmental Science & Technology Letters
a result of compaction in the uppermost skin layer of UF
membranes.62 The compaction behavior of UF membranes
may contribute to developing an understanding of RO
compaction as the support layer of state-of-the-art thin-film
composite (TFC) membranes is typically a polysulfone (PSf)
UF membrane. However, the polyamide selective layer
dominates resistance in TFC membranes, which complicates
direct translation from the study of UF membranes. In TFC
membranes, compaction is typically considered to occur in the
support layer;64 however, a recent study speculated that
compaction can occur in the dense selective layer, as well.65 A
much greater understanding of the location and impact of
compaction is critically needed for the development of
deformation-resistant HPRO membranes.
Once the mechanisms of compaction are understood, high-
strength membranes must be fabricated with high water
permeability and salt rejection under HPRO conditions. At
high pressures, membranes may follow two possible modes of
failure: severe compaction, resulting in no permeability, or
rupture, resulting in no salt rejection. In the case of severe
compaction, polymer networks may deform to the extent they
form a dense, impermeable film. Above a certain pressure limit,
however, membranes are likely to rupture, causing a
catastrophic loss of solute rejection. In spiral wound
membranes, rupture is likely to occur within the voids of the
permeate-side spacer. Alternatively, in hollow fibers with a
shell-side feed, membranes are likely to collapse under
pressure.
To gain an understanding of membrane mechanical strength,
Figure 3C estimates the compression pressure for nonporous
hollow fibers fabricated from different polymers, with steel and
Kevlar shown for reference. This analysis focuses on hollow
fiber membranes because their cylindrical shape is more well-
defined than flat sheet membranes supported by permeate
spacers, as in spiral wound modules. The von Mises criterion
estimates the first point of fiber compression as a function of
applied pressure, material compressive yield strength, and fiber
radii ratio (details in the Supporting Information).66,67 The
results in Figure 3C, calculated for nonporous polymer
materials, suggest high pressures may be achievable; however,
the material strength will decrease considerably for porous
materials. A critical research need is to identify porous
membrane morphologies that exhibit high compressive yield
strength without compromising membrane performance. It can
be seen that polysulfone (PSf), the typical TFC RO support
layer material, has a relatively large pressure tolerance in
comparison to those of the other polymers shown. As such, it
may be necessary to develop novel high-strength support layer
materials to provide the pressure resistance needed for HPRO.
Figure 3C also shows a plateau in compression pressure may
be reached at a certain fiber radii ratio, indicating that an
increased support layer thickness may not significantly increase
pressure resistance and high-strength materials may be needed.
In addition to the unknown behavior of compaction,
transport mechanisms in HPRO are poorly understood.
Water and solute transport in RO is traditionally characterized
by the solution−diffusion model.19 While this model is widely
accepted and adequate for conventional RO, it has not been
tested at salinities and pressures relevant to HPRO. In the
solution−diffusion model, salt flux, Js, is typically defined as Js =
BΔC, where ΔC is the difference in salt concentration between
the feed- and permeate-side interfaces of the selective layer and
B is the salt permeability coefficient, typically assumed to be
473
Review
constant for a given membrane.19 However, recent work has
found B to increase substantially with salt concentration,
possibly because of the decreased impacts of electrostatic
repulsion to reject ions at higher salinities.49 To understand
this behavior, the mechanisms and assumptions of the
solution−diffusion model must be studied under HPRO
conditions.
■ OUTLOOK FOR HPRO
The development of HPRO has the potential to enable energy-
efficient and cost-effective hypersaline brine desalination,
although, because of the high thermodynamic minimum
energy of desalination, the quantity of energy required by
HPRO remains relatively large. Therefore, HPRO may be best-
suited for applications where strict regulations or operational
circumstances preclude direct reuse or safe disposal of saline
brines. Nevertheless, the discharge of saline wastewater to the
environment is undesirable. If the development of HPRO
enables energy-efficient brine desalination, future regulations
may further restrict brine discharge practices, motivating
greater need for ZLD.
Decades of work improving conventional RO will provide a
foundational knowledge from which HPRO can be developed.
It is possible that many aspects of conventional RO membrane
and process design will directly translate to HPRO. Even so,
significant work will be needed where knowledge gaps exist,
notably the fundamental nature of compaction. Similarly,
inorganic scaling, a performance-limiting phenomenon in
conventional RO, may limit the achievable recoveries of
HPRO and necessitate the development of effective and
efficient pretreatment to remove scale-forming species.
Current brine management practices are expensive and
environmentally unsustainable. At present, saline waste streams
are discharged to the environment, evaporated in large ponds,
or injected into the ground. Where ZLD is required, inefficient
thermal separation processes must be used. These costly and
environmentally unsound disposal practices prevent the use of
inland brackish groundwater, often abundant in water scarce
regions, and inhibit the beneficial reuse of saline industrial
wastewater. To help increase the utilization of these waters,
HPRO offers great promise as an energy-efficient and cost-
effective brine desalination technology.
■
*
ASSOCIATED CONTENT
S Supporting Information
The Supporting Information is available free of charge on the
ACS Publications website at DOI: 10.1021/acs.es-
tlett.8b00274.
Derivation of energy consumption equations, method-
ology of module-scale water flux analysis, methodology
for specific area calculations of various module designs,
calculation of nonporous hollow fiber compression
pressure, industrial wastewater data (Table S1), depend-
ence of the CP modulus on Re and Sc (Figure S1), water
flux as a function of module position (Figure S2), and
pressure drop for various feed concentrations (Figure
S3) (PDF)
■ AUTHOR INFORMATION
Corresponding Author
*E-mail: menachem.elimelech@yale.edu. Phone: (203) 432-
2789.
DOI: 10.1021/acs.estlett.8b00274
Environ. Sci. Technol. Lett. 2018, 5, 467−475
Environmental Science & Technology Letters
ORCID
Menachem Elimelech: 0000-0003-4186-1563
Notes
The authors declare no competing financial interest.
■ ACKNOWLEDGMENTS
The authors acknowledge the support received from the
National Science Foundation under Grant CBET-1701658 and
Graduate Research Fellowship DGE-1122492 awarded to
J.R.W.
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