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In situ remediation of leaks in potable water supply systems

  • Min Tang

    Min Tang is currently a PhD candidate in the Civil and Environmental Engineering Department at Virginia Tech. She received her Bachelor’s degree from Sichuan University and Master’s degree from Virginia Tech in Environmental Engineering in 2011 and 2013, respectively. Her research interests include aquatic water chemistry, in situ remediation in water supply systems, corrosion, and water/wastewater treatment.

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    , Simoni Triantafyllidou

    Simoni Triantafyllidou was a postdoctoral researcher at Virginia Tech when this work was undertaken. Dr. Triantafyllidou earned her MS and PhD degrees in Environmental Engineering at Virginia Tech, and her research interests include aquatic chemistry, corrosion science, drinking water quality/treatment, sustainable drinking water infrastructure, and public health. She has authored and coauthored numerous publications on these topics. Dr. Triantafyllidou is the recipient of First Place MS Thesis Awards by the Association of Environmental Engineering and Science Professors (AEESP) and AWWA, an Outstanding PhD Dissertation Award by AEESP, a Larson Research Aquatic Support Scholarship by AWWA, and a Best Paper Award in the journal Environmental Science and Technology.

    and Marc Edwards

    Marc Edwards received his Bachelor’s degree in Bio-Physics from SUNY Buffalo and an MS/PhD degree in Environmental Engineering from the University of Washington. His MS thesis and PhD dissertation won national awards from the AWWA, the Association of Environmental Engineering and Science Professors, and the Water Environment Federation. In 2004, Time Magazine dubbed Dr. Edwards “The Plumbing Professor” and listed him among the four most important “Innovators” in water from around the world. The White House awarded him a Presidential Faculty Fellowship in 1996. In 1994, 1995, 2005, and 2011, Edwards received Outstanding Paper Awards in the Journal of American Waterworks Association and received the H.P. Eddy Medal in 1990 for best research publication by the Water Pollution Control Federation (currently Water Environment Federation). He was later awarded the Walter Huber Research Prize from the ASCE (2003), State of Virginia Outstanding Faculty Award (2006), a MacArthur Fellowship (2008–2012), the Praxis Award in Professional Ethics from Villanova University (2010), and the IEEE Barus Award for Defending the Public Interest (2012). His paper on lead poisoning of children in Washington, D.C., due to elevated lead in drinking water, was judged the outstanding science paper in Environmental Science and Technology in 2010. Since 1995, undergraduate and graduate students advised by Edwards have won 23 nationally recognized awards for their research work on corrosion and water treatment. Edwards is currently the Charles Lunsford Professor of Civil Engineering at Virginia Tech, where he teaches courses in environmental engineering ethics and applied aquatic chemistry.

Published/Copyright: November 22, 2013

Abstract

Water leaks in distribution system mains and premise plumbing systems have very high costs and public health implications. The possible in situ remediation of leaks while a pipeline is in service could reduce leaking at costs orders of magnitude lower than conventional pipe repair, rehabilitation, or replacement. Experiences of Roman engineers and recent field observations suggest that such processes can occur naturally or may even be engineered to ameliorate leaks, including those caused by metallic corrosion. Three mechanisms of in situ leak remediation (i.e., metallic corrosion, physical clogging, and precipitation) are described in this paper, in an effort to understand the role of physical factors (e.g., temperature, pressure, and leak size) and water chemistry (e.g., pH, alkalinity, corrosion inhibitors, dissolved oxygen, and turbidity) in controlling in situ remediation for both inert (plastic and aged concrete) and chemically reactive (new concrete, copper, and iron) pipe materials. Although there are possible limitations and uncertainties with the phenomenon, including the fraction of pipeline leaks to which it might apply and the durability/longevity of remediation, such approaches may prove useful in economically sustaining some aging drinking water infrastructure assets and reducing future failure rates.

1 Introduction

A large fraction of the U.S. potable water infrastructure is leaking and is on the verge of failure (an overall condition grade of D), representing one of the most urgent societal infrastructure challenges (ASCE, 2011, 2013; U.S. EPA, 2010) and the single most challenging issue facing the water industry (Wallis-Lage & Chevrette, 2012). The issue profoundly impacts consumers from the perspective of both water mains and premise plumbing piping. Similar problems have been noted in European and Asian distribution systems, where it is reported that leakage rates ranged from 3% to 70% from one country to another over the past 15 years (Frauendorfer & Liemberger, 2010; TEPPFA, 2007).

1.1 Distribution system water mains

Distribution system water mains in the United States are typically composed of cementitious pipes (concrete or asbestos cement), plastic pipes [polyvinyl chloride (PVC), chlorinated PVC, or high-density polyethylene], and iron pipes (cast, ductile, or steel) (Folkman, Rice, Sorenson, & Braithwaite, 2013; Tomboulian, Wilson, Mullin, & Schweitzer, 2004). Many such systems were installed after World War II and are reaching the end of their design lifetime of 60 to >100 years (U.S. EPA, 1982). Water main breaks are currently occurring at a rate of 240,000 per year and rising (U.S. EPA, 2010; Walker & Schaefer, 2009). Aside from obvious public health implications associated with compromised delivery of uncontaminated drinking water to the tap, failure events can cause extensive property damage and water loss (U.S. EPA, 2002). The U.S. Environmental Protection Agency (EPA) estimated that about $200 billion needs to be invested in existing infrastructure to ensure distribution of safe drinking water in the next 20 years (Shanaghan, 2012). The American Water Works Association (AWWA) took into account population growth needs and reported in 2012 that at least $1 trillion must be invested in drinking water infrastructure through 2035 in the United States (Shanaghan, 2012). The American National Standards Institute (ANSI) noted that many of the pipes installed in recent decades have thinner walls than the pipes installed a century ago (PPFA, 2002), and as a result, there are many cases in which newer pipes are failing at a faster rate (and sooner) than older pipes. The estimated cost of replacing failing infrastructure mains is $6300 on average per household in the United States over the next 10 years (AWWA, 2001).

1.2 Premise plumbing systems

An underappreciated problem of similar or perhaps greater magnitude is associated with privately owned potable water plumbing systems in U.S. buildings (Scardina, Edwards, Bosch, Loganathan, & Dwyer, 2007), which are mostly composed of copper, galvanized iron, PVC, or cross-linked polyethylene (PEX) pipes (Tomboulian et al., 2004). Nonuniform copper corrosion was estimated to cause 750,000 copper pinhole leaks annually in premise plumbing systems, comprising about 50% of the total estimated leaks in premise plumbing materials nationwide (Scardina et al., 2007). Plastic plumbing materials’ leak rates are similar to those determined for copper pipe, and the overall costs of all leaks to consumers are currently about $1 billion each year in repair and property damages alone (Bosch & Sarver, 2007; Scardina et al., 2007). The net present value of premise plumbing in buildings is on the order of that for public water mains, and replacing a premise plumbing system can be an expensive unforeseen expense to consumers (up to $4000–$10,000 or even higher for single family homes) (Edwards, 2004; Scardina et al., 2007).

As aging potable water distribution systems fall deeper into disrepair and the costs of traditional replacement increasingly dwarf society’s ability to invest in upgrades, innovative approaches that can extend the lifetime of existing assets are urgently needed.

1.3 Corrosion: usually detrimental but sometimes beneficial

A major cause of pipe leaks is corrosion (Folkman et al., 2013; Walker & Schaefer, 2009). Estimates by the AWWA, the American Society of Civil Engineers (ASCE), U.S. EPA, the Water Infrastructure Network, and the National Academy of Corrosion Engineers suggest that direct costs for inspection, repair, or rehabilitation of water pipeline corrosion range between $8 billion and $36 billion annually and indirect costs are much higher (U.S. EPA, 2002; U.S. FHWA, 2002). Since the 1970s, the U.S. water industry has invested heavily in research and application of corrosion control measures (pH/alkalinity adjustment and dosing of certain corrosion inhibitors into the water), with the intent to reduce all types of water main and premise plumbing corrosion to the extent possible (AWWA, 2011). A cost-benefit analysis for such efforts suggested that investing each $1 in corrosion control for water mains reduced costs from corrosion by $1–$5 (Koch, Brongers, Thompson, Virmani, & Payer, 2001; Ryder, 1980). A cost-benefit analysis for premise plumbing corrosion control has been considered even more favorable at about $5 or $6 saved for each $1 invested (Ryder, 1980). While understanding of corrosion control is imperfect, much progress has been made in reducing corrosion and controlling costs.

The possibility of benefits sometimes arising from corrosion is emerging. It was recently discovered that existing pipe materials, such as leaking copper pipes, have a remarkable ability to self-remediate in some water chemistries as a result of certain corrosion processes (Scardina, Sheffer, & Edwards, 2008). Discovery of this heretofore unknown mechanism of pipe remediation, which has now been reported to occur naturally in at least two water systems (Lytle & Nadagouda, 2010; Scardina et al., 2008), raises prospects of a class of potentially transformative approaches to extending the lifetime of pipeline assets. That is, after more than a century of effort to minimize corrosion at every opportunity, the notion that some types of corrosion might actually be used to repair some existing leaks, or that attempts to control corrosion might sometimes increase the incidence of leaks, is an important consideration and possible paradigm shift. While much more research is needed to document these phenomena and to harness this potential, this paper presents the first comprehensive review of research concepts related to pipeline leak in situ remediation.

1.4 Concepts and definitions for leak remediation of pipelines

The idea of leak remediation of pipes while in service, by manipulating the chemistry of water flowing through pipes, dates back to at least 15 BC, when Roman engineer Vitruvius noted that leaking terracotta pipelines could be permanently sealed by a one-time addition of wood ash to the water (Pollio 15 BC as translated by Morgan, 1960). This general concept was seemingly lost for two millennia, until 1836 when it was noted that new cement exposed to water had an ability to heal cracks (Hearn, 1998; Phillips, 1925; Turner, 1937). Lauer & Slate (1956) defined “autogenous healing” as the ability of cement paste and concrete to heal cracks occurring in the parent material.

The term “in situ remediation of leaks” includes both autogenous and nonautogenous repair mechanisms and is defined herein as the ability of any pipe material (plastic, concrete, or metal) to physically-chemically repair or stop existing leaks via interaction with waters while in normal service. In situ pipe leak remediation can occur for pipe materials that are relatively chemically reactive with water (e.g., iron, copper, and concrete) or relatively chemically inert (e.g., plastic and stainless steel). Chemically active materials can undergo aqueous chemical reactions such as corrosion or dissolution/precipitation, which can locally alter water chemistry and create solids within existing leak holes, in a manner that can actively promote leak remediation. This type of in situ repair is defined as “autogenous” herein. In contrast, chemically inert materials that do not react with water significantly can only be remediated nonautogenously; for example, by dosing or forming high concentrations of particles in the water that can clog leak holes.

The types of leaks encountered also vary with pipeline materials and circumstance. Iron and copper (and sometimes plastic) pipes often initially leak through very small holes termed “pinholes,” whereas concrete pipes (or plastic pipes) often initially leak through very small cracks (Figure 1). A primary measure for tracking success of in situ remediation is the flow rate through each leak, as per prior studies with concrete materials (Edvardsen, 1999; Li & Yang, 2007; Ramm & Biscoping, 1998; Tsivilis, Tsantilas, Kakali, Chaniotakis, & Sakellariou, 2003; Wang, Jansen, Shah, & Karr, 1997), with the ultimate goal of completely stopping leaks and restoring the pipeline integrity.

Figure 1 
            Leak types depend on pipe material.
            Copper (A) (adapted with permission of Sarver, 2010), iron (B), and other metallic materials tend to form holes.
Figure 1

Leak types depend on pipe material.

Copper (A) (adapted with permission of Sarver, 2010), iron (B), and other metallic materials tend to form holes.

1.5 Some encouraging exemplars of in situ remediation of leaks

1.5.1 In situ remediation of concrete in water mains

The Delaware Aqueduct is an extreme exemplar of infrastructure challenges associated with many water mains in the United States. The Aqueduct provides half of New York City’s daily water demand via the world’s longest concrete-lined tunnel (Simpson, Wegner, & Michaels, 2009). After 65 years of service, very small cracks have formed in the concrete liner of this engineering marvel, leaking 35 million gallons of water per day at a cost of $28 million annually for water alone (Kennedy, 2001; NYC, 2008; Simpson et al., 2009). The leaks have also flooded homes, created massive sinkholes, and raised fears of a catastrophic pipeline failure event, which would have devastating economic and public health consequences for the city (Simpson et al., 2009). Conventional repair of leaks via construction of a 2.5-mile bypass tunnel for just one part of this pipeline is scheduled to be completed no sooner than 2021 at a cost of $2.1 billion (NYC, 2011).

The inability to easily access the 91–455 m (i.e., 300–1500 ft) deep pipeline or even shut it off for inspection/repair prompted an evaluation of novel approaches to mitigate leaks, reduce the chance of failure, and extend the lifetime of the pipeline. A bench-scale study of in situ remediation via temporary formation of suspended calcium carbonate by increasing the pH of the water was undertaken with very promising results (Letterman, Chen, Lavrykova, & Snyder, 2008). The change in water chemistry was able to reduce the rate of leaks by 55% in just 2.5 h by clogging simulated cracks (Letterman et al., 2008). This novel approach is currently being pilot-tested as a promising stop-gap measure, to buy time and increase the chances that effective repairs can be implemented on a cost, plan, and schedule suitable to ratepayers and the utility. The approach is justified by the short-term benefit alone, but permanent or semipermanent repair is also a possibility, as was proven by Roman engineers.

1.5.2 In situ remediation of copper pinholes in premise plumbing systems

A case study by Scardina et al. (2008) demonstrated that remediation of copper pinholes is sometimes occurring naturally in premise plumbing without our prior knowledge (Figure 2). Specifically, two adjacent cities used essentially the same source water, but one had very high incidence of copper pinhole leak damages in buildings while the other did not. Thorough investigation revealed that a similar number of leaks were probably occurring in both cities. The difference was that in one city after a few drops of water leaked the copper pinhole would completely heal itself (Figure 2B) before the consumer even became aware of the problem. This seems to be analogous to autogenous (self) repair that sometimes occurs for concrete, but which occurs as a result of metallic corrosion filling the leaks with scale (rust), as opposed to formation of precipitates in the concrete cracks as a byproduct of concrete dissolution reactions. The only evidence of leaks were visually repaired holes roughly every 0.08 m (1/4″) along a 0.9 m (3′) copper pipe at a pressure of 344,738 Pa (50 psi) with no resulting water damages or repair costs. This particular case of in situ remediation has now been documented to persist for more than a decade. In the adjacent city, the leaks grew rapidly after they first formed (Figure 2A), and each leak created up to thousands of dollars of water damage per incident. One city distributed their water at a slightly different pH and used a different type of corrosion inhibitor. It is therefore speculated that differences in water chemistry likely determined whether the leaks eventually caused the failure or in situ remediation, because there were no significant differences in the copper pipes. Preliminary investigation showed that the materials in the sealed holes were mainly copper corrosion precipitates, with some silica, calcium, and magnesium compounds.

Figure 2 
              Conventional wisdom is that leaks invariably get larger with time (A) (adapted with permission of Scardina & Edwards, 2008), but it has been discovered that, in some real-world situations, copper leaks can be remediated if appropriate water chemistry is present (B) (adapted with permission of Scardina et al., 2008).
Figure 2

Conventional wisdom is that leaks invariably get larger with time (A) (adapted with permission of Scardina & Edwards, 2008), but it has been discovered that, in some real-world situations, copper leaks can be remediated if appropriate water chemistry is present (B) (adapted with permission of Scardina et al., 2008).

Another case study by Lytle and Nadagouda (2010) verified the same observation by studying copper pitting corrosion in buildings of Cincinnati, Ohio. The water dripping rate through certain copper pinhole leaks decreased, due to blue-green corrosion deposits, such as Cu4(OH)6SO4 and Cu2O, which formed in the pit structure. Aluminum and silica were also identified in the corrosion deposits. No microbiological activity was identified; thus, water chemistry was demonstrated to play an important role to form the deposits, stopping or reducing the leaks. The water had high pH (∼8.8), chlorine dioxide (0.1–0.37 mg/l), low alkalinity (∼50 mg/l as CaCO3), and significant levels of chloride (∼64 mg/l) and sulfate (∼120 mg/l).

2 Mechanisms of in situ remediation

Three mechanisms can induce in situ remediation of leaks, including corrosion for metallic pipes, physical clogging for all pipe materials, and active precipitation for concrete (Table 1).

Table 1

Summary of metallic corrosion and other mechanisms as contributors to in situ remediation of leaks in water pipes depending on materials.

Mechanism Applies to pipe materials Fundamental healing process References
1. Metallic corrosion Iron Iron corrosion rust precipitates in the leaks by electrochemical reaction, e.g., 4Fe+2H2O+3O2=2Fe2O3·H2O(s)

Illustrative half reactions are: anode (i.e., oxidation): Fe=Fe2++2e- cathode (i.e., reduction): O2+2H2O+4e-=4OH-
Evans, 1963; McNeill & Edwards, 2001; Shreir, Jarman, & Burstein, 1994
Copper Copper corrosion rust precipitates in the leaks by electrochemical reaction, e.g., 2Cu+H2O+O2+CO2=Cu2(OH)2CO3(s)

Illustrative half reactions are: anode (i.e., oxidation): Cu=Cu2++2e- cathode (i.e., reduction): O2+2H2O+4e-=4OH-
Evans, 1963; Shreir et al., 1994
2. Physical clogging All (plastic, concrete, iron, and copper) Waterborne particles (e.g., bacteria, clay, dust, aluminum hydroxide, and sand) can physically block pipe cracks/leaks Clear, 1985; Edvardsen, 1999; Hearn, 1998; Letterman et al., 2008; Neville, 2002; Ramm & Biscoping, 1998
3. Precipitation New concrete Water-formed particles can seal leaks through precipitation reactions, e.g., Carbonation: Ca2++CO32-=CaCO3(s)

Hydration: calcium silicate (or magnesium silicate) precipitation: Ca(OH)2+H4SiO4→Ca2++H2SiO42-+2H2O→CaH2SiO4·2H2O(s)
Clear, 1985; Edvardsen, 1999; Hearn, 1998; Hearn & Morley, 1997; Helmuth, Stark, Diamond, & Moranville-Regourd, 1993; Li & Yang, 2007; Munday, Sangha, & Dhir, 1974; Neville, 2002; Parks, Edwards, Vikesland, & Dudi, 2010; Ramm & Biscoping, 1998; Santhanam, Cohen, & Olek, 2002; Wagner, 1974

2.1 Metallic corrosion

Electrochemical (reduction-oxidation) reactions in nascent leaks of iron or copper pipes can release iron or copper ions and form corrosion rust [e.g., Fe2O3(s) or Cu2(OH)2CO3(s), respectively] (Table 1), which may eventually seal leak-holes because rust solids occupy a greater volume than the metal itself (Figure 3; Evans, 1963; McNeill & Edwards, 2001; Shreir et al., 1994). For instance, each 1×10-3 m3 of iron metal that rusts (i.e., corrodes) can create 2×10-3 to 4×10-3 m3 of rust deposit at high pH (Zemajtis, 1998). However, if the corrosion products are soluble ions or small colloids, and rusts are not formed that adhere to the pipe, then the hole will not be filled but will instead grow rapidly in size. It is therefore hypothesized that the critical path of a nascent leak to either in situ remediation or eventual catastrophic failure depends on the overall balance between the rate at which metals are eaten away and the rate at which scale forms along the wall of holes.

Figure 3 
            Cross-section through a conceptual pinhole in a leaking copper pipe.
            Corrosion reaction precipitates can contribute to remediation of leaks.
Figure 3

Cross-section through a conceptual pinhole in a leaking copper pipe.

Corrosion reaction precipitates can contribute to remediation of leaks.

The rate of metallic corrosion and identity of the corrosion products is controlled by water constituents such as alkalinity, pH, corrosion inhibitors (e.g., polyphosphate), natural organic matter (NOM), dissolved oxygen (DO), and water disinfectants (e.g., free chlorine) (AWWARF, 1996). The pressure and resultant velocity of water in holes, temperature, and other physical factors may also likely influence the ability of rust to form and block holes (McNeill & Edwards, 2001, 2002; Rushing & Edwards, 2004a; Scardina et al., 2008; Wagner, 1974).

Metallic corrosion is known to occur as either nonuniform corrosion (e.g., galvanic, crevice, pitting, erosion, and biological corrosion) or uniform corrosion (Schweitzer, 2006), and each of these forms may have implications for the likelihood of in situ remediation (Table 2).

Table 2

Metallic corrosion forms commonly occurring in pipelines and their potential effects on existing leaks (adapted from Schweitzer, 2006).

Metallic corrosion form Process Informed speculation regarding influence on existing leaks and in situ remediation
Uniform corrosion Even rate of metal loss over the exposed surface Passive film formed on the surface could potentially prevent leaks or create solids that could detach and/or plug existing leaks.
Galvanic corrosion Dissimilar metal corrosion due to the difference of electric potential between two metals The corrosion rate of the less noble metal is locally accelerated, increasing the likelihood of corrosion and leaks but perhaps also increasing the likelihood of in situ remediation. Conversely, the more noble metal is protected, with a lesser likelihood of corrosion and leaks, but possibly a lower likelihood of remediation.
Crevice corrosion Localized corrosion due to the difference of oxygen concentrations When exposed to oxygen, species stable in the crevice may rapidly oxidize to form solids [e.g., CuO and Fe(OH)3] involved in in situ remediation.
Pitting corrosion Localized loss of metal Existing leaks would be expanded. Pits usually appear as deep and tiny holes in metallic pipes. Upon pit breakthrough and initial leak, low DO solution and low pH solution contacts air and precipitates may form (e.g., Figure 2).
Erosion corrosion Deterioration due to cavitation or macro-cell formation Localized attack might be difficult to remediate, and high velocities through pinholes might dramatically accelerate rate of hole growth.
Biological corrosion Deterioration due to corrosive metabolites Biofilms and biological reaction products might assist in physically blocking holes or accumulating solids.

2.2 Physical clogging

Water treatment utilities attempt to minimize waterborne turbidity from particles such as soil, bacteria, sand, clay, Al(OH)3(s), or Fe(OH)3(s). Utilities try to stop these particles from entering distribution systems via coagulation and filtration processes and also to minimize generation of particles in the distribution system such as rust derived from iron pipe. These approaches are credited with protecting public health from waterborne pathogens and improving aesthetics by reducing discolored water complaints. However, practices of Roman engineers indicate that suspended particles may be beneficial by clogging holes, stopping leaks, and perhaps extending the lifetime of water pipes (Table 1; Figure 4; Clear, 1985; Edvardsen, 1999; Hearn, 1998; Neville, 2002; Ramm & Biscoping, 1998). Hearn and Morley (1997) described physical clogging of concrete cracks in infrastructure by entrapment of small particles and formation of a relatively impermeable filter cake. This type of approach has recently been applied to seal leaks in pressurized oil and gas pipelines via injection of discrete particles that seek out and then seal leaks (Ryan, Evans, Alexander, Chirnside, McEwan, & Stebbings, 2007) and in the practical feasibility studies of crack clogging by suspended calcium carbonate particulates for simulated Delaware Aqueduct water leaks (Snyder, 2009).

Figure 4 
            Cross-section through a conceptual crack of a leaking plastic pipe.
            Physical clogging by water particles can seal leak-holes and cracks in all types of materials, including inert pipes (e.g., plastic or aged concrete).
Figure 4

Cross-section through a conceptual crack of a leaking plastic pipe.

Physical clogging by water particles can seal leak-holes and cracks in all types of materials, including inert pipes (e.g., plastic or aged concrete).

Clogging of membranes with well-defined micropores (Benjamin & Lawler, 2013) provides some insight into leak remediation in pipelines. Specifically, pressure gradient would be the main driving force for particles transport to and then through the leak hole. The likelihood that waterborne particles passing through a small leak would contact the hole wall and contribute to clogging is controlled by sieving, diffusion (Brownian diffusion and shear-induced diffusion), and charge attraction/repulsion between formed particles and the hole wall, which in turn are a strong function of particle size, leak diameter, and surface chemistry. Sieving can play an important role in remediation when the particle diameter is nearly equal to or exceeds the size of leak. In general, smaller particles (<4×10-8 m) are likely to collide and attach due to Brownian diffusion, whereas larger particles (>1×10-6 m) are likely to attach due to shear-induced diffusion (Benjamin & Lawler, 2013). Other than diffusion, the motion of an isolated particle is also a function of drag force, London-van der Waals attractive force, and electrical force.

The likelihood of successful attachment to leak walls (and clogging) may be a particularly strong function of surface charge for both the surface of leak holes and the waterborne particles. If the surface charges, as indirectly measured by zeta potential of the particles and leak walls, are low (often -1.0×10-2 to +1.0×10-2 V), the likelihood of particle attachment and entrapment in a leak is very high (Davis, Edwards, & Knocke, 2001; Tseng, Segal, & Edwards, 2000). Higher surface charge (more than +1.5×10-2 V or less than -1.5×10-2 V) can prevent attachment and might prevent clogging due to the charge repulsion (Davis et al., 2001; Tseng et al., 2000). Because the surface charge of waterborne particles suspended in distribution systems is dependent on particle type, water pH, phosphate, NOM concentration, and other water constituents (Davis et al., 2001; Lytle & Snoeyink, 2002; Naidu, Morrison, Janik, & Adghar, 1997), water chemistry and particle type will determine whether particles pass through or clog holes in a pipe. These same parameters might be manipulated to engineer improved pipeline leak outcomes and distribution system lifetimes.

2.3 Precipitation

Precipitation of carbonation products and hydration products as a result of lime dissolution are considered the main mechanisms of autogenous healing for cracks in new concrete (Table 1; Figure 5) (Clear, 1985; Edvardsen, 1999; Hearn, 1998; Helmuth et al., 1993; Munday et al., 1974; Parks et al., 2010; Ramm & Biscoping, 1998). Hydration refers to the reaction of flowing water with unhydrated concrete to form hydrated precipitates (mainly calcium silicate hydrate or C-S-H) that seal cracks (Hearn & Morley, 1997). Carbonation refers to precipitation of calcium with carbonate in the flowing water to form calcium carbonate precipitates [CaCO3(s)] (Clear, 1985; Edvardsen, 1999; Hearn & Morley, 1997; Lauer & Slate, 1956; Li & Yang, 2007; Neville, 2002; Wagner, 1974). This process requires sufficient carbonate ion present from water, whereas the calcium can be from water or leaching of calcium hydroxide (i.e., lime) from new cement (Neville, 2002). Calcium hydroxide was detected in the material clogging leaks in some waters (Neville, 2002). Precipitation of magnesium solids is another possibility if sufficient magnesium and silica are present at the high pH present in leak pores (Parks et al., 2010; Santhanam et al., 2002). However, as concrete “ages” with time, the once reactive concrete pipe becomes relatively unreactive with water constituents and unable to further leach lime and other precipitates, reducing this dimension of remediation (Table 1).

Figure 5 
            Cross-section through a conceptual crack in a leaking concrete pipe.
            Carbonation and hydration reaction precipitates can seal cracks in concrete pipes.
Figure 5

Cross-section through a conceptual crack in a leaking concrete pipe.

Carbonation and hydration reaction precipitates can seal cracks in concrete pipes.

3 Physical and chemical impacts on creation of leaks in water pipelines

Some physical and chemical factors can cause localized corrosion or pinholes depending on circumstances. Specifically, high water velocity can cause erosion corrosion of metallic pipes, occasionally resulting in leaks (Schweitzer, 2006). Temperature can cause cracks in concrete pipes due to thermal expansion (Neville, 2002). High pH (9.0) and low alkalinity also favor localized pitting corrosion, which may result in pinhole leaks in copper pipes (Ha, Taxen, Williams, & Scully, 2011; Lytle & Schock, 2008; Marshall & Edwards, 2005, 2006; Rushing & Edwards, 2004b; Sarver & Edwards, 2012; Sarver, Dodson, Slabaugh, & Edwards, 2011). NOM in water distribution systems is a carbon source for microbes such as sulfate-reducing bacteria, which can cause microbially induced copper and iron pitting corrosion and pipeline leaks (Hamilton, 1985; Jacobs & Edwards, 2000; Jacobs, Reiber, & Edwards, 1998; Scardina et al., 2008). Sulfate can cause pitting corrosion in iron and copper pipes depending on the flow rate and pH condition (Duthil, Mankowski, & Giusti, 1996; Edwards, Ferguson, & Reiber, 1994; Edwards, Meyer, & Rehring, 1994; Edwards, Rehring, & Meyer, 1994; Shemilt, Cha, Fiadzigbe, & Ponter, 1980; Szklarska-Smialowska, 1978). Chloride has complex impacts on metallic pitting corrosion depending on the circumstances (Duthil et al., 1996; Edwards et al., 1994; Mattsson & Fredrikksson, 1968). Water disinfectants such as free chlorine could also prompt pitting corrosion (Marshall, 2004; Sarver & Edwards, 2012).

4 Physical and chemical impacts on leak in situ remediation potential of water pipelines

Physical and chemical factors can also play important roles in in situ remediation of existing leaks. Their effects (beneficial, detrimental, or mixed) are likely dependent on the reactivity of different pipe materials (Table 3).

Table 3

Summary of expected effects of physical factors and water chemistry on in situ remediation of leaks in water pipes.

Parameter Potential effect on in situ remediation in
References
Plastic (I) Concrete (R when new) Iron (R) Copper (R)
Physical factors
 Water velocity increase ? ± ± Calle, Vargas, Pastén, & Pizarro, 2007; Rodolfo, Pisigan, & Singley, 1987; Scardina et al., 2008; Taxén, Letelier, & Lagos, 2012; Vargas et al., 2010; Wagner, 1974
 Pressure increase Edvardsen, 1999; Neville, 2002; Scardina et al., 2008
 Temperature increase ± Boulay & Edwards, 2001; Lytle & Nadagouda, 2010; McNeill & Edwards, 2000; Neville, 2002; Obrecht & Quill, 1960a, b, c, d, e, f
 Leak size increase Li & Yang, 2007; Neville, 2002; Wang et al., 1997
Water chemistry
 pH increase ? + ± ± Edwards et al., 1994; Edzwald, 2011; Kosmulski, 2009; Lytle & Nadagouda, 2010; McNeill & Edwards, 2001; Montgomery, 1985; Moulin & Rogues, 2003; Naidu et al., 1997; Noh and Schwarz, 1989; Pourbaix, 1984; Ramm & Biscoping, 1998; Sarin, Snoeyink, Lytle, & Kriven, 2004; Scardina et al., 2008
 Carbonic species increase ? ? ± ± Broo, Berghult, & Hedberg, 1998; Dodrill & Edwards, 1995; Edwards, Schock, & Meyer, 1996; Ha et al., 2011; McNeill & Edwards, 2001; Rehring & Edwards, 1996
 Alkalinity increase ? ? ± ± Broo et al., 1998; McNeill & Edwards, 2001; Mishra, Olson, & AI-Hassan, 1992; Sarver & Edwards, 2012
 Calcium carbonate increase ? + ? ? Clear, 1985; Hearn, 1998; Hearn & Morley, 1997; Lauer & Slate, 1956; Letterman et al., 2008; Neville, 2002; Parks et al., 2010
 NOM increase ? ± ± Campbell & Turner, 1983; Edwards et al., 1994; Korshin, Perry, & Ferguson, 1996; Lin, Singer, & Aiken, 2005; Murray-Ramos, 2006; Rehring & Edwards, 1996; Sarver & Edwards, 2012; Stumm & Morgan, 1996; Zhang, 2005
 Phosphate inhibitors increase ? ? ± ± Edwards & McNeill, 2002; Lewandowski, Lytle, & Carno, 2010; McNeill, 2000; McNeill & Edwards, 2000, 2001; Vargas, Alsina, Pasten, & Pizarro, 2009
 Sulfate increase ? ± ± ± Neville, 2004; Santhanam et al., 2002; Santhanam, Cohen, & Olek, 2003; Traubenberg & Foley, 1971
 Chloride increase ? ? ± ± Edwards et al., 1994; Elzenga, Graveland, & Smeenk, 1987; Mattsson & Fredrikksson, 1968; McNeill & Edwards, 2001; Van Der Merwe, 1988
 Magnesium, silica, and calcium increase ? + ± ± Davis et al., 2001; Lytle & Nadagouda, 2010; McNeill & Edwards, 2001; Parks et al., 2010; Rushing, McNeill, & Edwards, 2003; Santhanam et al., 2002, 2003; Scardina & Edwards, 2008
 DO increase ? ? + + AWWARF, 1996; Lytle & Nadagouda, 2010; McNeill & Edwards, 2001; Sarin et al., 2004
 Disinfectant (ClO2, Cl2, and NH2Cl) increase ? ? ± ± Edwards, Jacobs, & Taylor, 2000; Frateur, Deslouis, Kiene, Levi, & Tribollet, 1999; Hallam, West, Forster, Powell, & Spencer, 2002; Hamilton, 1985; LeChevallier, Lowry, Lee, & Gibbon, 1993; Lytle & Nadagouda, 2010; Nguyen, 2005; Nguyen, Stone, Dudi, & Edwards, 2010; Pourbaix, 1974; Sarin, Snoeyink, Lytle, Kriven, & Clement, 2001; Sarver et al., 2011; Volk, Dundore, Schiermann, & LeChevallier, 2000; Zhang, 2005; Zhang, Stout, Yu, & Vidic, 2008
 Turbidity increase + + + + Clear, 1985; Edvardsen, 1999; Hearn, 1998; Letterman et al., 2008; Morgan, 1960; Neville, 2002; Ramm & Biscoping, 1998
 Ionic strength increase ? ? ± ± Dunn, Bogart, Brossia, & Cragnolino, 2000; Edzwald, 2011; Smart & Bockris, 1992; Zhang, Pehkonen, Kocherginsky, & Ellis, 2002

I, inert material; R, reactive material; +, increases likelihood of remediation; -, reduces likelihood of remediation; ±, mixed effects on remediation; ?, unknown.

4.1 Physical factors

Potentially dominant physical factors include water velocity, pressure on leaks, temperature of water, and leak size in the pipeline (Table 3).

4.1.1 Water velocity

Water velocity within the pipe can influence many aspects of corrosion, including the type of corrosion (i.e., uniform, erosion corrosion, and cavitation) or the chemical and mechanical conditions at the metal-solution interface, and concentration gradients of dissolved and particulate constituents at the pipe wall (Calle et al., 2007; Taxén et al., 2012; Vargas et al., 2010). Crossflow filtration in membrane gives insight into the potential effect of water velocity on the transport of water constituents within a leak. Specifically, the water velocity is expected to influence diffusion, the shear stress between water flow and the wall, and therefore the potential volume of particles potentially deposited (or eroded from within) on the leaks. As an example of how lower water flow can contribute to autogenous repair, stagnant water allowed healing of cement cracks five times faster compared to water velocity of 0.025 m/s in one study, although differences in the test specimens and crack geometry provide only strong suggestive proof (Wagner, 1974).

Water velocity above 3 m/s can cause copper pipe to fail in field studies due to wall penetration from erosion corrosion (Scardina et al., 2008). Conversely, higher water velocities may be beneficial when delivering more oxygen to the holes/cracks, allowing formation of more corrosion precipitates, which can potentially seal leaks. One study showed that more oxide precipitates were formed at higher velocity (1.2 m/s) in mild steel pipes than lower velocity (0.6 m/s) with 9.0±0.1 mg/l DO at 20°C (Rodolfo et al., 1987), and similar trends might occur within scale formed within leaks. One experiment with flushing demonstrated that high water velocity (0.167 m/s) caused detachment of more particles from the copper pipes into the water mainly due to the greater shear stress than the lower water velocity (0.022 m/s) (Vargas et al., 2010).

Overall, it is expected that lower velocities within leaks might enhance the likelihood of particle attachment and physical blocking of plastic pipe holes by waterborne/water-formed particles. While delivering a larger volume of particulate matter to the proximity of holes would be beneficial, higher scouring rates and reduced attachment would be detrimental. It can also be expected that impacts of velocity would be complex and highly dependent on circumstances.

4.1.2 Pressure

Higher pressure in the pipeline would be anticipated to reduce the likelihood of in situ remediation, as it increases the force on deposits that are needed to plug the holes/cracks and the detachment of accumulated particles. Experimental studies showed that four times higher water pressure (97,000 vs. 24,000 Pa; i.e., 14 vs. 3.5 psi) on 2×10-4 m wide concrete cracks could lead to 50% less healing, as measured by water flow through the cracks (Edvardsen, 1999). Pressure might also be an impediment to in situ remediation if the sealed leaks fail to withstand the imposed pressure, and the pressure load versus strength recovery of the sealed cracks/hole may become one key to long-term success of in situ remediation (Neville, 2002). The capability of sealed cracks or holes to withstand a typical 140,000–420,000 Pa (20–60 psi) pressure in premise plumbing systems, or even higher pressure (420,000–1,400,000 Pa; i.e., 60–200 psi) in water mains (Woodson, 2006), might be limiting factors. One field study cited herein demonstrated that remediation of leaks in copper pipes by forming scales could occur even under typical premise plumbing pressures of 350,000 Pa (50 psi) (Scardina et al., 2008) and the Roman systems also sometimes operated at high pressure (>1,400,000 Pa; i.e., 200 psi; Pollio 15 BC as translated by Morgan, 1960). No experimental or other field data are currently available to demonstrate the role of pressure on the three mechanisms of in situ remediation.

4.1.3 Temperature

Temperature is a master variable due to its role in solubility, kinetics of precipitation, crystallization, diffusion, sedimentation, and virtually all aspects of in situ remediation mechanisms. Temperature can also affect DO solubility, corrosion precipitates’ solubility, redox kinetics, and biological activity in water (McNeill & Edwards, 2000). Neville (2002) found that lower temperature helped heal cracks in concrete and speculated the enhancement was due to thermal contraction of leaks, whereas high temperature increased the crack size and delayed the remediation of leaks. Temperature has a complicated effect on in situ remediation since it would affect the kinetics of the dissolution reaction from metal (tending to increase the hole size) and the corrosion or precipitation reactions (tending to decrease the hole size). The destiny of leaks and possibility of in situ remediation would depend on which trend is dominant.

A short-term (4.5 months) experiment with intact iron pipes showed that lower temperature (5°C) created slightly more corrosion products on the pipe surface and more iron leaching into water compared to higher temperature (20–25°C) (McNeill & Edwards, 2000). The much bigger volume of the corrosion precipitates created in this study might suggest an improved likelihood of in situ remediation. On the contrary, higher temperature would generally accelerate the kinetics of other reactions that enhance growth of leaks for copper including erosion corrosion and release of particulates (Obrecht & Quill, 1960a, b, c, d, e, f). For intact copper pipes, a 6-month study indicated that higher temperature (60°C) would release a higher proportion of particulate copper in soft water (5 mg/l alkalinity as CaCO3) compared to lower temperature (4°C, 20°C, and 24°C) (Boulay & Edwards, 2001). Hot temperature could, on the contrary, accelerate the aging of copper pipes and help to develop a stable uniform layer of corrosion products on the pipe surface (Lytle & Nadagouda, 2010). As a result, the dominant rate between metal leaching rate and corrosion product formation rate in leaks determines the pathway toward remediation or failure. As was speculated for concrete, any pipe will expand with higher temperature and contract with lower temperature.

4.1.4 Leak size

Larger leaks are expected to be more difficult to seal due to the need to accumulate more adherent precipitates to clog up the leaks, and the greater total force that must be withstood by the area of new deposit in the leaks. Various authors reported that in situ remediation of concrete was not possible in reasonable time periods if the crack width exceeded a certain threshold (Li & Yang, 2007; Neville, 2002; Wang et al., 1997). This threshold ranged from 150 μm for cracked engineered cementitious composite specimens in a study by Li and Yang (2007) to 200 μm in research by Wang et al. (1997). The reported threshold size of a repairable crack width varies in different studies because of variations in water chemistry and other test conditions as well as differences in the concrete test specimens. Considering the novel concept of in situ remediation for metallic and inert pipes, no prior studies have examined the effect of leak size in these materials. It is logical to expect that larger leaks in copper, iron, and plastic pipes would also be more challenging to in situ remediation, similar to observations for larger concrete cracks.

4.2 Water chemistry

Water chemistry plays a central role in the corrosion process of all reactive pipe materials, including iron, copper, and concrete. Specifically, pH, alkalinity, carbonic species, calcium carbonate, sulfate, chloride, NOM, corrosion inhibitors, DO, calcium, magnesium, silicate, water disinfectants, and ionic strength affect corrosion in metals and concrete and by extension would probably affect leak in situ remediation as well (Table 3). Turbidity, a surrogate indicator of particle concentrations in water, is hypothesized to beneficially affect physical clogging for the in situ remediation of all pipes including inert materials, but it is uncertain how other water parameters would affect in situ remediation of relatively inert plastic pipes (Table 3).

4.2.1 pH

pH is also a master variable in drinking water systems, which controls many chemical reactions in water. Both acidic and basic conditions can be corrosive to metallic pipes, but acidic conditions often tend to favor metallic ions as reaction products (i.e., soluble form), whereas basic conditions tend to form corrosion precipitates (i.e., insoluble form). This trend would be expected to increase the likelihood of success of in situ remediation at higher pH. Indeed, in iron pipes, higher pH (pH 7–9) was generally found to develop a greater volume of corrosion products on pipe surfaces (McNeill & Edwards, 2001), a necessary step in the remediation of leaks. Another study indicated that higher pH (7.5–9.5) also decreased soluble iron release into the water, minimizing the chance of red water (Sarin et al., 2004). At very high pH, however, it is possible that corrosion rates would be substantially reduced, to the point that leak clogging by corrosion precipitates might be impeded.

For copper pipes, some studies identified a difference between the pH of local water near the pinhole (pH 3.5–5.5) and the pH of the bulk water inside the pipes (pH 8.8) (Edwards et al., 1994; Lytle & Nadagouda, 2010; Pourbaix, 1984). This local pH change might also play a role in preventing remediation of copper pinholes, because the lower pH near the leak would accelerate corrosion and creation of soluble ions. For concrete, a 2-year study on reinforced concrete cracks showed that moderate pH (pH 7) lowered the flow rate through cracks, while lower pH (pH 5.2) allowed more flow through cracks (Ramm & Biscoping, 1998). This indicated potential success of in situ remediation at higher pH and a path to failure at lower pH.

Aside from effects on reactive pipe materials, pH may influence physical clogging of leak holes in inert pipes. pH determines the point of zero surface charge (PZC) for waterborne particles and plastic pipes in drinking water systems, which in turn influences the size of suspended particles present in water by coagulation processes. The attractive or repulsive force between particles and crack/leak walls will also be highly dependent on the pH for the point of zero charge (pH-PZC) and therefore affects the chance of particles adhering to block pipeline cracks or holes. Thus, at or near the PZC of waterborne or water-formed particles, the likelihood of larger particles and attachment to holes (Figure 4) will tend to be maximized. The pH-PZC is controlled by the type of particles (Naidu et al., 1997). For example, aluminum hydroxide, calcium carbonate, and silica particles are commonly present in potable water supplies and their pH-PZCs are quite different. The pH-PZC is 8.5 for aluminum hydroxide, 8–10 for calcium carbonate, and 2–4 for silica in relatively pure water (Edzwald, 2011; Kosmulski, 2009; Montgomery, 1985; Moulin & Rogues, 2003; Noh and Schwarz, 1989). Thus, clogging of leaks in inert materials by waterborne particulates is expected to demonstrate different optimal pH dependent on the particles present.

4.2.2 Carbonic species/alkalinity/calcium carbonate

Calcium and carbonate are two important components participating in in situ remediation of concrete materials. Carbonate species participated in self-repair of concrete in experiments, and the material repairing concrete cracks was mainly calcium carbonate (Clear, 1985; Hearn, 1998; Hearn & Morley, 1997; Lauer & Slate, 1956; Neville, 2002; Parks et al., 2010). As a common waterborne particle in natural water sources or by purposeful formation/addition, suspended calcium carbonate was proven capable of physically clogging simulated cracks of aged concrete pipes in a bench-scale study (Letterman et al., 2008).

In copper pipes, one study proved that the soluble copper concentration in bulk water leached from copper pipes increased with the free carbon dioxide (Broo et al., 1998; Rehring & Edwards, 1996). In monitoring for copper to tap water, the highest copper concentration was observed when alkalinity (7.4 mg/l as HCO3-) and pH (6.4) were very low (Broo et al., 1998; Dodrill & Edwards, 1995; Rehring & Edwards, 1996), and corrosion rates showed a similar dependence (Broo et al., 1998; Rehring & Edwards, 1996). Overall, the presence of carbon dioxide and alkalinity can be expected to exert a strong effect on the corrosion rates of copper, copper speciation, and the likelihood for in situ remediation.

For cast iron pipes, alkalinity is a controlling factor in multiple steps of the corrosion process and can be expected to influence leak remediation. For example, high alkalinity and higher buffering intensity tend to reduce the corrosion rate (McNeill & Edwards, 2001; Sarver & Edwards, 2012) and the corresponding volume of corrosion precipitates that form. Carbonate could also help remediation by formation of siderite (FeCO3) scale, which is believed to be more protective in pipes compared to ferric species, such as goethite (FeOOH) and hematite (Fe2O3) (McNeill & Edwards, 2001; Mishra et al., 1992). Free carbon dioxide, on the contrary, could complex with iron oxides and cause higher soluble ferrous iron in water (McNeill & Edwards, 2001) and possibly put leaks on a path to failure.

4.2.3 NOM

NOM is an important constituent of drinking water controlling corrosion rates, colloid stability, and solubility (Rehring & Edwards, 1996). NOM interactions are very complex due to its inherently heterogeneous nature, and after decades of research, these reactions are moderately well understood if not perfectly predictable chemically. Thus, leak in situ remediation in the presence of NOM may be complicated due to its complex secondary impacts on water chemistry and microbes.

For iron pipes, NOM (0.2 mg/l Aldrich humic acid) in one study had no effect on iron corrosion rates under both saturated and low oxygen conditions when microbes were absent (Zhang, 2005). However, in another study, NOM increased the formation of iron oxide scale layers and inhibited iron dissolution (Campbell & Turner, 1983), potentially increasing the likelihood of in situ remediation. For copper pipes, NOM was an effective corrosion inhibitor when its concentration was above 0.3 mg/l in aggressive water, as defined by Larson’s index (Edwards et al., 1994; Murray-Ramos, 2006; Rehring & Edwards, 1996). NOM is also known to reduce leaks by stopping copper pitting corrosion (Edwards et al., 1994; Sarver & Edwards, 2012). Korshin et al. (1996) also showed that NOM could markedly enhance nonuniform corrosion tendencies and potentially form more precipitates in a narrow range of concentrations (0.1–0.2 mg/l), therefore enhancing the likelihood of leak in situ remediation.

Calcite (calcium carbonate) precipitation could also be poisoned by NOM (Lin, 2005; Lin & Singer, 2005; Lin et al., 2005) and inhibit self-healing of concrete. NOM can also coat suspended particulates and decrease the zeta potential, thereby stabilizing colloids in smaller size ranges (Stumm & Morgan, 1996), which could tend to prevent clogging of leaks.

4.2.4 Phosphate corrosion inhibitors

Polyphosphate, orthophosphate, zinc orthophosphate, zinc metaphosphate, and bimetallic phosphate are commonly used iron and copper corrosion inhibitors in the United States (Lewandowski et al., 2010; McNeill & Edwards, 2000, 2001). These inhibitors affect both the metal release rate and scale formation rate within existing leaks, thereby influencing in situ remediation. For example, McNeill (2000) showed that the presence of 1 mg/l orthophosphate as P at pH 9.5 decreased iron release from cast iron pipe into water but increased scale buildup on the pipe wall, relative to conditions without phosphate. The greater rate of scale buildup might indicate that phosphates could assist in remediation. Corrosion inhibitors can also slow the copper corrosion rate and reduce the copper release rate by forming a protective insoluble layer [such as Cu3(PO4)2] outside the pipe (Edwards & McNeill, 2002; Lewandowski et al., 2010; Vargas et al., 2009). This also indicates a potential for in situ remediation of copper pipe leaks.

4.2.5 Magnesium, silica, and calcium

Silica is naturally present in water and can be added as a corrosion inhibitor. Silicate was reported to decrease the corrosion rate of iron and is expected to become part of the corrosion products via sorption (Davis et al., 2001; McNeill & Edwards, 2001). Rushing et al. (2003) noted that higher levels of silicate (50 mg/l as SiO2) would release more iron into water, initially causing a red water problem but in the longer term would then be incorporated into a protective scale layer of the pipe, which might stop leaks. Silica has also been identified in the corrosion products of leaks in copper pipes (Lytle & Nadagouda, 2010). In one field study where pits in copper pipes were remediated, the deposits were mainly composed of copper and silica with a small amount of calcium and magnesium (Scardina & Edwards, 2008). Calcium silica hydrate and magnesium silica hydrate were also identified in sealed concrete cracks as facilitators of in situ remediation (Parks et al., 2010; Santhanam et al., 2002, 2003). Magnesium, calcium, and silica can therefore contribute to remediation of leaks in a wide range of circumstances. On the contrary, silicate can coat iron hydroxide particulates and create a highly negative surface charge, maintaining smaller colloids and preventing attachment in leaks (Davis et al., 2001).

4.2.6 Sulfate/chloride

Sulfate has been identified as aggressive to concrete and cause concrete degradation or expansion in concentrated sodium sulfate and magnesium sulfate solutions (Neville, 2004; Santhanam et al., 2002, 2003). This trend might reduce in situ remediation potential of water by enhancing dissolution rates. Sulfate has mixed effects on iron corrosion depending on pH and flow conditions. One study showed that, at 35°C with pH close to 3 in sulfuric acid solution for 6 h, the weight loss of pure iron coupons increased with sodium sulfate concentrations (from 0.1 to 0.5 mol/l; i.e., from 0.1 to 0.5 M) but decreased thereafter (from 0.5 to 1 M sodium sulfate) (Traubenberg & Foley, 1971). That study concluded that sulfate enhanced corrosion rate, but the extrapolation to results at circa neutral pH in potable water is unclear.

Chloride is expected to have a complex influence on in situ remediation. For copper, chloride tends to help seal the leaks in the longer term due to stifling reactions and possible formation of CuCl (Edwards et al., 1994; Mattsson & Fredrikksson, 1968). For iron, one study indicated that chloride would complex with iron in the scale and increase ferrous iron concentration in water that could potentially help remediation by forming more solids (Elzenga et al., 1987; McNeill & Edwards, 2001). However, Van Der Merwe (1988) showed that chloride had no effect on the weight loss of cast iron, reinforcing the possible complex impact of chloride on in situ remediation.

4.2.7 DO

DO is probably the dominant electron acceptor for corrosion in potable water (see cathode reactions in Table 1). This might lead to increased rates and concentrations of corrosion scale relative to situations with low DO. Perhaps more importantly, at low DO for iron, dissolved Fe2+ species will predominate relative to very insoluble Fe3+ species that tend to favor rust formation (AWWARF, 1996; Lytle & Nadagouda, 2010; Sarin et al., 2004). More precipitates will potentially form compared to metal ion leaching into water with increasing DO concentration, thereby reducing leaks. For example, approximately 18 mg/l less iron was leached into the stagnant water compared to the water without any DO (pH 6.2–6.8) in intact iron pipes in 2 h, and iron scales were observed outside pipe surface with the presence of 9.7 mg/l DO (Sarin et al., 2004). For copper pipes, little or no corrosion occurs in the absence of oxygen, so at very low DO copper pipe might behave as an inert material (Edwards et al., 1994). Overall, DO could be an important parameter in in situ remediation of copper and iron pipes through participation in corrosion reactions but would not be expected to affect remediation of inert concrete and plastic pipes.

4.2.8 Water disinfectant

Free chlorine, monochloramine, and chlorine dioxide are commonly used for drinking water disinfection in the United States. Disinfectants could influence in situ remediation by (1) increasing corrosion rates (metal dissociation rate and scale formation rate), (2) promoting the formation of less soluble species, and (3) controlling or minimizing biofilms in water and on pipe surfaces.

By nature, these disinfectants can accelerate corrosion (e.g., copper and iron pipes) by redox reactions (Frateur et al., 1999; Hallam et al., 2002; LeChevallier et al., 1993; Nguyen, 2005; Sarin et al., 2001; Zhang et al., 2008). Several studies have shown varied effects of chlorine and chloramine on corrosion rate in metallic pipes depending on water chemistry (Nguyen, 2005; Zhang, 2005). Sarver et al. (2011) indicated that high levels of chlorine could encourage copper pitting (nonuniform) corrosion, and several researchers (Lytle & Nadagouda, 2010; Nguyen et al., 2010; Pourbaix, 1974) have demonstrated that the concentration of ions within pits was dramatically different than in bulk water, which could affect the reactions contributing to or hindering self-remediation. For example, very low pH <4 within pits could hinder the likelihood of self-remediation after leaks begin, but very high levels of Cu(I) ions, which are easily oxidized to Cu(II) oxide scale, could enhance the likelihood of remediation. Sarver et al. (2011) found that chloramine did not contribute to pitting corrosion to the extent that chlorine did, but it nonetheless oxidized copper and contributed to scale formation (Nguyen et al., 2010).

These disinfectants can also transform corrosion products and form less soluble species, potentially promoting the chance of in situ remediation. Specifically, both iron and copper pipe scale products were shown to react with chlorine dioxide in a first-order rate (4.2×10-4 to 1.4×10-3 s-1 for iron and 8.7×10-5 to 1.0×10-4 s-1 for copper), which could oxidize the main scale components Fe3O4 or Cu2O into less soluble ferric or cupric solids (Zhang et al., 2008). The ferrous iron, which was commonly found in corrosion products [e.g., FeCO3 or Fe(OH)2], could also be oxidized by free chlorine, forming more insoluble Fe (III) oxides, such as Fe2O3 or FeOOH (Sarin et al., 2001). Free chlorine was also demonstrated to react with copper corrosion precipitates [e.g., Cu2O or Cu(OH)2] to form more aged solids, such as tenorite (CuO) (Nguyen, 2005).

Disinfectants can control or inhibit microbial activity and biofilms both in water and on pipe surfaces and therefore decrease microbially induced corrosion (MIC) and resulting leaks in pipelines (Edwards et al., 2000; Hamilton, 1985; LeChevallier et al., 1993). However, this process is greatly affected by corrosion byproducts, which could provide a habitat for bacteria and decrease the efficiency of disinfection (Volk et al., 2000). In addition, the type of disinfectant would control biofilms, which might have their own propensity to induce leak repair via biofouling. Overall corrosion, disinfectant type, and microbial activity are expected to sometimes work in synergy and sometimes in opposition in relation to in situ remediation.

4.2.9 Turbidity

High turbidity is conventionally considered an indicator of poor water quality due to its indication of poor removal of waterborne microorganisms. However, in Roman pipelines in 15 BC, wood ashes were purposefully added to water to help in situ remediation of leaks by clogging (Pollio 15 BC as translated by Morgan, 1960). Waterborne or water-formed particles have been acknowledged to physically block holes or cracks in concrete materials (Clear, 1985; Edvardsen, 1999; Hearn, 1998; Letterman et al., 2008; Neville, 2002; Ramm & Biscoping, 1998). This indicates that some forms of turbidity could be helpful in in situ remediation.

4.2.10 Ionic strength

Ionic strength can affect the stability of waterborne and water-formed particles by compressing the electrical double layer and increasing the likelihood of attachment of particles to surfaces (Edzwald, 2011). Thus, ionic strength could affect the type and size of particles present in water and the chance of in situ remediation via physical clogging of leak holes.

Ionic strength can also influence corrosion products and corrosion rates (Dunn et al., 2000; Smart & Bockris, 1992). Higher ionic strength generally has a positive effect on the corrosion rate of metals. Dunn et al. (2000) indicated that the corrosion rate for iron at lower ionic strength (0.0028 M Cl-) was, on average, 74.4% slower (2.1×10-4 vs. 8.2×10-4 m/y) than that at higher ionic strength (0.028 M Cl-). Moreover, corrosion products such as lepidocrocite (γ-FeOOH) and magnetite (Fe3O4) formed in low ionic strength (0.028 M Cl-) solution versus the more soluble akaganeite (β-FeOOH) in high ionic strength (0.028 M Cl-) solution. In another study by Smart and Bockris (1992), the corrosion rate of iron linearly increased with increasing ionic strength. In a study by Zhang et al. (2002), the corrosion rate of copper increased when ionic strength increased from 0.005 to 0.01 M. The corrosion products [Cu2O and Cu(OH)2] were more soluble due to smaller copper ion activity at higher ionic strength. All these studies indicate that ionic strength could change the solubility and type of corrosion products, which could exert considerable influence on leak remediation efforts.

5 Possible limitations of in situ remediation approaches to seal water leaks

In situ remediation offers a suite of novel approaches to reduce or stop leaks in drinking water infrastructure, and certain limitations to their successes may be anticipated. First, it is impossible in practice to identify pipelines that have been remediated in situ, without removing and forensically investigating underground pipes. This means that real-world cases of remediation might remain undiscovered, reducing our appreciation for its overall importance in pipeline performance and distribution system longevity. Second, if the deposits do not accumulate in leaks, then in situ remediation in metallic and concrete pipes may not be possible. Third, it is uncertain if the materials sealing leaks are able to endure high pressures (140,000–1,400,000 Pa; i.e., 20–200 psi) commonly present in both water distribution systems and building plumbing systems. There is no knowledge regarding how long-lasting and durable the repairs can be, although the field studies suggest that remediation of copper leaks can persist for more than 10 years. Fourth, metallic corrosion, scaling, and particle formation in water pipelines, which could produce in situ remediation, might also cause high turbidity, colored water, and other consumer concerns. While these issues might limit the longevity and application of leak remediation in practice, the topic is highly deserving of future research given the attractive economics and public health benefits.

6 Summary and conclusions

In situ leak remediation gives potentially transformative approaches with multiple mechanisms to reducing leaks and extending the lifetime of certain aging U.S. water distribution infrastructure. The phenomenon appears to be occurring in practice without our knowledge in at least some cases. Corrosion is correctly perceived as detrimental to the mechanical integrity of metallic water pipes. However, in at least some cases, corrosion may also provide a pathway to natural in situ remediation of some leaks. Two field studies provided practical evidence for the potential of relatively inert (aged concrete) and active (copper) pipes to seal leaks in situ, if appropriate and as yet incompletely identified repair mechanisms are enabled.

Three mechanisms are described for in situ remediation. These include corrosion for metallic pipes, physical clogging for all types of pipes, and precipitation for concrete pipes. Metallic corrosion can seal holes in pipelines with corrosion precipitates. The balance between the rate of hole growth via corrosion and hole shrinkage via scale formation, and the durability of the deposits, will determine the potential for success of remediation in metallic (iron or copper) pipes. Suspended particles in water can also sometimes be beneficial in terms of in situ remediation as opposed to the conventional perception that they are invariably harmful. Physical clogging can be achieved by waterborne or water-formed particles [e.g., sand, bacteria, clay, rust, and Al(OH)3(s)], and its effectiveness is expected to depend on their size and surface charge. Cracks in concrete may also heal due to precipitation reactions, in which calcium carbonate, calcium silicate hydrate, or magnesium silicate hydrate can be the main materials remediating leaks.

The three mechanisms for in situ remediation are predicted to be highly dependent on both physical factors and water chemistry. The impact of individual physical or chemical parameters is complex and has not explicitly been studied previously in the context of water leak remediation, with the exception of cracked concrete under conditions not typically found in pressurized potable water pipelines. Additional research work and field observations will be needed to determine if these novel approaches can be applied in practice. Despite potential limitations, in situ leak remediation could possibly be used as an economically innovative way to sustain vulnerable drinking water infrastructure – an issue that has been deemed among the most urgent infrastructure problems facing the United States and is also significant around the world.


Corresponding author: Min Tang, Civil and Environmental Engineering Department, Virginia Tech, Durham Hall 418, Blacksburg, VA 24061, USA, e-mail:

About the authors

Min Tang

Min Tang is currently a PhD candidate in the Civil and Environmental Engineering Department at Virginia Tech. She received her Bachelor’s degree from Sichuan University and Master’s degree from Virginia Tech in Environmental Engineering in 2011 and 2013, respectively. Her research interests include aquatic water chemistry, in situ remediation in water supply systems, corrosion, and water/wastewater treatment.

Simoni Triantafyllidou

Simoni Triantafyllidou was a postdoctoral researcher at Virginia Tech when this work was undertaken. Dr. Triantafyllidou earned her MS and PhD degrees in Environmental Engineering at Virginia Tech, and her research interests include aquatic chemistry, corrosion science, drinking water quality/treatment, sustainable drinking water infrastructure, and public health. She has authored and coauthored numerous publications on these topics. Dr. Triantafyllidou is the recipient of First Place MS Thesis Awards by the Association of Environmental Engineering and Science Professors (AEESP) and AWWA, an Outstanding PhD Dissertation Award by AEESP, a Larson Research Aquatic Support Scholarship by AWWA, and a Best Paper Award in the journal Environmental Science and Technology.

Marc Edwards

Marc Edwards received his Bachelor’s degree in Bio-Physics from SUNY Buffalo and an MS/PhD degree in Environmental Engineering from the University of Washington. His MS thesis and PhD dissertation won national awards from the AWWA, the Association of Environmental Engineering and Science Professors, and the Water Environment Federation. In 2004, Time Magazine dubbed Dr. Edwards “The Plumbing Professor” and listed him among the four most important “Innovators” in water from around the world. The White House awarded him a Presidential Faculty Fellowship in 1996. In 1994, 1995, 2005, and 2011, Edwards received Outstanding Paper Awards in the Journal of American Waterworks Association and received the H.P. Eddy Medal in 1990 for best research publication by the Water Pollution Control Federation (currently Water Environment Federation). He was later awarded the Walter Huber Research Prize from the ASCE (2003), State of Virginia Outstanding Faculty Award (2006), a MacArthur Fellowship (2008–2012), the Praxis Award in Professional Ethics from Villanova University (2010), and the IEEE Barus Award for Defending the Public Interest (2012). His paper on lead poisoning of children in Washington, D.C., due to elevated lead in drinking water, was judged the outstanding science paper in Environmental Science and Technology in 2010. Since 1995, undergraduate and graduate students advised by Edwards have won 23 nationally recognized awards for their research work on corrosion and water treatment. Edwards is currently the Charles Lunsford Professor of Civil Engineering at Virginia Tech, where he teaches courses in environmental engineering ethics and applied aquatic chemistry.

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Received: 2013-06-04
Accepted: 2013-09-20
Published Online: 2013-11-22
Published in Print: 2013-12-01

©2013 by Walter de Gruyter Berlin Boston

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