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Review papers

Acid Mine Drainage from Coal Mining in the United States – An Overview

Bharat Sharma Acharya, Gehendra Kharel

PII: S0022-1694(20)30521-7
DOI: https://doi.org/10.1016/j.jhydrol.2020.125061
Reference: HYDROL 125061

To appear in: Journal of Hydrology

Received Date: 4 February 2020

Revised Date: 1 April 2020
Accepted Date: 9 May 2020

Please cite this article as: Sharma Acharya, B., Kharel, G., Acid Mine Drainage from Coal Mining in the United
States – An Overview, Journal of Hydrology (2020), doi: https://doi.org/10.1016/j.jhydrol.2020.125061

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© 2020 Published by Elsevier B.V.

Acid Mine Drainage from Coal Mining in the United States ─An

Overview

Bharat Sharma Acharya1* and Gehendra Kharel2

1Oklahoma Department of Mines, State of Oklahoma, 2915 N Classen Blvd., Oklahoma City, OK 73106
2Department of Environmental Sciences, Texas Christian University, TCU Box 298835, Fort Worth, TX
76129

Corresponding Author
Bharat Sharma Acharya
Oklahoma Department of Mines
State of Oklahoma
2915 N Classen Blvd.,
Oklahoma City, OK 73106
Email: bikatiaas@gmail.com

Contents
Introduction ..................................................................................................................................................2
AMD: A Global Concern .............................................................................................................................4
Chemistry of Acid Mine Formation..............................................................................................................5
Factors Affecting AMD................................................................................................................................6
Prediction of AMD .......................................................................................................................................8
Static Test: Acid-Base Accounting (ABA)...............................................................................................9
Kinetic Tests...........................................................................................................................................11
AMDTreat ..............................................................................................................................................12
Prevention and Treatment of AMD ............................................................................................................14
Treatment of AMD .................................................................................................................................14
Active Treatment ................................................................................................................................15
Passive Treatment...............................................................................................................................17
Other Treatments ....................................................................................................................................20
Bactericide Treatment Systems ..........................................................................................................20
Industrial By-products and Wastes .....................................................................................................21
Holistic and Integrated Approach .......................................................................................................22
Remote and Ground Sensing Techniques in AMD Studies ........................................................................22
Material Damage Criteria and Mine Closure..............................................................................................24
Challenges and Opportunities.....................................................................................................................25

0
Conclusions and Recommendations ...........................................................................................................28
References ..................................................................................................................................................30

Abstract

Water discharged from active, abandoned and/or reclaimed coal mine sites with relatively higher acidity

continues to be a global concern due to variable impacts on the quality of surface water and groundwater.

Treatment of such acid mine drainage (AMD) is often complex, costly and challenging. Towards this end,

this review provides an overview of the formation and effects of AMD, reviews prediction and treatment

methods, identifies critical research gaps, and explores the associated challenges and opportunities AMD

poses for environmental scientists and researchers. Acid drainage occurs through oxidation of sulfide

minerals such as pyrite. The main sources of AMD include runoff and seepage from mine rock dumps,

open pit mines, stockpiles, tailings, construction rocks, and rock cuts. While different active and passive

treatment systems are available to treat AMD, prevention techniques and integrated management

approaches could better identify possible risks, abate treatment costs, and reduce eco-hydrological

hazards. Also, the coal mining sector could benefit from remote and ground sensing techniques, including

the use of unmanned aerial vehicles and hyperspectral imaging for hydrogeochemical investigations.

Effective treatment of acid drainage from mine areas reduces material damage, allows resource reuse and

recovery, and enables successful post-mine land use. Environmental scientists must, however, design and

implement a proper framework to address AMD in a timely manner. While mining and treatment plans

may vary with land-use history, climate, topography, hydrogeology, available technology, and socio-

political outlooks, environmental scientists and mining companies must make it a priority to form

multidisciplinary partnerships, advocate for effective enforcement of discharge standards, encourage

performance bonding, and formulate remediation plans.

Keywords: Acid-base accounting; Acid mine drainage; Active treatment; Coal; Kinetic tests; Passive

treatment; Pyrite

1
Introduction

Although experiencing remarkable turmoil in the last few decades, the coal industry is

nevertheless a prominent source of power generation and one of the roots to economic growth

and infrastructure development. Worldwide coal production reached 7813.3 million tons (Mt) in

2018 (WCA, 2020). The dynamic realm of the coal market is globally recognized; for example,

Asia is expanding its coal mining and coal power generation, largely driven by rapidly growing

population, economic expansion, and energy demands (WCA, 2020). The U.S. is one of the

largest coal producers in the world, with recoverable coal reserves totaling 253 Mt. The total U.S.

coal production is 756.2 Mt, out of which the U.S. uses 636 Mt in electric utilities and power

generation (Table 1; NMA, 2019).

Surface coal mining underpins the shallow mining method to extract coal embedded in earth by

removing overburden covering a coal seam. It includes strip, auger, highwall, box cut, open pit,

and area mining. After mining, coal companies reclaim sites by grading, replacing topsoil, and

revegetation driven by specific set of soil, air, and water quality regulations and health and safety

standards. In the U.S., surface mining for coal is mostly common in Central Appalachian (Ferrari

et al., 2009; Pericak et al., 2018), Eastern States (Barnhisel & Hower, 1997), and the Great Plain

(Hemish, 1989; Mamula, 1978; Martinez-Salazar, 1985; Vestal, 1987) regions, among others. It

accounts for nearly 63% of the 679 total mines in the U.S. (Table 1; NMA, 2019) and dominates

both the mining method and coal mine productivity (Table 2).

Coal mining has significant economic, ecologic, hydrologic, and geomorphic ramifications.

Recently, Feng et al. (2019) reviewed the effects of surface mining and reclamation on the

physical, chemical and biological properties of fundamentally inter-connected soil, and they

2
highlighted management needs and reclamation strategies for environmental protection. Others

(Bonta, 2000; Bonta et al., 1997; Negley & Eshleman, 2006) have documented the hydrological

impacts of surface mining. Those studies indicated that mining disturbance could alter water

flowpaths and increase runoff, erosion, nutrient leaching and drainage, subsurface void space,

and baseflow. Non-point pollution, for example acid drainage, is highly likely when mining

exposes sulfide minerals. Sulfide oxidation could furthermore initiate several in-mine chemical

reactions that adversely affect water quality (Mayo et al., 2000). But after mining companies

reclaim sites, runoff attenuates, water chemistry improves, and recharge increases; those effects,

however, vary with reclamation methods, climate, hydrogeology, vegetation, and remediation

bonding (Evans et al., 2015; Lines et al., 1981; Surber & Simonton, 2017).

Acid mine drainage (AMD) continues to be a concern in coal mining because it reduces surface

water and groundwater quality (Verburg et al., 2009) and may perhaps persist for several years.

In the U.S. only, AMD pollutes over 20,000 km of streams (Skousen et al., 2019). Blasting and

dewatering exposes sulfide minerals, posing threats to environment. Treatment of AMD is often

complex, costly, and challenging, but any discharge from mine sites ought to comply with local,

regional, national, and international laws and regulations such as the Surface Mining Control and

Reclamation Act (SMCRA) and the Clean Water Act (CWA) (Zipper, 2000). Treatment costs

may vary with site conditions, composition of acid mine water, and treatment methods. Globally,

governments and private companies spend millions of dollars each year in capital and

operational costs to treat AMD, meet effluent limits and minimize environmental risks. For

example, construction costs of Keister Wetlands in West Virginia, U.S., was nearly $225,000

(1994 U.S. dollar value) to treat AMD by using passive biological system (Faulkner and

Skousen, 1994).

3
This review provides an overview of AMD problems, describes the state-of-the-art methods in

predicting, preventing, and treating AMD, and identifies critical research gaps along with the

associated challenges and opportunities for additional research. While the review focuses

primarily on the U.S., the authors synthesize information from several other countries for better

understanding of AMD problems globally. First, this paper briefly discusses AMD as a global

environmental pollution and management issue, followed by the chemistry of acid mine

formation and the factors affecting it. Subsequently, it addresses a wide range of AMD

prediction methods along with their strengths and weaknesses. This review provides a

comprehensive review of different prevention and treatment methods, and the use of remote

sensing techniques in mining operations, the assessment of the cumulative impact of mining

through Material Damage Criteria, and a guide to effective mine closure. Finally, this paper

discusses existing challenges and opportunities in AMD treatments, and proposes

recommendations for AMD treatments.

AMD: A Global Concern

Acid mine drainage refers to water discharged from active, inactive, or abandoned mine and

reclaimed areas with relatively higher total acidity compared with total alkalinity. It encompasses

several chemical, biological, and electrochemical reactions, which the paper discusses in later

sections. Different sources of AMD include runoff from mine rock dumps and open pit mines,

tailings, diffuse seeps, construction rocks, rock cuts/chips, and stockpiles, among others (Fig. 1).

There are documentation of AMD issues in different parts of the globe (e.g., India: Equeenuddin

et al., 2010; Swer, S., & Singh, 2004; Tiwary, 2001; U.S.: Brady et al., 1994; Skousen et al.,

2019; Canada: Ramasamy & Power, 2019; Brazil: Silva et al., 2013; South Africa: Geldenhuis &

4
Bell, 1998; Ochieng et al., 2010), and concurrently extensive research on characterization,

prediction, prevention, treatment, and control measures have been ongoing for >50 years

(Verburg et al., 2009). Acidic and metal-rich water presents a major threat to terrestrial and

aquatic ecosystems, besides human health. Reported effects of AMD include increased levels of

suspended solids, mobilization of heavy metals, decreased pH on water bodies, and groundwater

contamination; entry of heavy metals into food chain and their uptake by plants and animals; and

degradation of drinking water (Ochieng et al., 2010; Geldenhuis & Bell, 1998; Silva et al., 2013).

Toxic metals in water may cause human and animal cells damage and diminution in the

percentage of cell viability (Dutta et al., 2019). Effects due to acidic drainage differ with site,

land-use history, climate, scale of mining, geochemistry of overburden material, and composition

of mine water. Researchers largely discuss groundwater seepage of AMD as a challenging and

most problematic route. While AMD effects are multifold (Fig. 2), they generally pollute water

bodies. According to the U.S. Environmental Protection Agency (EPA), environmental risks due

to AMD are “second only to global warming and ozone depletion (Manders et al., 2009;

Moodley et al., 2018; Mudd and Weng, 2012).”

Chemistry of Acid Mine Formation

Water discharged from mine sites may potentially comprise higher acidity due to the exposure of

sulfide minerals to the atmosphere. Table 3 lists some of the selected sulfide minerals. Coal

sulfur may occur in organic sulfur, pyritic sulfur, or sulfate sulfur forms. Pyritic sulfur occurs in

its disulfide phase as pyrite, and is chemically active. Pyrite oxidizes to ferrous iron, sulfate and

5
acidity. The sequential reactions below (Equations 1 – 4) depict the chemical weathering of

pyrite (Blowes et al., 2003; USEPA, 1994):

FeS2 + 7/2 O2 + H2O → Fe2+ + 2 SO42- + 2 H+ …………………………………………………..1

Fe2+ + 1/4 O2 + H+ → Fe3+ + ½ H2O ………………………………………………….................2

Fe3+ + 3 H2O → Fe (OH)3 + 3 H+ ………………………………………………………………...3
FeS2 + 14 Fe3+ + 8 H2O → 15 Fe2+ + 2 SO42- + 16 H+ …………………………………………..4
Equation (1) shows the oxidation of sulfide to sulfate and generation of H+ ions in presence of

water and oxygen. According to Simate & Ndlovu (2014), Equation (1) relies on oxygen

concentration, pH >3.5, and bacterial activities. The presence of Thiobacillus and Ferroplasma

bacteria accelerate the oxidation process in the refuse. The ferrous iron then oxidizes to ferric

iron (Equation 2). This step is usually a slow process, and many papers discuss this process as a

“rate-determining step” (Hallberg, 2010; Sahoo et al., 2013). Under abiotic condition when

pH<5, the process is relatively slower, but at pH = 2.3 to 3.5, ferric iron in Equation (2)

precipitates as ferric hydroxide, which tends to lower the pH of the solution (Simate & Ndlovu,

2014). In the Equation (3), ferric iron hydrolyzes to ferric hydroxide; the rate of formation varies

with fluid pH; for example, the rate could surge rapidly at pH > 4. Ferric hydroxide precipitates

to appear as white and yellow crust on surface of rocks and sediments. Some ferric iron formed

during Equation (2) may not play their part in Fe(OH)3 formation, which possibly could oxidize

pyrite (Equation 4) and produce ferrous iron, sulfate and acids. Overall, these reactions will

increase H+ ions in the solution, which lower pH to form acidic drains. These reactions and acid

formation will differ largely due to multiple and interactive factors, as discussed next.

6
Factors Affecting AMD

Factors that affect AMD include sulfur content, acidity, alkalinity, pH, distribution and mode of

pyrite occurrence, and interactions between calcium carbonate and pyrite, among others (Fig. 3).

Literature suggests that such factors vary with geographic locations, and therefore prediction,

prevention, and treatment must be site-specific (Simate & Ndlovu, 2014). Factors affecting

AMD fall within three broad categories: generation factors (oxygen, water, bacteria), chemical

factors (acidity, alkalinity), and physical factors (particle size, permeability, weathering,

hydrology) (Pat-Espadas et al., 2018). The pH has the most likely effect on AMD, which may

function in conjunction with several other factors. Based on pH, Kirby (2014) classified mine

drainage into five types: Type 1: pH<4.5 with iron, aluminum and manganese metals, and higher

oxygen levels; Type 2: pH>6.0 with higher levels of ferrous iron, manganese and dissolved

solids; Type 3: alkaline, with low to moderate levels of iron, manganese, and dissolved solids;

Type 4: neutralized AMD (pH>6.0), with high levels of suspended particles; and Type 5:

neutralized AMD with high levels of dissolved solids, and dissolved calcium and magnesium.

Type 1 drainage is a primary mode of acidic drains. A lower pH in acidic waters generally

translates into higher electrical conductivity (EC) due to the dissolution of metals along with the

oxidation of pyrite and mobility of metals occurring at lower pH (Equeenuddin et al., 2010).

The literature review herein indicates that the presence of iron sulfides and quantity of calcareous

material affect the amount of acid and quality of drainage (Fig. 3). Similarly, field studies

support a strong co-relation between pyrite morphology and AMD (Caruccio et al., 1977; Geidel

& Caruccio, 2000). Pyrite may occur in different forms such as framboidal, euhedral, and

anhedral, but the decomposition of framboidal pyrites is critical to produce acid drainage. Non-

framboidal iron disulfides are less reactive, and they decompose slowly and produce lower acids

7
(Caruccio et al., 1977). In general, fine-grained pyrites produce more acid than coarse-grained

pyrites.

Many studies discuss the effects of paleoclimatic and paleodepositional environments on rock

chemistry and distribution of minerals, such as sulfides and carbonates, are unambiguous. For

example, Caruccio et al. (1977) observed that pyrite distribution and acid drainage in the

Appalachian coalfield of eastern Kentucky was related to coal’s paleoenvironment. Their

findings explicitly demonstrated higher reactive pyrite in the lower delta plain sequence (back-

barrier) than the upper delta plain, causing acid drainage. Paleoenvironmental factors could

further modify or influence rock types and chemistry at a spatial scale. For example, Brady et al.

(1988) detected rapid change in the amount of carbonates and stratigraphy at lateral spaces on

surface mining sites in Pennsylvania, U.S., due to paleodeposition. In summary, forms of pyrite,

their occurrences, and their interactions with carbonates may influence AMD and, therefore, the

study and examination of such factors is necessary to predict and control acid drainage, as

discussed next.

Prediction of AMD

Mining operators should develop plans and control measures to prevent AMD or design

treatment systems appropriate to climate, topography, and regulatory requirements, upon the

prediction of AMD risks, and thereby to minimize potential ecological and human health issues.

Regulations set forth in different countries require mining operators to analyze soil and

overburden samples to identify potentially acid- and toxic- forming materials prior mining using

either static or kinetic tests. Static tests evaluate if the given sample will generate acid whereas

kinetic tests predict timings of acid production, rates of acid generation, and the assessment of

8
the released elements (Dold, 2017). According to Skousen et al. (2000), accurate prediction of

AMD depends on three principal factors: overburden geochemistry, overburden handling and

placement, and post-mine hydrology. Upon the prediction of acid- and toxic- forming materials,

mining operators must cover those materials with non-toxic and non-combustible materials, or

treat them to correct acid drainage and minimize water pollution. Studies report that controlled

placement of overburden materials and water management provide beneficial effects on

regulating acid drainage (Sahoo et al., 2013). Other measures that correct acid drainage and

minimize water pollution include diverting surface water away from the pyrite-bearing spoil or

passing it through alkaline materials. Mining operators could remove or isolate contaminated

water from non-contaminated water to substantially reduce acid formation. Also, mining

operators may impound the contaminated water in the structures that are non-toxic forming and

restrict oxygen diffusion (Skousen et al. 2019). These measures also serve as preventive ways of

reducing AMD in coal mining areas.

Static Tests: Acid-Base Accounting (ABA)

First described in 1973 (Grube et al., 1973), ABA is a rapid and relatively cheap method of

overburden analysis to determine either acid production potential (APP) or acid neutralizing

potential. This method evaluates sulfide in the overburden sample based on the stoichiometry of

complete pyrite oxidation, and calculates APP (Sobek et al., 1978) using the Equation (5)

(USEPA, 1994):

APP =31.25 × percent S …………………………………………………………………………..5

9
Neutralization Potential (NP) represents the buffering effects of alkaline materials such as

carbonates that neutralize acid by using the acid-base titration method (Sobek et al., 1978). This

static test, therefore, connotes the balance between acid production and consumption. If the net

NP value exceeds 20 kg CaCO3/t, the sample is non-acid-generating, but at values less than 20 kg

CaCO3/t, the sample will generate acids. One can estimate acid generating potential by using

neutralization potential ratio (APP/NP). Values less than one indicate acid-generating samples.

During ABA, the pulverization of samples destroys their initial textures. Therefore, many use the

degree of sulfide and carbonate release to correct ABA results (Elghali et al., 2018). While ABA

method assumes all the sulfur in sample as reactive, it neglects the manifestation of gypsum and

other non-reactive sulfur minerals. This assumption of ABA method potentially leads to

overestimation of NP by three ways: dissolution of pH regulating minerals through strong acid

usage, reaction of iron and manganese carbonates with acid, and precipitation of metal

hydroxides during the titration with sodium hydroxide (USEPA, 1994). Dold (2017) reviewed

static and kinetic tests used in acid rock drainage prediction and suggested that the calculation

factor of 31.25 overestimates neutralization potential of carbonate by roughly 100%.

Additionally, ABA underestimated acid potential of Fe3+ hydroxides and sulfates and failed to

discern different carbonate minerals. However, Yucel and Baba (2016) compared different static

tests such as paste pH and electrical conductivity, ABA, and net acid generation test to predict

AMD in the Etili open pit mine in Turkey. They observed uniformity between the results and the

association of AMD with mine waste and altered volcanic rocks. USEPA (1994) provided a

comparison between the ABA method and other static methods such as the Modified ABA, BC

Research Initial, Alkaline Production Potential, and Net Acid Production (Table 4).

10
The modified ABA method excludes non-sulfide sources in sulfur assuming sulfate as a non-acid

producing source. This assumption leads to underestimation of APP when jarosite is present in

large quantities in waste materials (USEPA, 1994). Nevertheless, ABA serves as a useful method

to make treatment decisions in acidic areas. Skousen et al. (2002) used ABA to evaluate the

quality of overburden prior mining and to predict the drainage quality after mining for different

sites in West Virginia, U.S. They found that the ABA simulations were accurate for 50 out of 52

sites tested. Studies indicate that accurate prediction of APP fundamentally depends on volume

of samples to better represent and incorporate geologic heterogeneity within a site. However,

Caruccio& Geidel, (1986) criticized the ABA method for not relating to kinetic data that affect

weathering of mine rocks, which calls for additional studies and selection of kinetic tests.

Kinetic Tests

Kinetic tests examine long-term acid-generating and acid-neutralizing potentials using chemical

analysis of leachates on humidity cells or columns. Scientists and professionals have been using

humidity cell experiments to study acid-consuming potential of calcites in several waste rocks

(Langman et al., 2019). Tests in humidity cells are relatively faster than in columns and differ in

sample mass, and the number and duration of flush-drainage cycles. Table 5 shows the

comparison between humidity cells and column tests. In a study, Benzaazoua et al. (2001)

compared two different kinetic tests, humidity cells and the column test, for sulfide mine tailings,

which showed very little difference in oxidation-neutralization rate of minerals. Banerjee (2014)

performed kinetic tests on overburden samples that showed high acid generation potential and

observed better neutralizing capacity than oxidative capacity of the samples, but Banerjee also

reported risks of acid generation due to accelerated rates of carbonate weathering and

11
dissolution, and depletion of neutralizing materials in the study system. The oxidation of sulfides

depends on a number of factors like micro-textures, grain size, temperature, humidity, bacterial

activity, and oxidants (Dold, 2017). Bouzahzah et al. (2014) compared kinetic tests against

Sobek static tests and mineralogical static tests in synthetic tailing samples and provided

recommendations for better prediction of AMD. However, considering the amount of time

consumed in kinetic tests along with the production of large dataset with inconclusive results,

one must conclude that mineral characterization and quantification could be one of the predictive

tools for AMD, if available (Dold, 2017).

Scientists and researchers are increasingly using X-ray diffraction/ fluorescence analyses or

micro computed tomography, inductively coupled plasma atomic emission spectrometry, and

scanning electron microscopy for mineral characterization that quantify modal mineralogy and

predict the degree of sulfide release (Dold, 2017; Gottlieb et al., 2000). Elghali et al. (2018) used

mineralogical and chemical characterization to estimate net acid-generating potential of waste

rocks from the open pit mine in Abitibi, Canada. Results showed that sulfides primarily consisted

of fine to mid-sized fractions. Also, the fine-sized sulfides were highly reactive and had utmost

liberation, but the liberation was negligible when size exceeded 2.4 mm. The study also proposed

“diameter of physical locking of sulfides” as a new parameter to access AMD. This diameter

connotes particle size above which sulfides are locked by non-sulfide minerals (i.e., 2.4 mm in

this study). Therefore, scientists and researchers can determine reactive fraction and use it to

predict AMD and plan for drainage management; yet they must use the column tests to validate

the results.

12
AMDTreat

A literature review indicates increasing use of AMDTreat as a method to predict and recommend

treatment for acid mine drainage waters (Cravotta et al., 2015, 2010). AMDTreat is a computer-

based application jointly developed by the Pennsylvania Department of Environmental

Protection, the West Virginia Department of Environmental Protection, U.S. Geological Survey,

and the Office of Surface Mining Reclamation and Enforcement in 2003. In recent years,

scientists, researchers and mining operators have been using AMDTreat to estimate quantity of

caustic chemicals (NaOH, CaO, Ca(OH)2, Na2CO3, and NH3), effluent quality, and sludge

volume produced during treatments (Cravotta et al., 2015, 2010). Table 6 provides a summary of

the caustic equivalents used by AMDTreat to treat acidic water.

AMDTreat estimates the costs incurred to treat acid mine discharge using different chemical

treatment and constructed wetland systems. It consists of more than 400 variables that users can

modify as necessary to best estimate the costs of developing treatment systems, revegetation,

water sampling, surveying, sludge removal, chemical consumption, among others for both past

and future projects. Different tools embedded within the AMDTreat allow actual site-specific

financial forecasting, and calculation of the recapitalization cost, langelier saturation index,

acidity, flow, sulfate reduction, mass balance, oxidation, abiotic homogeneous Fe2+ oxidation,

biotic homogeneous Fe2+ oxidation, pH averaging, metric conversion, chemical cost conversion,

and PERT statistics (OSMRE, 2020). For example, a sulfate reduction calculator estimates

sulfate loading and the volume of organic matter required to reduce sulfate based on the specific

sulfate reduction rate of constructed wetlands.

AMDTreat consists of two geochemical PHREEQ modules, un-aerated PHREEQ, and pre-

aerated PHREEQ to compute AMD treatment costs, chemical consumption, chemical

13
composition of treated effluents, and volume of byproducts (Cravotta et al., 2015; OSMRE,

2020). In an un-aerated PHREEQ module, user uses water quality analysis data as an input,

which includes the amount of ferrous iron and inorganic carbon. By using the software, users can

also estimate the amount of ferrous iron, which largely depends on user-defined total iron

concentration and pH of water. It simulates the use of caustic chemical to fresh effluent, which

may contain limited to no dissolved O2 but relatively higher concentration of CO2. Pre-aerated

PHREEQ, however, allows for the simulation of pre-areated CO2, using log PCO2 values to

bring water to equilibrium with the atmosphere, and complete oxidation of ferrous iron and

manganese (OSMRE, 2020). For different treatment pHs, these modules simulate effluent

standards. For additional details, see Cravotta et al. (2015) and https://amd.osmre.gov/.

Prevention and Treatment of AMD

This review indicates the utmost importance of prevention techniques to sustainably reduce

AMD problems in coal mining and to ensure effective mine closure (Park et al., 2019).

Preventive methods eliminate or reduce AMD generation by protecting sulfide from exposure to

air and water during disturbance (Kefeni et al., 2017). Preventive methods could include land-

based storage in sealed heaps, blending acidic materials with acid-consuming materials,

solidification of tailings, use of anoxic surfactants, and microencapsulation (Johnson & Hallberg,

2005). Studies also recommend other surface-based techniques to prevent AMD, such as dry

cover, water cover, oxygen consuming cover (e.g. wood waste), and subaqueous tailing disposal

(Kefeni et al., 2017). The proper handling of earth materials, groundwater discharge, and runoff,

by facilitating the use of best technology available and ensuring the use of drainage control,

revegetation, diversion of runoff, and water-treatment facilities protect surface and groundwater

bodies during mining and reclamation (OAC, 2016). The U.S. EPA developed the sequential

14
steps and framework to prevent and treat AMD in abandoned mine sites (USEPA, 1997), which

remains valuable for active mining operations. We modified these sequential steps and

framework in Figure 4, which provide guidance for the treatment of acidic drains, and highlight

the roles of multiple stakeholders such as governmental and non-governmental agencies and

organizations, communities, industries, citizens, and civic groups, and their multi-disciplinary

partnerships for planning, reclamation and remediation.

Treatment of AMD
Once AMD forms, mining operations need to isolate, neutralize or remove it by exploiting

different abiotic and biotic processes (Kefeni et al., 2017). Johnson & Hallberg, (2005) reviewed

and discussed different abiotic and biological measures, each comprising active and passive

ways, to remediate AMD. For example, an active abiotic system could include aeration and

addition of lime, whereas a passive abiotic system comprises anoxic limestone drains. Active

biological systems include sulfidogenic bioreactors, whereas passive biological systems include

wetlands, permeable reactive barriers, and packed bed iron-oxidation bioreactors. Generally,

treatments are either active or passive; active systems use chemicals and passive systems use

natural treatment media.

Active Treatment
Active treatment refers to the addition of alkaline chemicals, such as Ca(OH)2, CaO, NaOH,

Na2CO3, and NH3, to polluted mine water or effluents (Table 6). Two commonly used chemical

treatment methods include high-density sludge and the ChemSulphideTM process (Ali et al.,

2019). The former method utilizes neutralizing reagents (CaO, NaOH) to raise pH and to

precipitate metals in sludge while the later utilizes sulfide reagent (NaHS or Na2S). Alkaline

15
chemicals raise pH, oxidize ferrous iron, and precipitate metals in hydroxides and carbonates

forms (Johnson & Hallberg, 2005). According to Siebert et al. (2019), four major processes

comprise the active treatment of AMD: precipitation, sulfate reduction, ion

exchange/absorption/adsorption and filtration, and crystallization. The sequential reactions

depicting the dissolution of calcium carbonate in water appear below, where dissolution of

carbonates hinge on partial pressure of carbon dioxide gas (Equation 6-8; USEPA, 1994):

CaCO3 + H2O → Ca2+ + HCO3- + OH- …………………………………………………………...6

HCO3- + H2O ↔ H2CO3 + OH-…………………………………………………………………...7

H2CO3- ↔ CO2 + H2O……………………………………………………………………………8

Webb and Sasowsky (1994) indicated that a combined effect of acid neutralization through

carbonic acid dissociation and acid neutralization by carbonate dissolution provides an improved

treatment of AMD. Of different alkaline chemicals, NaOH establishes 100% neutralization

efficiency as it completely dissociates in water to raise the water pH (Table 7; Kefeni et al.,

2017). Scientists and researchers use NaOH in low flow environments when acidity is high.

However, NaOH is relatively expensive, generates ferric hydroxide sludge and is difficult to

handle in cold weather (Skousen et al., 1996; USEPA, 1997). Table 7 shows the advantages and

disadvantages of different chemicals including NaOH in active treatments. Climate, mine water

composition, and operation costs largely determine the use of chemical treatments (Ali et al.,

2018). There are several other active treatment options that are in use. For example, Chen et al.

(2015) studied the short-term and long-term hydrological effects of dry flue gas desulfurization

product (FGD) and observed that FGD product could remediate acidic surface coal mined sites;

the pH of surface runoff increased to 7 or higher after 20 years. Peiravi et al. (2017) used a

16
cathode chamber under aerobic condition for bio-electrochemical treatment of AMD from

abandoned coal mines. Mulopo (2015) used an alkaline barium calcium desalination process to

treat AMD, and observed the sulfate reduction to very low levels and the recovery of barium

carbonates. Active treatment is more suitable for operating mines. It is a relatively low-cost

technology; cost, however, varies with the chemicals and labor involved. It may entail a long-

term commitment (Fripp et al., 2000). Also, whilst treating acidic water, scientists should equally

consider recycling and recovery of raw materials from sludge. Figure 5 provides a schematic

representation of active treatment methods involving alkaline chemicals, and resource recovery.

Passive Treatment
Passive systems rely on natural treatment media and construction materials to treat acidic water

through biological, physical, geochemical, and gravitational mechanisms (Siebert et al., 2019;

Zipper et al. 2018). Passive treatments include wetlands, anoxic limestone drains, open limestone

channels, vertical flow systems, and other systems such as limestone ponds, limestone sand beds,

and limestone diversion wells (Zipper et al. (2018). Passive treatment methods are more suitable

for abandoned mines (Ali et al., 2019) and several studies have documented their usage (Blowes

et al., 2003; Gazea et al., 1996; Hedin et al., 1994; Kaur et al., 2018; Nordstrom, 2009; Pat-

Espadas et al., 2018; Skousen et al. 2019; Zipper et al., 2018). For example, different passive

treatments, their design factors, and organic substrates pertinent to sulfate removal are available

from an earlier review by Skousen et al. (2017). Similar to active treatment options, the use and

efficacy of passive systems also differ with climate, mine water composition, and operational

costs. For example Ali et al. (2020) studied the effects of temperature (22 and 5 oC) and salinity

(0 and 20 g L-1) on the efficacy of passive biochemical reactors and observed lower efficiency at

17
low temperature and high salinity for synthetic AMD treatments. Garcia-Valero et al. (2020)

tested marl, sandstone, and calcareous crust in a batch experiment and observed increased pH

and reduced metal concentration by precipitation for all three alkaline materials; efficiency of

metals removal, however, differed with the particle size of alkaline materials, and contact time

between alkaline materials and AMD. They attained a complete removable of Pb, Fe, and Cu

when the particle size of these materials were 10 – 20 mm. Similarly, they found that a contact

time of six minutes between marl and AMD reduced metals.

Literature indicates the wide use of constructed wetlands for low-cost treatment of AMD, where

utilized emergent and submergent vegetation and microorganisms remediate contaminated water

(Qasaimeh et al., 2015). Acidithiobacillus thiooxidans and A. ferrooxidans are two autotrophic

iron- and sulfur-oxidizing microbes commonly found in constructed wetlands (Nicomrat et al.,

2006, 2008). Constructed wetlands generally incur low cost and maintenance compared with

active treatments, but acid neutralization potential largely depends on climatic events. A survey

of 142 constructed wetlands in eastern U.S. showed that approximately 50% wetlands reduced

H+ concentration by 68%, acidity by 67% and SO4-- by 8% (Wieder, 1989). Efficiency may,

however, vary with area, depth, organic substrates, plants used, and wastewater composition,

among other factors More details on constructed wetlands, and operational guidelines are

available from Brodie et al. (1988), Johnson & Hallberg (2005), Pat-Espadas et al. (2018), Perry

and Kleinmann (1991), and Sheridan et al. (2018). Therefore, this review is primarily focused on

anaerobic wetlands, bactericides technologies, and integrated methods.

Anaerobic wetlands are natural wetlands but engineered biologically to reduce AMD (Fig. 6)

using the Dissimilatory Sulfate Reduction (DMR) technique (Moodley et al., 2018). DMR takes

18
advantage of sulfate-reducing bacteria and organic substrates as carbon sources to remove

sulfides (Moodley et al., 2018). Three major groups of organic substrates used in sulfate

removal include easily available materials (soluble sugars, starch, amino acids, and proteins),

cellulose and hemicellulose, and lignin (Skousen et al., 2017). The designs of anaerobic wetlands

exclude plants to treat a wide range of pollutants (Siebert et al., 2019), but generally for 3.5 g

acidity m-2 day-1 and 10 g Fe m-2 day-1 rates of removal (Skousen et al., 2017). These anaerobic

wetlands consist of limestone and gravel bedrock about 15-30 cm thick layer underneath a

permeable organic substrate of 30-60 cm to increase alkalinity. Water flows into the organic

substrate, where bacteria remove O2 (Zipper et al. 2018). Sulfate-reducing bacteria convert sulfur

to sulfides, which undergo reduction reaction to form hydrogen sulfide and bicarbonates

(Equation 9). Bicarbonates that from in anaerobic wetlands raise pH and remove metals as

hydroxides and oxyhydroxides.

SO4-2 + 2 CH2O → H2S + 2 HCO3-……………………………………………………………….9

Anaerobic wetlands can be reducing and alkalinity producing system (RAPS), successive

alkalinity producing system (SAPS), or permeable reactive barriers (PRBs). For details on each

of these systems, refer to Siebert et al. (2019). Anaerobic wetlands bestow several advantages

including removal of metals and sulfate, stabilization of metal precipitates, lowering sludge

volume, enhancing ecological integrity, increasing habitat for birds and biodiversity, and

lowering maintenance cost (Moodley et al., 2018). Overall, passive systems can reduce acidic

drains by >50% but their performance is, however, site-specific, and largely influenced by

biogeochemical, and physical processes (Kaur et al., 2018). Table 8 lists advantages and

disadvantages of active and passive treatment systems.

19
Apart from sulfate and iron, manganese (Mn) also occurs in acidic drains at higher levels,

affecting water quality (Cheong et al., 2010; Karathanasis et al., 2010; Neculita and Rosa, 2019).

Mn is autocatalytic, with high sorption capacity for other metals (Cr, Cu, Pb, Hg, Ni, Zn). A high

pH will possibly increase Mn requisitioning in colloids, suspended particulate matter, and

sediments, whereas a low pH induces reductive dissolution of oxyhydroxides to further increase

Mn levels and/or release trace elements. Passive systems, such as open limestone beds, can

remove Mn by oxidizing and precipitating Mn, which is mediated by Mn (II)-oxidizing

microbes. Mn oxide coated limestone improves performance in Mn (II)-removal beds. Mussel

shells can also remove Mn by more than 35% (McCauley et al., 2009). Studies reported removal

efficiencies of <10% to as high as100% in bioreactor batch experiments with mushroom compost

substrates (Karathanasis et al., 2010; Song et al., 2012). Generally, Mn removal is challenging

due to higher solubility, and it warrants further research. For additional details on the prevalence,

effects, treatments, and challenges of Mn removal from acidic drains, refer to Neculita and Rosa

(2019).

Other Treatments

Bactericide Treatment Systems

ProMac, a bactericide system developed in the 1980s by BFGoodrich Company, used spray

liquid and controlled-release pellets to inhibit iron-oxidizing bacteria at a source point. ProMac

treatment systems eliminated Thiobacillus ferrooxidans, the iron-oxidizing bacteria, and thereby

reduced AMD. Sobek & Rastogi (1986) identified four-step approach of using ProMac to abate

AMD, which includes problem identification, proposing treatment, supervising the use of

controlled release bactericides, and monitoring treatment and its effectiveness. Guerrero &

20
Oliver, (1999) reported that ProMac promoted the proliferation of beneficial heterotrophic

bacteria such as Acidiphilium.

Researchers use bactericides directly to the effluents or as intimate mixtures (Blowes et al.,

2003). Sobak et al. (1990) used controlled-release bactericides to reclaim coal refuse areas in

East Springfield, Ohio, and Dawmont, West Virginia, and reported that bactericides reduced

AMD and facilitated vegetation growth and development for extended years. The production and

use of this bactericides technology, however, ceased during late 1990’s (Gusek, 2018).

Nonetheless, studies indicate that heterotrophic biofilms and bactericides technologies are

rapidly developing and extensively scrutinized to reduce iron-oxidizing bacteria (Kalin et al.,

2018; Moodley et al., 2018). In a microcosm study, Jin et al. (2008) observed that microbial

inoculum could raise water pH and reduce concentration of Al, As, Cu, Fe, Pb, Ni, and Zn

metals. Zhang & Wang, (2017) observed anionic surfactant, sodium dodecyl sulfate, as an

effective bactericide technology that suppressed iron-oxidation caused by Thiobacillus

ferroxidans. More studies are however necessary to confirm or refute benefits from such

bactericides technologies.

Industrial By-products and Wastes

Other treatments include use of industrial by-products such as basic oxygen furnace slag and

argon oxygen decarburization slag from steel industries to potentially remove sulfate from acidic

drains (Moodley et al., 2018). Mussel shell is another waste material with high acid-neutralizing

potential with >80 wt% CaCO3 (Moodley et al., 2018), and as such, Butler et al. (2019),

DiLoreto et al. (2016) and Weber et al. (2008), among others have used mussel shell to reduce

AMD risks. Researchers more recently tested and used biochar to reduce heavy metals from
21
AMD (Wibowo & Naswir, 2019). For example, Giachini et al. (2018) used poultry-litter biochar

enriched with three sulfate-reducing bacteria sources, sediments from AMD, cattle manure and

domestic activated sewage sludge, to treat AMD from coalmine pond in Brazil and observed

41% reduction in sulfate with cow manure sulfate-reducing bacteria-enriched biochar. In

summary, different methods are available to treat AMD and to remove metals from acidic drains,

but their combination with a passive system could improve performance and lower treatment

costs as discussed next.

Holistic and Integrated Approach

Integrated approaches use a combination of different methods and are efficient ways to treat

AMD (Masindi, 2017; Wei et al.; 2018). Kefeni et al. (2017) suggested a “holistic approach,”

such as resource recovery and reuse, to control AMD. Naidu et al. (2019) suggested the

integration of membrane techniques with active and passive remediation systems to facilitate

water reuse. Geldenhuys, (2003) integrated synthetic organic polymers with limestone treatments

and used those as coagulant and flocculent to remove suspended and colloidal substances.

Masindi (2017) used an integrated approach with cryptocrystalline magnesite for pre-treatment

of AMD and barium chloride to eliminate residual sulfate from an aqueous system. Results

indicated the removal of 99% heavy metals and 40% sulfate with magnesite, and the removable

of 99% residual sulfate with barium. Integrated assessment of AMD and treatment of waste and

effluents therefore prevent and reduce acidic water, but the effects are largely site- and

treatment-specific. More studies on integrated technologies are, however, warranted in the

treatment of AMD and recovery of resources.

22
Remote and Ground Sensing Techniques in AMD Studies

Remote and ground-sensing techniques are popular and cost effective ways to map land use and

land cover, delineate groundwater potential zones (Kumar and Krishna, 2018), analyze ground

subsidence (Baek et al., 2008), study coal fires and fires-related emissions (Saraf et al., 1995;

Zhang et al., 2004), detect near-surface interfaces (Strange et al., 2005), access hydrologic

conditions and AMD (Ebraheem et al., 1990; Kumar and Krishna, 2018), and develop water

treatment plans (Jin et al., 2008), to accomplish other tasks. Ebraheem et al. (1990) used vertical

electrical sounding and horizontal resistivity profiling to study AMD at a reclaimed coal mine

site near Wheatland, Indiana. Results showed a strong negative relationship between resistivity

and total dissolved solids. Moreover, oxidation, dissolution, and infiltration of iron disulfides

resulted in the contamination of Wheatland aquifer. In northeastern India, Blahwar et al. (2012)

used high-resolution satellite imagery to study AMD in artisanal coal mining. Results indicated

an acidic drain problem due to dissolution of pyrites and highlighted potential use of satellite

imagery to largely identify iron precipitates on streambeds. Moreover, others used remote

sensing techniques o facilitate AMD treatment methods. For example, in Tennessee, a biological

source treatment method utilized remote sensing for down-hole injection of microbial inoculum

to prevent sulfides oxidation (Jin et al., 2008).

Drones or unmanned aerial vehicles (UAVs) equipped with active or passive sensors are rapidly

evolving and increasingly being tested as non-intrusive remote sensing machineries for

surveying terrains and developing digital models, promptly collecting water quality samples

(Banerjee et al., 2018), and mapping and monitoring such coal mining areas and water pollution

issues as acidic drains by using multi- and hyperspectral imaging (Kirsch et al., 2018; Hermann

et al., 2019). In a recent review, Ren et al. (2019) discussed the development and application of

23
UAVs, and challenges and opportunities of using them in a mining sector. Among different

UAVs available, fixed wing and multi-rotar wing UAVs are common in mining (Ren et al.,

2019). Jackisch et al. (2018) used drone-based hyperspectral imaging to monitor AMD in Litov

tailings in the Sokolov district, Czech Republic, where they identified the association of acidic

drains with Jarosite and Goethite minerals, and validated iron absorption bands in UAV-

hyperspectral images by using ground-truth spectroscopy. While studies based on UAVs are

relatively safe, flexible, efficient, economical, and precise, such studies remain few. Thus, there

is a need for more of such research for the effective use of remote sensing techniques in

understanding coal mine production, gathering soil and water samples, and integrating

hyperspectral images with field-based hydrological and geochemical data.

Material Damage Criteria and Mine Closure

In the U.S., researchers developed “Material Damage Criteria” to access the cumulative impact

of mining to water availability and changes in pH, total dissolved solids, total suspended solids,

iron and manganese, among others. These criteria signify water quality standards, established

under the EPA 40 Code of Federal Regulations (CFR) and are also important to determine the

cumulative impact during mining and reclamation phase to control water pollution. For example,

a desirable pH range is 6.0 - 9.0, iron content is 7.0 mg/L, and total suspended solid content is

70.0 mg/L. Worrall et al. (2009) highlighted 14 criteria and 72 indicators for the sustainable

development and use of legacy mine lands that are abandoned, derelict, and orphan lands. In

their study, they recognized AMD as one of the environmental criteria to determine the success

of post-mine land use.

24
Effective treatment of acid drainage prevents material damage, determines the success of mine

closure and reclamation, and enables sustainable development of post-mine lands. In a recent

report, Young et al. (2019) suggested a 6-step framework to guide effective mine closure and

completion determining post-mine land use, setting realistic and achievable mining closure

objectives, selecting references and setting targets, establishing risk-based prioritization of post-

mine land use and closure plans, developing completion criteria, and monitoring reclamation

plans against completion criteria. Completion criteria are of utmost importance to determine

success of reclamation, to achieve closure objectives, and to ensure environmental sustainability

(Young et al., 2019). Studies indicate a wide use of pre-disturbance conditions as reference

conditions in post-mine planning, but they require adequate baseline data. Such data may include

different physio-chemical, biological and geological attributes: surface water quality,

groundwater quality, hydraulic conductivity, electrical conductivity, cation exchange capacity,

pH, sediment loss, and vegetation, among others. The baseline data are also important for

assessing water quality after AMD treatment. In the absence of such adequate data, scientists and

researchers often used or suggested a similar site or a conceptual model (Young et al., 2019). In

summary, while effective mine closure prevents AMD risks, prevention and control of AMD

dictates the post-mine land use success.

Challenges and Opportunities

AMD studies, treatment methods, and control measures are not without challenges. Below, this

study highlights major challenges and opportunities in preventing and treating acidic mine

waters.

25
1. There is a need for regular monitoring of acid drainage and water quality from

overburden, rock dumps, refuse piles, mine tailings, and diffuse seeps to determine

emerging problems, sought proper treatment designs, and reclaim mine sites for future

use. Use of baseline data, paleo-depositional information, and geochemical models,

wherever possible, would improve AMD prediction and control. Effective treatment of

acid drainage from mine areas offers opportunities for resource reuse and recovery of

such substances as ferric hydroxide, ferrite, sulfur, and sulfuric acids (Kefeni et al.,

2017; Rakotonimaro et al., 2017), and post-mine land usage. Recovery of gypsum,

calcite and ferrihydrite is possible from the sludge that is used as raw materials in

cement manufacturing. Scientists and researchers used two different methods to recover

dissolved metals and water from AMD: (1) pH dependent methods: selective

precipitation, selective adsorption, and selective ion exchange and (2) pH independent

methods: electro-dialysis, microfiltration, ultrafiltration, nano-filtration, reverse osmosis,

and membrane distillation (Simate & Ndlovu, 2014). Opportunities also exist to generate

electricity and produce iron pigments during wastewater treatment by using Microbial

Fuel Cells (MFC) technology. However, no single technology could effectively

eliminate dissolved metals, and, therefore, Simate & Ndlovu (2014) recommended a

combination of different systems.

2. Static and kinetic tests are associated with large uncertainties, and results are often

difficult to interpret (USEPA, 1994). Developing a standard kinetic test could potentially

reduce uncertainties and errors in analytical results. More research is, however,

warranted to develop, examine, and enact new tests and techniques. Also, there are

multiple opportunities to use UAVs and hyperspectral imaging in active and abandoned

26
 mines and reclamation areas for monitoring water pollution including AMD, and

developing treatment plans.

3. Climatic change and associated variability in weather events, such as drought, rainfall,

and snowmelt runoff, is an emerging challenge and could modify flushing effects, AMD

generation and treatments (Hotton et al., 2019; Nordstrom, 2009). A dry spell followed

by first-flush event could increase sulfate concentration (Gzyl and Banks, 2007;

Nordstrom, 2009; Younger and Blachere, 2004). The effect may, however, decrease

after attaining a peak discharge level. Generally, drought will increase low-flow

conditions and reduce carbonate-containing groundwater, which escalates acid

concentration in drainage water (Nordstrom, 2009). Increased temperature will likely

increase oxidation and sulfuration, and the release of heavy metals (Fu and Lu, 2018).

Also, intense rainstorm events will increase dissolution of sulfates. Treatment plans and

measures are also susceptible to the impacts of climate change. For example, covers

with capillary barrier effects (CCBE) are sensitive to precipitation events; increased

moisture from precipitation events will maintain saturation of moisture-retaining layer

and, therefore, reduce acid drainage whereas drought could accelerate desaturation and

AMD formation (Hotton et al., 2009). As such, environmental scientists and mining

companies need to account for climate variability and flush-out events in developing and

targeting treatment plans (Nordstrom, 2009).

4. Mine closures that adhere a properly designed and implemented framework in a timely

manner may prevent AMD risks and vice-versa. Challenges and opportunities exist for

multidisciplinary partnerships among agencies, organizations, industries, and general

public for problem assessment, treatment planning, funding, and remediation.

27
 5. Spontaneous combustion of coal waste piles represents a special category of mining-

waste problems, and may emit heavy metals into the atmosphere, which later deposit

into aquatic and terrestrial ecosystems (Wang et al., 206). McConnell and Edwards

(2008) reported the deposition of heavy metals and bio-magnification risks in Artic

ecosystems. Further studies on spontaneous combustion of coal wastes, atmospheric

deposition of heavy metals, and the potential for acid leaching are necessary.

6. Developing and implementing cost-effective treatments is challenging but crucial.

Designing and implementation of treatment methods must consider local settings to

ensure post-mining safety and land-use. Each mining project is peculiar and the science

of mine drainage prediction continues to evolve. Also, codes of mining regulations vary

with states and countries, unveiling needs for site-specific framework and criteria. While

plans may vary with sites, land-use history, mines, available technology, eco-

hydrological settings, socio-economic conditions, political outlooks, collaboration

among multiple stakeholders, long-term monitoring, effective enforcement of effluent

limitation, treatment standards, and performance bonding must be a priority.

Conclusions and Recommendations

This paper reviewed different methods of AMD prediction, prevention, and treatment and

identified critical research gaps, challenges and opportunities. The literature, in general, suggests

that AMD can affect water quality and post-mine land-use, depending on multiple interactive

factors. This review draws the following important conclusions:

1. AMD effects are multifarious and therefore future studies should focus on

characterization, prediction, prevention, long-term monitoring, and effective treatment of

AMD.

28
 2. Scientists and researchers use both static and kinetic tests to predict AMD risks. New

tests are, however, warranted to potentially reduce uncertainties and errors in analytical

results.

3. Mineral characterization and quantification could be one of the predictive tools, and

therefore, require further studies.

4. AMD risks demand developing site-specific plans and control measures depending on

land-use history, climate, topography, hydrogeology, and regulatory requirements.

5. Mining sector and AMD studies could benefit from the use of emerging UAVs and

hyperspectral imaging technology in active and abandoned mines and reclamation areas

for hydrogeochemical investigations.

6. Different active and passive treatment systems, bactericides technologies and industrial

by-products and wastes are available to reduce AMD problems in coal mining. However,

preventive methods, integrated treatments, and multidisciplinary partnerships are

necessary to understand the complexity of multiple factors and acid drainage, to curtail

material damage, and to ensure effective mine closure and reclamation.

Disclaimer

The authors are responsible for the views expressed in this paper and do not necessarily represent

or reflect the views and policies of the Oklahoma Department of Mines.

Acknowledgement

29
The authors express their sincere thanks to Dr. Steve Sherwood from the William L. Adams

Center for Writing at Texas Christian University for English language editing.

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Figures Captions:
Fig 1: Sources of AMD (Modified from Akcil & Koldas, 2006)
Fig. 2. Effects of AMD (Adapted and Modified from: Gray, 1997), which include modified
stream health and sediment geomorphology, increased aqueous contaminant concentration,
metals accrual onto sediments, reduced species richness and diversity, altered distribution,
structure and function of algal, microbial, invertebrate, and fish communities, and decreased
primary production, among others. Effects differ with site, land-use history, climate, scale of
mining, geochemistry of overburden material, and composition of mine water.
Fig. 3. Multiple and interactive factors affecting AMD
Fig 4: Sequential steps and framework to address AMD (Adapted and modified from: USEPA,
1997). The concept was originally envisioned for abandoned mine sites. It shows different steps
(1-6) to guide treatment of acidic drains, and highlights role of governmental and non-
governmental agencies and organizations, communities, industries, citizens, and civic groups,
and their multi-disciplinary partnerships for planning, reclamation and remediation.
Fig. 5. Flow chart showing treatment of AMD (Modified from: Mulopo, 2015; USEPA, 1983).
Different caustic chemicals are used to remove acidic water through iron oxidation,
sedimentation and sludge disposal. Other methods include bioelectrochemical treatment, reverse
osmosis and alkaline barium calcium desalination process to treat AMD, and recover metals and
water.
Fig. 6. Anaerobic wetland, a RAPS system (Siebert et al., 2019). RAPS is a passive system used
to treat acidic water by passing it through a compost layer where Fe3+ is reduced to Fe2+. The
water will subsequently flow into a limestone bed, which raises pH through calcite dissolution.
Finally, water is drained into sedimentation ponds to precipitate sludge and retain hydroxides.

48
 Acid Mine Drainage

Primary Source Secondary Source

Mine rock dumps Treatment sludge

ponds
Underground and
open pit mine Emergency ponds

Tailings Rock chips

Diffuse seeps Stockpiles

Construction rocks Concentrate spills

49
 Fig 1

Acid Mine
Drainage

Physical Chemical Biological Ecological Socio-

economical

 Behavioral impacts  Habitat modification  Human health

 Modified substrate  Increased acidity
and sediment  Respiratory impacts  Niche loss impacts
 Reduced pH
geomorphology  Impacts on  Bioaccumulation  Impact outside
 Reduced
reproduction  Loss of food source permit boundary
 Increased stream bicarbonate buffering
velocity  Impacts on  Reduced primary  Increased bond
system
osmoregulation productivity release time
 Increased turbidity  Increased aqueous
 Acid-base imbalance  Reduced species  Cost to prevent,
 Increased contaminant
 Increased toxicity richness and neutralize, isolate,
sedimentation concentration  Migration of animals diversity and remove acids
 Metals adsorbed onto  Increased particulate  Death of sensitive  Altered food chain  Demands funding,
sediments metals species
 Elimination of partnerships,
 Reduced turbulence
sensitive species technology transfer,
and policies

50
Fig. 2

Acidity

Water and
Oxygen Alkalinity

Multiple and
Interactive
Factors Pyrite
Bacteria Affecting Morphology
AMD and
Occurrence

Paleoenvironment pH

51
 Fig. 3

How to address
AMD?

1 2 3 4 5 6
Understanding Getting Assessing the Understanding Implementing
Planning Clean-up
AMD Organized Watershed Treatment Options Plan
Establish priorities
Define AMD Find potential Target problems Target clean-up Identify funding
partners sites
Identify sources Collect Set goals and Finance project
Develop outreach background Identify preventive objectives
Initiate work
information ways and treatment
Form watershed options Develop action-plan Continue
partnership Assess watershed monitoring

52
Fig 4

Acid Mine Drainage

Alkali Selection Alkali Storage and Electrochemical

1. Caustic Soda
Feeding Treatment
2. Soda Ash 1. Direct Feed
3. Limestone Reverse
2. Solution Feed
4. Hydrated Lime 3. Slurry Feed
Osmosis
5. Quicklime
6. Alkaline
Barium
Calcium
Mixing Iron Oxidation Desalination
1. Mechanical 1. Aeration
2. Turbulent 2. Chemical Oxidants
Neutralization
3. Natural 3. Biological
Dissolution Oxidants
Addition of Sulphate
Coagulant Removal
Sedimentation
Sludge
1. Clarifiers
Processing
2. Separators
3. Ponds
53
4. Impoundments Effluent
Fig. 5

Outflow

Water
Inflow Organic Matter/Compost

Limestone Drain

Fig. 6

Highlights
 AMD treatment methods, critical research gaps, challenges, and opportunities are

discussed

54
  Different active and passive treatment systems, and integrated methods are available

 Prevention techniques and integrated management minimize AMD risks

 Effective treatment allows resource recovery and reuse

 Use of UAVs and effective enforcement of discharge standards, performance bonding,

and remediation plans deemed necessary

Table Captions:
Table 1: Coal production, recoverable reserves, domestic consumption, and surface and
underground mining in the United States (2011-2018) (National Mining Association, 2019)
Table 2: Coal Mine Productivity in the US, 1990-2018 (Average Tons per Miner per Hour;
NMA, 2019)
Table 3: Select list of sulfide minerals (USEPA, 1994)
Table 4: Comparison of acid-base accounting with other static tests (USEPA, 1994)
Table 5: Advantages and disadvantages of humidity cells and column test (USEPA, 1994)
Table 6: Caustic chemicals used for neutralization of coal mine drainage and their associated
conversion factors and neutralization efficiencies (Source: Cravotta et al., 2015, 2010; Skousen
et al., 2019)
Table 8: Advantages and disadvantages of active and passive treatments (; Fripp et al., 2000;
Johnson and Halberg, 2005; Skousen et al. 2019)

55
 Table 1: Coal production, recoverable reserves, domestic consumption, and surface and
underground mining in the United States (2011-2018) (National Mining Association, 2019)
2011 2012 2013 2014 2015 2016 2017 2018
Production (1,000 Short 1,095,628 1,016,458 984,842 1,000,049 896,941 728,364 774,609 756,167
Tons)
East of Mississippi 456,447 423,476 407,341 409,521 348,978 281,631 304,430 310,663
River‡
West of Mississippi 639,181 592,983 577,501 590,528 547,963 446,734 470,179 445,504
River

Appalachian‡ 336,017 293,253 271,638 268,603 222,114 180,477 198,545 200,903

Interior 170,327 179,961 182,994 188,604 167,430 143,917 145,194 136,935
Western 587,633 543,244 530,210 542,842 507,397 403,971 430,870 418,329
Refuse Recovery 1,650 1,324 1,966 1,624 1,384 851 699 726
U.S. Recoverable 258,619 257,648 256,709 255,755 254,896 254,197 253,453 252,733
Reserves (Mil. Sht.
Tons)
Recoverable Reserves at 19,223 18,664 19,746 19,351 18,327 16,956 16,101 15,216
Producing Mines
(Million Short Tons)†
Total Value of $44,931,704 $40,607,497 $36,675,516 $34,831,707 $28,549,632 $22,266,087 $26,119,815 $27,214,450
Production ($1,000)
Domestic Consumption 1,002,948 889,185 924,442 917,731 798,115 731,071 716,856 687,994
(1,000 Short Tons)
Electric Utilities/power 932,484 823,551 857,962 851,602 738,444 678,554 664,993 636,498
Coking 21,434 20,751 21,474 21,297 19,708 16,485 17,538 18,312
Other Industrial 46,238 42,838 43,055 42,946 38,459 34,849 33,264 31,512
Residential/Commercial 2,793 2,045 1,951 1,887 1,503 1,183 1,061 968
Exports (1,000 Short 107,259 125,746 117,659 97,257 73,958 60,271 96,953 115,632
Tons)
Imports (1,000 Short 13,088 9,159 8,906 11,350 11,318 9,850 7,777 5,954
Tons)
Number of Mines (EIA) 1,325 1,229 1,061 985 853 710 680 679
Underground Mines 508 488 424 372 324 268 246 249
(includes refuse)
Surface Mines 788 719 637 613 529 442 434 430
Number of Mine 1,973 1,871 1,701 1,632 1,460 1,289 1,216 1,192
Operations (MSHA)
† At active producing coal mines
‡Includes refuse
EIA = Energy Information Administration
MSHA = Mine Safety & Health Administration

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Table 2: Coal Mine Productivity in the US, 1990-2018 (Average Tons per Miner per Hour;
NMA, 2019)

Year Underground Surface

1990 2.54 5.94
1991 2.69 6.38
1992 2.93 6.59
1993 2.95 7.23
1994 3.19 7.67
1995 3.39 8.48
1996 3.57 9.05
1997 3.83 9.46
1998 3.90 9.58
1999 3.99 10.39
2000 4.15 11.01
2001 4.02 10.60
2002 3.98 10.38
2003 4.04 10.76
2004 3.96 10.57
2005 3.62 10.04
2006 3.37 10.19
2007 3.34 10.25
2008 3.15 9.82
2009 2.99 9.22
2010 2.89 9.47
2011 2.72 8.97
2012 2.84 8.97
2013 3.07 9.69
2014 3.35 10.42
2015 3.45 10.95
2016 3.83 10.73

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2017 3.77 10.92
2018 3.68 10.36

Table 3: Select list of sulfide minerals (USEPA, 1994)

Mineral Composition
Pyrite FeS2
Marcasite FeS2
Pyrrhotite Fe1-xS
Chalcopyrite CuFeS2
Chalcocite CuS2
Galena PbS
Millerite NiS
Sphalerite ZnS
Arsenopyrite FeAsS
Cinnabar HgS

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 Table 4: Comparison of acid-base accounting with other static tests (Adapted and modified from
USEPA, 1994)
Acid-base Modified Acid- BC Research Alkaline Net Acid
accounting Base Accounting Initial Production Production
Potential
Acid production determination
Acid Producing Acid Producing Acid Producing Total S is used as Addition of 300 mL
Potential = 31.25 * Potential = 31.25 * Potential = 31.25 * indicator H2O2 to 5 g sample
Total S Total S Total S to directly oxidize
sulfides
Advantages
Simple and rapid; no Simple and rapid; Simple and rapid; Simple and rapid; Simple and rapid;
special equipment no special no special no special no special
required; easy equipment; easy to equipment equipment equipment required;
interpretation; interpret required; easy to required easy to interpret
appropriate for many interpret;
samples appropriate for
many samples
Disadvantages
Fails to relate to Does not relate to Assumes acid/ Moderate ease of Limited
kinetic data; kinetic data; acid/ alkaline release interpretation reproducibility;
assumes acid/ alkaline release parallelly; if APP uncertainty
alkaline release parallelly; if APP and NP are close, depending on
parallelly; if APP and NP are close, difficult to sulfide oxidation
and NP are close, hard to interpret; interpret; does not
difficult to interpret; does not depict depict different
does not depict different particle particle size
different particle size
size

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Table 5: Advantages and disadvantages of humidity cells and column test (USEPA, 1994)
Humidity Cells Column Tests
Advantages
Rapid examination of acid generating Examines acid generating potential and
potential and neutralizing potential than neutralizing potential
column test
Models wet/dry samples Models wet/dry samples
Mimics field condition, although method is Models diverse rocks, and grain sizes, and
not intended to simulate site-specific better representation of field condition
leaching conditions
Disadvantages
Moderate to use Difficult to interpret
Time consuming method Time consuming method
Moderate ease of interpretation Unsuitable for large number of samples
Generates large data set Generates large data set
Requires special equipment and handling Irregular leachate application

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 Table 6: Caustic chemicals used for neutralization of coal mine drainage and their associated conversion factors and neutralization
efficiencies (Source: Cravotta et al., 2015, 2010; Skousen et al., 2019)

Common Chemical Formula Unit Acid CaCO3 Efficiency Conversion Mixing Neutralization Purity of Sludge
name Name Weight equiv- factor factor factor efficiency efficiency industrial density
(g/mol) alents (g/g factor (%) grade (proportion
(eq/mol) CaCO3) chemical solids)
50% Liquid Sodium NaOH 39.998 1 1440 1.0 256 1.0 100 0.99 0.02-0.05
Caustic hydroxide
20% Liquid Sodium NaOH 39.998 1 3276 1.0 784 1.0 100 0.99 0.02-0.05
Caustic hydroxide
Caustic Sodium NaOH 39.998 1 0.80 1.0 0.8 1.0 100 0.99 0.02-0.05
Soda (solid) hydroxide
Soda Ash Sodium Na2CO3 105.991 2 1.06 0.6 1.06 0.6 60 0.99 0.02-0.05
carbonate
Limestone Calcium CaCO3 100.091 2 1.00 0.3 1 0.3 30 0.85 0.05-0.10
carbonate
Hydrated Calcium Ca(OH)2 74.096 2 0.74 0.8 0.74 0.8 90 0.96 0.05-0.10
Lime hydroxide
Pebble Calcium CaO 44.011 2 0.44 0.7 0.56 0.7 90 0.94 0.05-0.10
Quicklime oxide
Ammonia Anhydrous NH3 17.030 1 0.34 0.9 0.34 0.9 100 0.99 0.02-0.05
ammonia

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Table 7: Different caustic chemicals used in active treatment and their advantages and
disadvantages (Skousen et al., 1996; USEPA, 1997)

Advantages Disadvantages
Caustic Soda (NaOH)
High solubility and dispersion Relatively expensive
Applicable to low flows with high acidity Generates ferric hydroxide sludge
Difficult to handle in cold weather due to
freezing
Corrosive
Soda Ash (NaCO3)
Applicable for low flows with low acidity Higher cost
Pellets are fairly easy to handle Mixing required at iron concentration >10
mg/L
Pellets may absorb moisture in hopper system
Armoring occur with iron precipitates
Unstable sludge
Limestone (CaCO3)
Cheap, low handling cost, stable, and safe Under high metal concentration, armoring
occurs, which may affect AMD treatment
Easily available and stored Low solubility and require long-term
application
Handling of sludge with moderate ease Hardness of effluents due to Ca
Hydrated Lime (Ca(OH)2)
Fairly cheap and stable Longer treatment required
Available in solid and liquid forms Extensive mixing required
Effective under extreme conditions Generates sludge/gypsum precipitate under
higher sulfate concentration
Needs proper storage
Quick Lime (CaO)
Cheap Sludge-like-precipitate cause clogging
Applicable for low flows with high acidity Requires metering equipment
Generates heat during slaking, which cause
handling problems
Human health issues (e.g., eye burns)
Longer storage is not recommended
Anhydrous Ammonia (NH3)
Lower cost and stable Human health issues (e.g. eye burns)
Applicable for small flows Needs proper handling and monitoring
Can remove Manganese

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Table 8: Advantages and disadvantages of active and passive treatments (Fripp et al., 2000; Gar
Garcia-Valero et al. 2020; Johnson and Halberg, 2005; Skousen et al. 2019)
Active Treatment Passive Treatment
Advantages
Low capital cost Low operating cost
Flexible Periodic maintenance
Relatively controlled Less supervision
Effects are more uniform
Governed by pseudo-natural process
Disadvantages
High operating cost High capital cost
Higher and frequent maintenance Less flexible
Higher supervision; affected by Lower control
weather, equipment failure, among
others
Needs proper handling and disposal of Forms ferrous carbonate and manganous
sludge produced carbonate gels

63
Interest Statement/Disclaimer
The authors are responsible for the views expressed in this paper and do not necessarily represent

or reflect the views and policies of the Oklahoma Department of Mines.

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Acid Mine Drainage from Coal Mining in the United States ─An

Overview

Abstract

Water discharged from active, abandoned and/or reclaimed coal mine sites with relatively higher acidity

continues to be a global concern due to variable impacts on the quality of surface water and groundwater.

Treatment of such acid mine drainage (AMD) is often complex, costly and challenging. Towards this end,

this review provides an overview of the formation and effects of AMD, reviews prediction and treatment

methods, identifies critical research gaps, and explores the associated challenges and opportunities AMD

poses for environmental scientists and researchers. Acid drainage occurs through oxidation of sulfide

minerals such as pyrite. The main sources of AMD include runoff and seepage from mine rock dumps,

open pit mines, stockpiles, tailings, construction rocks, and rock cuts. While different active and passive

treatment systems are available to treat AMD, prevention techniques and integrated management

approaches could better identify possible risks, abate treatment costs, and reduce eco-hydrological

hazards. Also, the coal mining sector could benefit from remote and ground sensing techniques, including

the use of unmanned aerial vehicles and hyperspectral imaging for hydrogeochemical investigations.

Effective treatment of acid drainage from mine areas reduces material damage, allows resource reuse and

recovery, and enables successful post-mine land use. Environmental scientists must, however, design and

implement a proper framework to address AMD in a timely manner. While mining and treatment plans

may vary with land-use history, climate, topography, hydrogeology, available technology, and socio-

political outlooks, environmental scientists and mining companies must make it a priority to form

multidisciplinary partnerships, advocate for effective enforcement of discharge standards, encourage

performance bonding, and formulate remediation plans.

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