AGRICULTURAL WASTEWATER TREATMENT USING CONSTRUCTED

WETLAND WITH NITROGEN-PHOSPHORUS RECOVERY

THROUGH STRUVITE CRYSTALLIZATION

I. INTRODUCTION

Overpopulation contributes to the emergence of agricultural innovations. Some of which

is the use of fertilizers and pesticides to produce quality crops. The Philippines where agriculture

serves as a main source of economic rise had been greatly reliant to both synthetic fertilizers and

pesticides. The utilization these chemicals compromised the safety of the environment but its used

cannot be prevented due to the high grade crop yield it offers.

According to the recent Food and Agriculture Organization of the United Nations data,

between 1961 and 2005 fertilizer applications in the Philippines increased by 1000%. In general,

the excessive and inappropriate use of chemical fertilizers in crop soils cause land degradation and

losses in soil fertility worldwide. Moreover, agrochemicals cause water pollution that directly and

indirectly affects human health. According to the National Economic and Development Authority,

37% of the total water pollution originates from agricultural practices, which include animal waste

and fertilizer and pesticide runoff. Water pollution from nitrates derived from fertilizer runoff is

more widespread in the Philippines than previously thought (Tirado et. al, 2008).

A possible solution to handle this problem without restricting the use of chemicals in

agriculture is to design a process that would enable the treatment of wastewater produced and

possibly the recovery of nutrients. This research focuses on selecting a wastewater treatment and

nutrient recovery process for agricultural wastewater. Integration of these processes is the main
objective of this study as well as to design a control process for the selected treatment and recovery

system.

Specifically, it aims to:

1. To make a comparative study on the different agricultural wastewater treatment and

nutrient recovery technologies.

2. To treat agricultural wastewater by reducing its BOD concentration.

3. To recover N and P nutrients from agricultural wastewater;

4. To design a control process for the selected treatment and recovery system.
II. REVIEW OF RELATED LITERATURE

A. Wastewater

The Philippine environment is exposed to a lot of various pollutant sources and 37% of

which is from agricultural wastewater. One of its negative impact to the environment is its effect

to water reservoirs like freshwater. As presented from the data of Environmental Management

Bureau (EMB), Philippines showed that out of the 127 freshwater bodies being sampled, 47%

percent were found to have good water quality. However, 40% of those sampled were found to

have only fair water quality, while 13% showed poor water quality (Claudio, 2015).

Sources of agricultural wastewater are the excess water that runs off the field at the low

end of furrows and effluent from plants processing crops. The effluents from agricultural regions

contains high organic matter, salts, nutrients, pesticides, herbicides, and other agricultural

chemicals which are harmful in the environment when discharged (CAWSI).

Excessive and inappropriate use of chemical fertilizers in crop soils cause land degradation

and losses in soil fertility worldwide. In addition, agrochemicals cause water pollution that directly

and indirectly affects human health. According to the National Economic and Development

Authority (NEDA), 37% of the total water pollution originates from agricultural practices, which

include animal waste and fertilizer and pesticide runoff. Water pollution from nitrates derived from

fertilizer runoff is more widespread in the Philippines than previously thought (GreenPeace).

B. Wastewater Treatment Technology

Physical, chemical, and biological methods are used to remove contaminants from wastewater.

In order to achieve different levels of contaminant removal, individual waste water treatment

procedures are combined with variety of systems. More rigorous treatment of waste-water includes

the removal of specific contaminants as well as the removal and control of nutrients.
1. Terrestrial Treatment Technologies

Terrestrial treatment systems include slow-rate overland flow, slow-rate subsurface

infiltration, and rapid infiltration methods. In addition to wastewater treatment and low

maintenance costs, these systems may yield additional benefits by providing water for

groundwater recharge, reforestation, agriculture, and/or livestock pasturage. They depend

upon physical, chemical, and biological reactions on and within the soil. Slow-rate

overland flow systems require vegetation, both to take up nutrients and other contaminants

and to slow the passage of the effluent across the land surface to ensure maximum contact

times between the effluents and the plants/soils. Slow-rate subsurface infiltration systems

and rapid infiltration systems are "zero discharge" systems that rarely discharge effluents

directly to streams or other surface waters. Each system has different constraints regarding

soil permeability. Although slow-rate overland flow systems are the costliest of the natural

systems to implement, their advantage is their positive impact on sustainable development

practices. In addition to treating wastewater, they provide an economic return from the

reuse of water and nutrients to produce marketable crops or other agriculture products

and/or water and fodder for livestock. The water may also be used to support reforestation

projects in water-poor areas. In slow-rate systems, either primary or secondary wastewater

is applied at a controlled rate, either by sprinklers or by flooding of furrows, to a vegetated

land surface of moderate to low permeability. The wastewater is treated as it passes through

the soil by filtration, adsorption, ion exchange, precipitation, microbial action, and plant

uptake. Vegetation is a critical component of the process and serves to extract nutrients,

reduce erosion, and maintain soil permeability.

 Overland flow systems are a land application treatment method in which treated

effluents are eventually discharged to surface water. The main benefits of these systems

are their low maintenance and low technical manpower requirements. Wastewater is

applied intermittently across the tops of terraces constructed on soils of very low

permeability and allowed to sheet-flow across the vegetated surface to the runoff collection

channel. Treatment, including nitrogen removal, is achieved primarily through

sedimentation, filtration, and biochemical activity as the wastewater flows across the

vegetated surface of the terraced slope. Loading rates and application cycles are designed

to maintain active microorganism growth in the soil. The rate and length of application are

controlled to minimize the occurrence of severe anaerobic conditions, and a rest period

between applications is needed.

2. Sequencing Batch Reactor

Sequencing Batch Reactors (SBR) are special forms of activated sludge treatment

in which all of the treatment process takes place in the reactor tank and clarifiers are not

required. This process treats the waste water in batch mode and each batch is sequenced

through a series of treatment stages.

Table 1. Typical SBR Process

STEPS DESCRIPTION
 Waste water fills the tank, mixing with biomass that

settle during the previous cycle.

Air is added to the tank to aid biological growth and

facilitate subsequent waste reduction

Mixing and Aeration stops during this stage to allow

solids settle to the bottom of the tank

Clarified effluent is discharged.

If necessary, sludge removal occurs during this stage

SBR reactors treat waste water such as sewage or output from anaerobic digesters

or mechanical biological treatment facilities in batches. Oxygen is bubbled through the

waste water to reduce biochemical oxygen demand (BOD) and chemical oxygen demand

(COD) to make suitable for discharge into sewers or for use on land. While there are several

configurations of SBRs the basic process is similar. The installation consists of at least two

identically equipped tanks with a common inlet, which can be switched between them. The

tanks have a “flow through” system, with raw wastewater (influent) coming in at one end

and treated water (effluent) flowing out the other. While one tank is in settle/decant mode

the other is aerating and filling. At the inlet is a section of the tank known as the bio-

selector. This consists of a series of walls or baffles which direct the flow either from side

to side of the tank or under and over consecutive baffles. This helps to mix the incoming
 influent and the returned activated sludge, beginning the biological digestion process

before the liquor enters the main part of the tank.

3. Adsorption/ Bio-oxidation Process

The adsorption process uses forces of molecular attraction to bind soluble and

gaseous chemicals to a surface. The process retains and accumulates toxic chemicals

present in wastes, yet does not chemically alter them. Carbon used for adsorption is usually

treated (activated) to make it very porous. Activated carbon has a large surface area that

can adsorb relatively large quantities of material per unit weight of carbon. It is “spent”

when it has adsorbed so much contaminant that its adsorptive capacity is severely depleted.

Activated carbon filters are widely used to produce drinking water at household

and community level (to remove certain organics, chlorine or radon from drinking water)

and to treat industrial or municipal wastewaters. It is not efficient for disinfection and

nitrates removal. Adsorption on activated carbon is a simple technology based on materials

such as fossil fuels and even agricultural waste.

4. Membrane Bioreactor Technology

Membrane Bioreactors (MBRs) can be broadly defined as systems integrating

biological degradation of waste products with membrane filtration. They have proven quite

effective in removing organic and inorganic contaminants as well as biological entities

from wastewater. Advantages of the MBR include good control of biological activity, high

quality effluent free of bacteria and pathogens, smaller plant size, and higher organic

loading rates. MBRs also can be achieve effective removal of nitrate, herbicides, pesticides,

and endocrine disrupting compounds.

 The principle of this process is that instead of separation, the sludge and water

settles. The MBR method uses the membrane which is more efficient and less dependent

on oxygen concentration of the water. It eliminates process difficulties and problems

associated with settling, which is usually the most troublesome part of wastewater

treatment. The potential for operating the MBR at very high sludge ages without having

the obstacle of settling, allows high biomass concentrations in the bioreactor.

Consequently, higher strength wastewater can be treated and lower biomass yields are

realized (Muller et al., 1995).

Figure 1. Flowchart of Membrane Bioreactor (Cicek, 2002)

5. Electrolysis

Electrolysis is an electrochemical wastewater treatment technology that is currently

experiencing both increased popularity and significant technical improvement. It is a

complex process involving many chemical and physical phenomenon that use consumable

electrodes to supply ions into the wastewater. In the process, the coagulant is generated in

situ by electrolytic oxidation of Fe and Al electrode as an anode material which produces

ions continuously in the system. The released ions neutralize the charges of the particles
 and thereby initiate coagulation. These ions may remove the undesirable contaminants

(metal hydroxide and metal phosphate flocs generated within the effluent) either by

chemical reaction and precipitation or by causing the colloidal materials to coalesce and

are then removed by EF, (Chopra et. al,2011).

The main processes occurring during electrolysis are electrolytic reactions at the

surface of electrodes, formation of coagulants in aqueous phase, adsorption of soluble or

colloidal pollutants on coagulants, and removal by sedimentation and floatation. The main

reactions at the electrodes are as follows,

Al  Al 3  3e  (at anode)
3H 2 O  3e   3
2 H 2  3OH  (at cathode)

The destabilized particles then aggregate to form flocs. In the meantime, tiny

hydrogen bubbles produced at the cathode induce the floatation of most flocs, helping to

effectively separate particles from wastewater. In addition, the cathode may be chemically

attacked by OH− ions generated together with H2 at high pH values.

6. Constructed Treatment Wetlands

Constructed wetlands (CWs) are engineered systems that have been designed and

constructed to utilize the natural processes involving wetland vegetation, soils, and the

associated microbial assemblages to assist in treating wastewaters. They are designed to

take advantage of many of the same processes that occur in natural wetlands, but do so

within a more controlled environment. Constructed treatment wetlands is a reliable

treatment technology which can be applied to all types of wastewater including sewage,
 industrial and agricultural wastewaters, landfill leachate and stormwater runoff. All types

of constructed wetlands are very effective in removing organics and suspended solids,

whereas removal of nitrogen is lower but could be enhanced by using a combination of

various types of CWs. Removal of phosphorus is usually low unless special media with

high sorption capacity are used. Constructed wetlands require very low or zero energy input

and, therefore, the operation and maintenance costs are much lower compared to

conventional treatment systems.

Figure 2. The Major Characteristics of various types of Constructed Wetlands for

wastewater treatment, H = horizontal, V = vertical.

C. Nutrient Recovery Techniques

Nutrient recovery is a process that enables the removal and concentration of nutrient by-

products from agricultural manures or anaerobic digestate (the output from anaerobic digesters).

Nutrient recovery technologies (NRTs) can facilitate improved nutrient management on

agricultural operations with excess nutrients. NRTs produce a concentrated nutrient by-product

that may more easily be transported off-farm and/or potentially transformed into a commercially

saleable nutrient product.

1. Mechanical Recovery Technologies

A widely used type of manure and digestate management technology in Europe and

North America is mechanical recovery, in which screens, screw or belt presses are used.

These technologies remove the larger fibers in manure and digestate, which if sufficiently

cleaned, can be re-used for bedding. Used on dairy farms in both Europe and North

America since the 1970s to reduce bedding costs, maximize liquid storage, and make

manure storage, handling and transportation easier, the N and P recovery abilities of these

technologies are low (~10 – 20% total N and P).

Over 85% of P in manure and digestate is bound to small suspended solids (Gungor

& Karthikeyan, 2008). Therefore, to increase P recovery, advanced mechanical NRTs such

as centrifuges, membranes and dryers have been developed. Centrifuges spin at high speeds

to create a strong centripetal force that separates materials of different densities, such as

suspended solids from liquids. Membranes act as a filter, letting liquids flow through while

catching suspended solids and other substances. Dryers evaporate the water, leaving behind

solids. These advanced mechanical NRTs have a much higher nutrient recovery potential

than screens, screw or belt presses.

2. Chemical Recovery Technology

A widely adopted chemical NRT is flocculation, whereby flocculants (also known

as coagulants), or polymers are used to bind together the small suspended solids in manure

and digestate, making them easier to collect and separate. Once separated, the suspended
 solids can be dewatered using mechanical technologies such as screw or belt presses to

increase DM content.

A second type of chemical NRT is struvite precipitation. The basic principle

underlying struvite precipitation is that in high pH environments where magnesium,

ammonia and phosphate are present, crystal struvite (magnesium ammonium phosphate

precipitate) forms. Historically, and due to the presence of calcium-P precipitate in dairy

manure, poor struvite crystallization performance has been observed. However, recent

technology modifications have resulted in much improved performance with both dairy

manure and digestate.

3. Biological Recovery Technology

A biological NRT is ammonia-N stripping, where soluble ammonia becomes

gaseous at certain temperatures and pH ranges. Achievement of the required temperature

and pH, and subsequent stripping of ammonia gas, can be accomplished through a variety

of techniques. Once the soluble ammonia is in a gaseous form, it can be recovered/re-

adsorbed in a solution or crystalline form. Suspended solids and P can then be removed

from the effluent. This technology is a better fit with digestate than manure, as AD

increases both pH and the proportion of N in ammonia form, and often provides excess

heat which can be used in the stripping process (Yanosek, 2002).

A second type of biological NRT widely used in municipal wastewater processing

is Enhanced Biological P Removal (EBPR) through consumption of P (and other nutrients,

e.g. Mg) by P-accumulating Organisms (PAOs). By storing P in greater quantities than

needed for their own cell components, these organisms concentrate P in their biomass,
 creating a sink for P which can be more easily collected. Once collected, P in the biomass

still requires separation before it can be used.10 As EBPR requires readily biodegradable

carbon, which is destroyed during AD to make biogas, this approach is unsuitable for

digestate (Ahn,, Park, & Park, 2007).

4. Struvite Crystallization

Struvite is notable for its production of a preferred product that is already pelleted,

mostly dry and quite balanced in fertilizer property. As a consequence, it is easily spread

using existing fertilizer application methods (Ma, Kennedy, Yorgey, & Frear, 2013).

P can also be recovered by crystallization in the form of struvite (MgNH4PO4 .

6H2O) ( (Battistoni, Paci, Fatone, & Pavan, 2006). Effective performance has been seen in

large-scale studies while treating swine manure (~80% TP removal; (Bowers &

Westerman, 2005)). However, several factors can affect struvite precipitation, including

pH, super-saturation of the three ions in the solution, and the presence of impurities (e.g.,

calcium), which can cause the formation of calcium-P precipitates (Le Corre,, Valsami-

Jones,, Hobbs, Jefferson, & Parsons, 2007). As dairy manure contains these calcium-P

precipitates, poor performance has been observed when using dairy manure, particularly

digested dairy manure (~15% TP removal) (Zhang, Bowers, Harrison, & Chen, 2010).

However, modifications to the struvite crystallization process have allowed for enhanced

removal efficiency (~75% TP removal) (Zhang, Bowers, Harrison, & Chen, 2010).
 Figure 3. Struvite Crystallizer, Qualco, Monroe WA (MFH, 2013)
Figure 3 shows a pilot-scale struvite crystallizer with process modifications

required for treatment of a portion of the digested dairy manure. The product of the

crystallizer is quite dry and pelletized form that allows for easy storage, transportation, and

application with existing fertilizer systems. Both digested and undigested manures can be

treated with removal efficiencies of 75% for total P and 10% for total N. The total system

performance is roughly 85-90% total P and 25-35% total N (MFH, 2013).

D. Process Selection

Nonpoint source pollution from farms is caused by surface runoff from fields during

precipitation events. According to the U.S. Environmental Protection Agency (2005), agricultural

runoff is a major source of pollution. Non-point source pollution, especially from agriculture,

remains as one of the principal water quality problems that need to be addressed (Hammer et al.

1993) Runoff from crop fields, barnyards and feedlots and the discharge of contaminated process

water can introduce significant amounts of unwanted nutrients and other pollutants into the

environment if it is not captured and properly treated. (Loehr, 1974).

Pesticide use is most prevalent kind of nonpoint source pollution. Pesticides are often

detected in surface waters (Anderson, 2005) and groundwater. According to Wikipedia, pesticides

may appear in surface water due to: direct application (e.g. aerial spraying or broadcasting over

water bodies), runoff during rain storms, and aerial drift (from adjacent fields). Nitrogen and

phosphorus are key pollutants found in runoff, and they are applied to farmland in several ways,

such as in the form of commercial fertilizer, animal manure, or municipal or industrial wastewater

(effluent) or sludge. These chemicals may also enter runoff from crop residues, irrigation water,

wildlife, and atmospheric deposition. (U.S. Environmental Protection Agency, 2003)

When wastewater is treated using physical and chemical means, usually a coagulant is

added which removes suspended solids, phosphorus, and some dissolved organics. The resulting

product is then settled or filtered before release. Considerable quantities of sludge are produced in

this process and the organic material is bound to the coagulant rather than being oxidized and

removed. In contrast, biological treatment will involve some physical and chemical processes

(such as adsorption, settling, precipitation, and filtration), but will also process different

compounds into other products. Biological treatment is also a highly unfavorable environment for
pathogenic microbes and their removal can proceed faster than in biologically inactive systems.

However, selected process will not be any of the typical biological treatment units used by

municipal treatment plants (e.g., anaerobic, partly aerobic, and aerobic oxidation ponds) since they

rely on a limited set of microorganisms mainly composed of bacteria and bacterial grazers

(protozoans). The units that will be dealt with in the process selected will have these components

and, in addition, will introduce structure (soil or gravel material) and higher plants, which will

provide both structure and increased surface area for microbes to attach to as well as performing

treatment functions in their own right. (Peterson, 1998)

Constructed wetlands (CW) are a treatment option for agricultural wastewater. They are

engineered systems that use natural functions such as vegetation, soil, and organisms to treat

wastewater. Their ability to adequately function continues to be evaluated as they are biologically

active systems that depend on microbial and plant activity. (Rozema et. al, 2016). According to

various studies conducted by Knight et. al, (2000), Werker at. Al, (2002), and Vyzamal (2010),

CWs are a relatively inexpensive and low-maintenance option for agricultural applications and are

capable of treating a number of wastewater types. CWs are engineered to optimize naturally

occurring biological, chemical, and physical processes to treat wastewaters. (Rozema et. al, 2016).

Constructed wetlands can be classified into two types: surface flow wetlands (SF) and sub-surface

flow wetlands (SSF). Surface flow systems will have an open water surface as part of the wetland.

The advantage of these types of wetlands is a low risk of clogging, but treatment efficiency for

some components is sacrificed because of lower substrate to pollutant interactions. Some

components can, however, be effectively treated in surface flow wetlands, notably ammonia and

phosphorus (Kadlec and Knight 1996). In contrast to natural wetlands, constructed wetlands can

be designed with a host of features that improve treatment efficiency. The most effective is the
addition of subsurface flow. In these systems, the water needs to take a tortuous path through a

particulate medium, usually gravel, sand or stones, which is interspersed with roots from vascular

aquatic plants. Commonly and frequently used plants for the reed beds include common water

hyacinth, pontederia, cattail, and common reed. The aim with these systems is to provide

interaction between substrate and pollutant to improve treatment efficiencies.

For the nutrient recovery, P can be recovered by crystallization in the form of struvite

(MgNH4PO4 . 6H2O) ( (Battistoni, Paci, Fatone, & Pavan, 2006). Effective performance has been

seen in large-scale studies while treating swine manure (~80% TP removal; (Bowers &

Westerman, 2005)).

Table 1. Summary of performance and cost estimates with partial list of concerns and scale tested
for representative class of P recovery approaches (Ma, Kennedy, Yorgey, & Frear, 2013)
Key Technology Performance Operating Cost Capital Cost Scale
Primarily P
Mechanical Screens TN 15-30%, 260-312 Php 1,664-1,872 Php Commercial
TP 15-25%
Sequential TN 45-55%, 1,300-3,900 Php 6,760-7,800 Php Commercial
Screening TP 75-90%
w/Advanced
Chemical
Struvite TN 30%, 4,680-5,720 Php 5,200-7,800 Php Commercial
Crystallization TP 75%
Enhanced Biological TP 42-91% 7,800-8,840 Php 14,300-15,600 Pilot
Phosphorus Php
Table 2. Nutrient Recovery Performance and Cost (British Columbia Ministry, 2013)

Technology type N% Recovery P% Recovery Cost

Mechanical 20 54 22,880 Php
Recovery
Chemical 30 90 33,800 Php
Recovery
Struvite 20 90 20,280 Php
Crystallization
Biological 50 0 16,120 Php
Recovery

Table 1 and 2 summarize the four main classes of approaches to Phosphorus and

Nitrogen recovery with estimated performance and costs ranges. In general, as P removal

improves, costs also increase. Also, while large pore size screening leads only to limited

removal (15-30%), methods that allow for recovery or absorption of small particle sizes

achieve near-maximum recovery of P (75-90%). While various methods can be utilized for

P recovery, it is clear from full-scale demonstrations that Struvite Crystallization is most

recommended in terms of cost requirement with higher efficiency near to Chemical

Recovery Technique.

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