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Abstract: This paper presents the results of an experimental study of the effects of porosity on the flow rate and Escherichia coli (E. coli)
filtration characteristics of porous ceramic water filters (CWFs) prepared without a coating of silver. Clay-based CWFs were fabricated by
sintering composites of redart clay and fine woodchips (sawdust) in three different proportions by volume, viz: 50∶50, 65∶35, and 75∶25.
Sintering the greenware below 1,000°C produced reddish colored pot of three different degrees of porosity and micro- and nanoscale pores,
which are the key to efficient filtration. The porosities and pore size distribution frequencies of the sintered clay ceramics were characterized
using mercury intrusion porosimetry (MIP). The porosity of the CWFs ranged from ∼36% to ∼47% and increased with increasing sawdust
content in a linear fashion, and the pore size varied from ∼10 nm to ∼100 μm. The volume flow rates of water through the CWFs were
investigated by measuring the cumulative amount of water flow as a function of time. The flow rate was found to increase with increasing
porosity of the CWFs. The effective intrinsic permeabilities of the CWFs were then obtained from Darcy fits to the flow rate data. These
were compared with values obtained using the Katz-Thompson method. Both approaches gave comparable results of permeability
between ∼1 millidarcy to ∼50 millidarcy. The tortuosity of the CWFs was found from Hager’s equation to range from ∼10 to ∼60.
In general, while the permeability of the CWFs decreased with increasing clay content, tortuosity increased with increasing clay content.
The CWFs removed E. coli from aqueous suspension very efficiently with average log reduction values between 5.7–6.4. The implications
and limitations of the results are discussed for the effective filtration of water in the developing world. DOI: 10.1061/(ASCE)EE.1943-7870
.0000669. © 2013 American Society of Civil Engineers.
CE Database subject headings: Filters; Flow rates; Permeability; Filtration; Porosity.
Author keywords: Ceramic water filters; Porosimetry; Flow rate; Intrinsic permeability; Tortuosity; E. coli filtration.
1 5
Lecturer, Dept. of Mechanical and Aerospace Engineering and the Undergraduate Student, Dept. of Chemical Engineering, Princeton
Keller Center for Innovation in Engineering Education, Princeton Univ., Univ., Princeton, NJ 08544. E-mail: kcfriedman@alumni.princeton.edu
6
Princeton, NJ 08544. E-mail: iyakub@princeton.edu Associate Professor, Dept. of Physics, Kyambogo Univ., P.O. Box 1,
2
Assistant Professor, Indian Institute of Technology Jodhpur (IITJ), Kampala, Uganda. E-mail: ksobwoya@yahoo.co.uk
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Rajasthan 342011, India; formerly Graduate Student, Dept. of Food, Agri- Senior Lecturer, Dept. of Physics, Univ. of Nairobi, P.O. Box 30197-
cultural and Biological Engineering, Ohio State Univ., 590 Woody Hayes 00100, Nairobi, Kenya. E-mail: fnyongesa@unonbi.ac.ke
8
Dr., Columbus, OH 43210. E-mail: anand.plappally@gmail.com Professor, Dept. of Water and Sanitation, International Institute for
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Assistant Professor, Dept. of Mechanical and Aerospace Engineering, Water and Environmental Engineering (2iE), Ouagadougou, Burkina Faso.
GeorgeWashingtonUniv.,Washington,DC20052.E-mail:mleftwich@gwu.edu E-mail: amadou.hama.maiga@2ie-edu.org
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Lecturer and Research Specialist II, Dept. of Mechanical and Aerospace En- Professor, Dept. of Food, Agricultural and Biological Engineering,
gineering,PrincetonUniv.,Princeton,NJ08544.E-mail:kmalates@princeton.edu Ohio State Univ., 590 Woody Hayes Dr., Columbus, OH 43210.
Note. This manuscript was submitted on February 15, 2012; approved E-mail: soboyejo.2@osu.edu
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on October 18, 2012; published online on October 19, 2012. Discussion Student, Montgomery High School, Skillman, NJ 08558. E-mail:
period open until December 1, 2013; separate discussions must be sub- stob50@myway.com
mitted for individual papers. This paper is part of the Journal of En- 11
Professor, Dept. of Mechanical and Aerospace Engineering, Princeton
vironmental Engineering, Vol. 139, No. 7, July 1, 2013. © ASCE, ISSN Univ., Princeton, NJ 08544 (corresponding author). E-mail: soboyejo@
0733-9372/2013/7-986-994/$25.00. princeton.edu
has helped to establish water filter factories in over 20 countries, of microbial contaminants could be assessed in the absence of the
including: Mexico, Cambodia, Haiti, Guatemala, El Salvador, antimicrobial effect of silver.
Pakistan, Sudan, Kenya, Benin, Ghana and Nigeria (Brown et al. The effects of porosity are explored using ceramics produced
2009; Dies 2003; Donachy 2004; Hwang 2003; Lantagne 2002; from different, well-controlled mixtures of redart clay and wood
Lantagne et al. 2010; Lee 2009; Oyanedel-Craver and Smith 2008; chips. The effective permeabilities of the CWFs were determined
PFP 2008; Swanton 2008; Van Halem 2006). In an effort to en- from fits to the Darcy equation and also by using the Katz and
hance the availability of the filters across borders in the developing Thompson method. The tortuosity of the CWFs was found using
world, the filter has not been patented. Jörgen Hager’s equation. The efficiencies of bacterial removal
Although there are other methods for the treatment of water in (filtration) were elucidated for two of the three CWFs. The impli-
developing countries [boiling, pasteurization, chlorination, floccu- cations of the results are then discussed for applications of CWFs in
lation disinfection, solar disinfection, biosand filter (Clasen et al.
the developing world.
2007; Fewtrell et al. 2005; Sobsey et al. 2008)], point-of-use filtra-
tion is one of the most promising solutions available (Sobsey et al.
2008). Ceramic water filters (CWFs) are especially appealing be-
cause of their low cost, ease of fabrication and use, and their ability Experimental
to filter out bacteria from water very effectively. CWFs are also
attractive because they represent a sustainable solution with the Materials and Processing
potential for large scale adoption. So far, about 500,000 people in CWFs were made by mixing clay (Cedar Heights Redart Airfloated
the developing world have adopted some form of porous ceramic Clay, Pittsburgh, PA) composed of illite and kaolinite clays with
filter technology (Sobsey et al. 2008).
sawdust consisting of 80% oak and 20% Spanish cedar (Hamilton
Clay-based ceramic water filters (CWFs) are usually produced
Building Supplies, Trenton, NJ). In order to produce filters with
by mixing of clay, sawdust (woodchips) and water. Other combus-
different porosities, three different proportions of clay to sawdust
tible organic materials, such as rice husk, coffee husk, or flour can
by volume (50∶50, 65∶35, and 75∶25) were used to produce
also be used (Oyanedel-Craver and Smith 2008). After drying and
the CWFs.
firing, the CWFs are usually coated with a layer of colloidal silver
Prior to mixing, the sawdust was manually sieved using
(PFP 2008), which is used because of its antimicrobial activity.
35–1,000 mesh wire sieves. The initial blending of sieved sawdust
By careful control of the clay and woodchip mixtures proportions,
and clay was then done manually to ensure a thorough mixing and
as well as the processes that are used for the fabrication of CWFs,
initial water flow rates of around 2 L outflow, in the first hour, have to avoid the formation of clustered pores. The dry mixture of clay
been shown consistently to result in the removal of many microbes and sawdust was transferred to an industrial mixer (Model A-200,
and pathogens in water (Brown et al. 2008; Lantagne 2002; The Hobart Manufacturing Company, Troy, OH) and thoroughly
Lantagne et al. 2010; PFP 2008). The flow rate, which may depend mixed again for approximately 5 minutes before the addition of
on the water turbidity conditions, decreases gradually with increas- water. Half (0.9 L) of the required amount of water (usually
ing filter use during the 2–3 year recommended lifetime of the 1.8–2 L for a 50∶50 CWF) was gradually added during mixing,
CWFs. This is due to the accumulation of solids on the inner and the mixture was again blended for 5–10 minutes. Next, half of
surface and gradual blockage of the pores by trapped contaminants the remaining water (one quarter of the total amount or 0.45 L) was
(Brown et al. 2008). During use, PFP recommends that the CWF added, and the mixture was mixed for another 5–10 minutes. The
be cleaned by fire heating, scrubbing and brushing to remove caked remaining water (approximately 0.45 L) was added in small incre-
impurities that form with time. This cleaning procedure, however, ments until the mixture began to coalesce into large clumps and no
is currently under debate because of the high risk of recontaminat- longer adhered to the walls of the mixer. No additional water was
ing treated water (personal communication, Reviewer #1, Jour added after coalescence occurred.
Environ Eng). Approximately 12 pounds of the blended mixture were then
Furthermore, the clay-water mixture has a rheological property, manually formed into a ball, which was pressed tightly together
which not only permits shaping, but also allows for doping with so that no cracks were visible on its surface. This ball was com-
other materials. Doping can potentially give the CWFs the robust- pacted in a two-piece aluminum mold that was covered with a
ness required for the removal of other contaminants besides 49.21 L (13 gallon) plastic bag to prevent the greenware from stick-
microbes from water. For instance, the removal of chemical con- ing to the walls of the mold during pressing. The blended mixture
taminants, such as arsenic, iron, and fluoride has also been reported was placed into the female part of the mold before applying a pres-
(Dies 2003; Friedman 2010; Yakub and Soboyejo 2013). Further- sure of 140 kPa (20 psi) to the male part of the mold using a 50 ton
more, it has also been shown that with the right amount of iron hydraulic press (TRD55002, Torin Jacks, Inc., Ontario, Canada).
(or disc part) and the side. The disc had a radius of ∼91.5 mm
and a thickness of ∼15 mm. The side had an interior slanted
Engineering Incorporated, Stamford, CT). The load cell was
height of ∼240 mm and a thickness of ∼10 mm. The CWFs had
connected to a LabView card (NI PCI-6259, National Instruments,
an interior depth of ∼237 mm and hence have a capacity of
Austin, TX) via a 68-pin digital and trigger I/O terminal block
about 10 L.
(CB-68LP, National Instruments, Austin, TX) to LabView soft-
After cooling, the porosities of the CWFs were characterized
ware (Version 8.0, National Instruments, Austin, TX) that re-
using mercury intrusion porosimetry (MIP). The flow rates and
corded the mass of the water as it flowed into the collection
bacterial filtration characteristics of the filters were also deter-
bucket.
mined. A standard PFP reference CWF, produced by Potters for
At the start of each experiment, a water-saturated CWF was
Peace in Managua, Nicaragua, was used as a reference in the
filled completely with approximately 10 Liters of purified water
porosimetry and flow tests. The PFP reference CWF was made
and covered with a plastic lid. The water was allowed to drain pas-
from a 60∶40 mixture of clay to sawdust by volume. This was also
sively from the CWF being tested. No additional water was added
coated with colloidal silver, and had a flow rate of between
to the CWF during the experiment. In this way, time durations
∼1–2 L per hour. This flow rate was estimated by measuring the
between 3 and 21 days were required to drain the range of CWFs
volume of water that drained from an initially full filter over a
examined in this study.
period of 1 h. A more accurate dynamic method of measuring the
water flow rate will be presented in section 2.4 below.
Modeling
Porosity and Pore Size Distribution An analytical hydrodynamic model was developed to describe
the flow of water through the filters due to the effect of gravity.
The porosities of the CWFs were characterized using mercury Flow continued until the filter had emptied to levels where there
intrusion porosimetry (MIP). MIP measurements were carried was not enough pressure head to overcome the resistance of the
out in a MicroMetrics Autopore III 9400 analyzer (MicroMetrics, membrane/filter. Fig. 1 is a schematic of the water filter with
Norcross, GA). The two-stage MIP experiments were used to char- the important variables labeled. Flow through the porous filters
acterize the nano- and the microscale pore size distributions. The was assumed to follow Darcy’s Law, which is given by (Bear
MIP tests were performed by filling up a penetrometer, with a stem 1972)
volume of 1.131 mL, with pieces of ceramics with dimensions of
∼3 mm × 3 mm × 3 mm that were cut from the three different κA
Q¼ Δp ð1Þ
CWFs (50∶50, 65∶35 and 75∶25) and also the PFP reference CWF. μL
Samples were cut from four different locations in each CWF [the
base and three locations (the top, middle, bottom) on the side of the where Q = flow rate; κ = permeability of the material; A = surface
filter], as shown in Fig. 1. area; L = thickness of the material; μ = dynamic viscosity of
the fluid; and Δp = pressure difference from the top to the bot-
tom of the surface. In this case, the bottom and sides of the
Water Flow Experiments filter are considered separately (denoted Qb and Qs , respectively)
Prior to the water flow experiments, the CWFs were saturated by and the corners are neglected. The pressure change between the
complete submersion in a vat containing purified water (Model surfaces is equal to the hydrostatic pressure of the water (as the
D8611, Barnstead/Thermolyne, Hampton, NH) for about 12 hours flow is very slow, a quasi-steady approximation is appropriate).
to remove internal air bubbles. The flow rates of purified water For the flow through the bottom, the change in pressure from
were then measured through the three CWFs (50∶50, 65∶35, and the inside bottom surface to the outside bottom surface (the
75∶25). Flow rates across the PFP reference filter CWF were also distance of porous media through which the water flows) is
determined as a control. The flow rates were obtained by measuring equal to the hydrostatic pressure of the fluid at that time. This
the volume of water discharged from the CWFs as a function is given by
of time. The flow measurement system was enclosed in a plastic Δp ¼ ρghðtÞ ð2Þ
container to minimize possible contamination and mass loss by
evaporation. where hðtÞ = height of water above the base of the filter at any
The CWF being tested ceramic pot was first placed into a plas- given time; ρ = density of water; and g = acceleration due to
tic receptacle that was fitted with a large plastic funnel. The filter gravity.
and receptacle-funnel were suspended above an empty collection Eq. (2) is substituted into Eq. (1). Additionally, the area of the
bucket that rested on a load cell (Model LSC 7000-50, Omega bottom of the filter (A ¼ πr2o , where ro is the radius of the base of
Fig. 2. Pore size distribution for samples taken from the bases of (a) PFP filter; (b) 50∶50 filter; (c) 65∶35 filter; (d) 75∶25 filter
incubated overnight at 37°C. To decontaminate CWFs between polystyrene beads (Bales et al. 1997; Bielefeldt et al. 2010; Dai and
experiments, the CWFs were rinsed thoroughly with purified Hozalski 2003; Hendricks et al. 2005). It has been shown that the
water and dried in full sunlight for 5–8 hrs to mimic conditions removal of microspherical beads from water by CWF decreases
in the field. The efficiency of E. coli filtration is expressed both with decreasing bead size (Bielefeldt et al. 2010). This means that
as a (Mwabi et al. 2012) and a log reduction value (Brown and to effectively filter out viruses from water the CWFs cannot rely on
Sobsey 2009). size occlusion alone. One solution that is currently been explored is
to doping the CWFs with materials that have affinity for viruses
(Brown and Sobsey 2009; Tsao 2011).
Results and Discussion The porosities determined from the MIP analyses showed that
the porosity of the base of the CWF (Fig. 1) increased with increas-
Porosity and Pore Size Distribution ing volume fraction of sawdust (Fig. 3). Similarly, the porosity
of each of the three samples extracted from the top, middle, and
The pore size distribution results obtained for CWFs with clay to
bottom of the sides of the CWFs (Fig. 1) also increased with the
sawdust ratios of 50∶50, 65∶35, and 75∶25 are compared with those
volume fraction of sawdust. Consequently, the average porosity ob-
from the base of a PFP reference filter (60∶40) in Figs. 2(a–d). All
tained from all four samples (from each specific CWF) increased
CWFs tested had a range of pore sizes between the nano- and
with increasing volume fraction of sawdust (in Fig. 3).
micron-scales. The fact that each CWF has both nano- and
micron-scale porosities is important because the micron-scale pores
can trap larger microbes and multicellular organisms, while the
nanoscale pores could potentially trap viruses. A unimodal distri-
bution of pore sizes was observed in the PFP reference filter and
the 50∶50 CWF [Figs. 2(a and b)]. In contrast, the 65∶35 and 75∶25
CWFs had bimodal micro- and nanoscale pore size distributions
[Figs. 2(c and d)].
In all cases, most of the pores in the three different CWFs were
between 0.05 and 1 μm in size. This is smaller than the typical
sizes of most bacteria and nonviral pathogens, which are usually
∼1–3 μm in size (Weart et al. 2007; Willey et al. 2008). All three
CWFs should, therefore, be effective in removing bacteria, as well
as larger cells such as helminth ova, which are typically between
10 μm and a few hundred microns in size (Crompton and Joyner
1980). The presence of a significant fraction of nanoscale pores is
also of some importance, since it raises the possibility of using
Fig. 3. Dependence of porosity on the volume fraction of sawdust used
CWFs in the nanoscale filtration of viruses, which are typically be-
in filter fabrication; solid line represents the CWF base porosity levels,
tween 10–100 nm in size (Willey et al. 2008). One way of confirm-
and the dash line is the overall average porosity with sample taken from
ing that the filter is capable of removing viruses by particle size
CWF sides and base
occlusion is the use of a surrogate in the form of fluorescent labeled
in determining the rate of fluid flow through the filter. The most
porous of the filters studied, the 50∶50 CWF, exhibited the fastest
discharge, followed by the PFP reference filter. The slowest dis-
charge rates, for both the short- and long-term, were associated with
the 75∶25 CWF. Therefore, the rate of water discharge by CWF
increases with porosity, or in other words with the volume fraction
of sawdust used in making the filter. The flow rates obtained for the
50∶50 CWF were between ∼1.3 and 2 L=hr during the first two
hours, which is the range that is typical of PFP filters. Flow rates
for the 65∶35 and 75∶25 CWFs were well below this level (Fig. 4). Fig. 5. Plots of volume flow rate against time—comparisons of experi-
It is important to note that the amount of water through the 50∶50 mental data and Darcy fits: (a) 50∶50: CWF; (b) 65∶35 CWF; (c) 75∶25
CWF approached an asymptote, as the pressure head decreased CWF (note: 1 m3 =s ¼ 3.6 × 106 L=h)
with increasing flow. Hence, the flow-time plots became increas-
ingly nonlinear with increasing flow, as shown in Fig. 4. This
asymptotic behavior was recently mathematically simulated with
a stochastic birth process model specific to respective amounts For a particular filter composition the variability in the value of
of organic raw material used in the manufacturing of these filters permeability obtained using the K-T approach is largely due to
(Plappally et al. 2009). However, asymptotic regimes were not ob- the variation of the porosity of the filter with respect to the location
served for the 65∶35 and 75∶25 CWFs (Fig. 4), since the amount of from which the sample was taken for the mercury porosimetry test,
flow was low, even after 24 hours. In these cases, the pressure head and also in part due to Lc , Lmax and SðLmax Þ [see Eq. (1)]. The
is insufficient to drive a significant amount of flow through the variability in the permeability obtained from the Darcy fit may be
porous CWFs, as the water level reduced. Figs. 5(a–c)shows how attributed to pores opening and clogging during multiple flow ex-
the measured volume flow rate of the different filters changes with periments and possibly the effect of the degree of saturation of
time. Darcy fits are also presented to show how well the measured the CWF prior to testing. The permeabilities of the filters studied
flow rate data fit the theory. The effective intrinsic permeabilities (obtained by both methods) were found to be between ∼10−15 m2
obtained for each of the CWFs from the Darcy fit (described in to ∼5.0 × 10−14 m2 (i.e., ∼1 millidarcy to ∼50 millidarcy), which
section 2.4) are plotted against the volume fraction of sawdust in means the filters can be classified as semipervious (Bear 1972). The
Fig. 6. This shows that the effective permeabilities of the filters value of the permeability is of the same order as that reported by
increase with increasing volume fraction of sawdust. van Halem (2006). The difference may be due to the choice of in-
Fig. 7(a) shows the comparison between the permeability ob- flexion point (Webb 2001) and the effects of production variables
tained from the Darcy fit to that obtained using the K-T method. during fabrication of the CWFs (Lantagne et al. 2010).
Fig. 4. Plots of effluent discharge as a function of time for one Fig. 6. Dependence of the effective CWF intrinsic permeability on the
day-long (24 hour) effluent discharge volume percentage of sawdust
Bacterial Filtration
Following the flow rate tests, E. coli filtration experiments were
performed on the two CWFs with the fastest flow rates, the 50∶50
CWF and the 65∶35 CWF. Each of these two CWFs were tested
twice using a 4 L prefiltrate with a high E. coli density as described
in section 2.7. Both CWFs tested were highly efficient at removing
E. coli from 4 L aqueous suspensions (Table 1), having high aver-
age filtration percentages (99.9996 and 99.9999%) and also high
average LRVs of 5.67 and 6.36, respectively. Thus, the removal
efficiency of the 65∶35 CWF was slightly greater than that of
the 50∶50 CWF. Both CWFs meet the WHO standard for water
treatment (WHO 2011b) that no E. coli nor coliform bacteria
should be detectable in 100 mL of drinking water. In comparison,
the filtration efficiency of the PFP filter has been reported to
be approximately 99.99% with LRV of ∼2–6 (Lantagne 2002;
Oyanedel-Craver and Smith 2008; Plappally et al. 2009; Sobsey
et al. 2008).
Fig. 7. Bar chart: (a) comparing the permeability obtained from Darcy Following the first set of filtration experiments, a second set of
fit with the K-T method; (b) showing the tortuosity of the CWFs; the experiments was performed on the same CWFs to explore possible
tortuosity was found by combining the Jörgen Hager approach with performance differences as a function of increased CWF use. Only
(1) the permeability obtained from the Darcy fit; (2) the permeability small differences in filtration efficiencies were observed between
obtained using the K-T method; the skeletal density used was obtained the first and the second sets of tests. These results suggest that
using helium pycnometer CWF pores did not become significantly clogged or plugged during
the first test because of the high E. coli density in the prefiltrate
suspensions. Further work is clearly needed to study the depend-
ence of flow and filtration characteristics of the CWFs on the
While the level of permeability of a porous ceramics gives a number of filtration cycles. In addition to tests using a prefiltrate
measure of the relative ease at which water (or any other fluid) will volume of 4 L, a prefiltrate volume of 8 L was also used to deter-
flow through it, the tortuosity gives an indication of the chances of mine whether the efficiency of filtration would be affected by the
capture of contaminants, such as E. coli bacteria that are carried volume of the prefiltrate. Base on a study of two different 50∶50
along with the water by processes such as adsorption, geometrical CWFs, the average LRV did not change significantly using
occlusion and sedimentation. The results for the tortuosity of the an 8 L prefiltrate compared to a 4 L prefiltrate (LRV4 L ¼
CWFs found by using the Jörgen Hager equation (combined with 5.67 2.50 and LRV8 L ¼ 4.61 0.53).
Table 1. E. coli Filtration Efficiency Obtained for Filters with Different Clay to Sawdust Volume Ratios Using 4 L and 8 L Prefiltrates
Volume fraction Percentage E. coli Average LRV E. coli Average Experiment
(clay : sawdust) Prefiltrate volume removal percent ± range removal LRV ± range number
50∶50 4 L 99.99 8.17 1
50∶50 4 L 99.99 99.99 0.00 3.16 5.67 2.50 2
65∶35 4 L 99.99 5.82 1
65∶35 4 L 99.99 99.99 0.00 6.9 6.36 0.54 2
Note: Results are expressed as percentages (Mwabi et al. 2012) and also as the Log10 reduction value (Brown and Sobsey 2009).
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