ASSESSING THE CLEANLINESS OF FINE AGGREGATES USING THE

METHYLENE BLUE TEST

Y. Chen1, N. Tregger2, A. Jeknavorian3, E. Koehler4
1
W. R. Grace, 62 Whittemore Avenue, Cambridge, MA 02140, USA; PH (617) 498-
4316; email: ying.chen@grace.com
2
W. R. Grace, 62 Whittemore Avenue, Cambridge, MA 02140, USA; PH (617) 498-
4396; email: nathan.tregger@grace.com
3
W. R. Grace, 62 Whittemore Avenue, Cambridge, MA 02140, USA; PH (617) 498-
4843; email: ara.a.jeknavorian@grace.com
4
Verifi LLC, 62 Whittemore Avenue, Cambridge, MA 02140, USA; PH (513) 874-3222;
email: eric.koehler@verifitechnologies.com

Abstract
Historically, the use of microfines (passing the No. 200 mesh (75 microns)) in concrete
has been associated with high water demand, high shrinkage, and subsequent low
strength. As a result, in specifying aggregate gradation limits, ASTM C33 allows a
maximum of up to 7% microfines content (or 5% when used in abrasive environments).
This limit on microfines has received greater attention with the increased use of
manufactured sands in recent years. Such studies have shown that inclusion of acceptable
microfines can actually improve workability, shrinkage resistance, abrasion resistance
and strength. Stewart and others, for example, show that up to 15% microfines can be
used without a detrimental effect on the concrete performance.
Manufactured aggregates differ from natural sands in that they attain proper gradation
through several crushing processes. These processes typically result in high percentages
of microfines, up to 20% of aggregate produced. Depending on the aggregate plant, these
fines are usually separated and discarded as waste. The increased use of these microfines
has a vast impact on the sustainability of both the concrete and aggregate industries.
The improvement associated with non-clay bearing fines is a direct result of particle
packing. Smaller fines can fit in the voids of larger fines, which in turn provides two
main benefits. First, more contact points are created between particles, improving
compressive strength (distribution of load), and second, filling voids allows more water
to lubricate interfaces, increasing workability. It should be noted, however, that
increasing fines does not necessarily lead to these benefits; if the fines do not fill voids
and increase the overall particle packing, the benefits may not be realized. Therefore,
overall gradation and size distribution must be considered.
A challenge in using microfines includes the ability to distinguish deleterious fines from
beneficial fines. Fines can impact concrete through their shape, gradation and cleanliness.
Currently, the sand equivalency test aims to estimate the impact of cleanliness. This

2012 International Concrete Sustainability Conference  1  ©National Ready Mixed Concrete Association 
paper will compare this test with the methylene blue test with regards to determining the
effect of deleterious material on the performance of concrete. It is shown that the
methylene blue test is more effective in identifying deleterious fines within an aggregate
source. A new, more accurate and user friendly methylene blue test will also be
introduced.

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Introduction
Historically, the use of microfines (passing the No. 200 mesh (75 microns)) in concrete
has been associated with high water demand, high shrinkage, and subsequent low
strength. As a result, in specifying aggregate gradation limits, ASTM C33 allows a
maximum of up to 7% microfines content (or 5% when used in abrasive environments)
(ASTM 2011). However, potential issues with fine aggregates are not limited to gradation
alone. Shape and cleanliness (or clay content) are also major factors. Manufactured
aggregates are especially prone to shape issues and depending on the quarry, clay issues
as well. The gradation limit, has received greater attention with the increased use of
manufactured sands in recent years.
Research topics on microfines range from effects on water-reducing admixtures (Abou-
Zeid); interfaces between coarse aggregate and cementitious binder (Muñoz 2010a,
2010b); as well as test methods that predict performance based on aggregate
characteristics (Quiroga). A comprehensive study was performed by ICAR at the
University of Texas at Austin (Ahn). Such studies have shown that inclusion of
acceptable microfines can actually improve workability, shrinkage resistance, abrasion
resistance and strength if the concrete and gradation are designed properly. Nevertheless,
microfines which are comprised of clay can still lead to significant water and water
reducer demand. Current aggregate characterization tests such as gradation cannot
reliably predict concrete performance, especially in manufactured aggregates.
Manufactured aggregates differ from natural sands in that they attain proper gradation
through several crushing processes. These processes typically result in high percentages
of microfines, up to 20% of aggregate produced (Hudson). Depending on the aggregate
plant, these fines are usually separated and discarded as waste. One study estimates the
amount of waste fines that accumulate annually is over 100 million tons in the United
States (Quire) alone. The increased use of these microfines has a vast impact on the
sustainability of both the concrete and aggregate industries.
A challenge in using microfines includes the ability to distinguish deleterious fines from
beneficial fines. Fines can impact concrete through their shape, gradation and cleanliness.
Currently, the sand equivalency test (ASTM 2009) aims to estimate the impact of
cleanliness. This paper will compare this test with an improved methylene blue test with
regards to determining the effect of deleterious material on the performance of concrete.
It is shown that the improved methylene blue test is more effective in identifying
deleterious fines within an aggregate source than the current sand equivalency test.

Background
Prior to the study, several concrete aggregate samples were obtained from different
regions of North America. Samples included manufactured, natural and blends. In
addition to typical aggregate properties, the sand equivalency (SE) and methylene blue
absorption were measured. In Figure 1, a comparison between SE and methylene blue
absorption as measured by an MBV is presented.

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 MBV versus SE for natural and manufactured aggregates
100
Blended
95 Manufactured
Natural
90

Methylene blue value [mg/g]

85

80

75

70

65

60

55
0 0.5 1 1.5 2 2.5 3
Sand equivalent [%]

Figure 1. Comparison between SE and MBV for different sands in North America.
It is immediately clear that there is no strong trend between the two values, even though
both aim to quantify deleterious content within an aggregate source.

Experimental program
In this study, methods to predict cleanliness is examined by comparing two different
model sands. They have been proportioned to give similar sand equivalent values, but
differing methylene blue values. The concrete performance is then evaluated and
compared to the cleanliness as predicted by the two fine aggregate characterization
methods.
Materials and proportioning. A base river sand (SAND A) was doped with two
different types fines in order to produced two different model sands. The first sand,
SAND B was produced by doping 2% of a fine ground silica, 99.9% passing the 325
mesh, with a specific gravity of 2.7. The silica sand is composed of 99.3% silicon dioxide
and trace amounts of other minerals (US Silica). The second sand, SAND C was
produced by doping 1% of a sodium montmorillonite clay, 99.0% passing the 325 mesh,
with a specific gravity of 2.6. The clay is composed of 75.4% silicon oxide, 15.3%
aluminum oxide and trace amounts of other minerals (American Colloid Company). Two
additional sands, SAND D and E were also produced with 1% fine ground silica and
0.2% sodium montmorillonite respectively. The gradation for each sand is given in Table
1 along with the fineness modulus (FM) and the ASTM C33 specifications [ASTM
2011].

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 Table 1. Sand gradations.

Sieve Sieve SAND A SAND SAND SAND SAND ASTM ASTM

# size % B% C% D% E% C33 low C33
[mm] passing passing passing passing passing % high %
passing passing
#4 4.75 100.0 100.0 100.0 100.0 100.0 95 100
#8 2.36 88.0 88.1 88.2 88.1 88.0 80 100
#16 1.18 58.9 59.3 59.7 59.3 59.0 50 85
#30 0.60 32.7 33.4 34.1 33.4 32.9 25 60
#50 0.30 12.5 13.4 14.2 13.4 12.7 5 30
#100 0.15 4.5 5.5 6.4 5.5 4.7 0 10
#200 0.075 3.4 4.4 5.3 4.4 3.6
Pan 0.0 0.0 0.0 0.0 0.0
FM 3.03 3.00 2.97 3.00 3.03

In each sand, the gradation meets specification of ASTM C33. In addition, the gradations
are relatively similar. The sand equivalent (SE) and methylene blue (MB) tests were
conducted on each model sand as is. Normal range concrete was then produced with each
sand type. An ASTM Type I-II ordinary Portland cement (OPC) with an alkali equivalent
of 0.56% and a free calcium oxide content of 0.84% was used with a polycarboxylate-
based high range water reducer (HRWR). The water-to-cement ratio (w/c) was varied to
achieve desired slumps. The mix design is given in Table 2. All mixes were defoamed
using an air defoamer to take out any effects of air content on workability or strength.
Table 2. Basic concrete mix design.

Material Value Unit

OPC 335 kg/m3
Fine aggregate 823 kg/m3
Coarse aggregate 1068 kg/m3
HRWR 0.12 % solids/cement

Test methods
Fine aggregate cleanliness characterization. Two methods were used to determine
cleanliness of the fine aggregate: the sand equivalent (SE) test and a methylene blue
(MB) test developed in-house. The SE test was carried out according to ASTM D2419
(ASTM 2009). Briefly, fine aggregate is shaken in a clear graduated cylinder containing a
solution of flocculant and preservative. After shaking, the particles are allowed to settle
for twenty minutes. The SE value is taken as the ratio of the height of the sand column to
the height of the sand and flocculated clay multiplied by one hundred. Higher percentages
indicate lower amounts of clay.
This test is used heavily in the United States to qualify aggregates for use in concrete and
asphalt applications. Still, in the experience of the authors, the test results are

2012 International Concrete Sustainability Conference  5  ©National Ready Mixed Concrete Association 
occasionally misleading where even though an unfavorable SE value (i.e. low indicating
poor quality aggregate) was obtained, the performance in concrete was sufficient. The
sand equivalent test relies on apparent density differences between “good” sand fines and
“bad” clay fines. Even though a flocculant is used to further encourage separation of clay
particles, similar sized sand particles can also be flocculated. As a result, even though
there is a significant difference in the impact on concrete properties between these fine
aggregates, the settling behaviors and subsequently the difference in SE may not be
sufficiently differentiated in this test.
There exist several variations of the MB in the literature (see for example AASHTO),
which involve an initial concentration of methylene blue and the determination of how
much is absorbed by a sand sample through a titration method. Most methods measure
the end point of the titration by visual detection of a blue halo on filter paper after a
titration process. Drawbacks of this test are that the halo can be subject to operator error,
the titration process can become laborious and only the minus 75 micron fraction is used
to determine the clay content. Clay content is measured in mg/g of sand sample.
An in-house improvement over current MB tests was developed which relies on a
colorimeter; a device that can measure the absorbance of a given solution at a specific
light wavelength (see for example Potgieter). The colorimeter provides portability and
ease for use in the field. Instead of a titration process, the MB content is correlated to the
light absorbed at a specific wavelength, thereby removing the visual interpretation of the
blue halo. An additional benefit is that the entire sand sample can be used; screening is
not necessary to separate the minus 75 micron fraction. The entire process takes
approximately 10 minutes, thus providing a quick and reliable MB value (MBV) that can
be measured easily in the field as well as in the laboratory. An illustration of the test is
shown in Figure 1.

Figure 1. Improved methylene blue method.

First, a sample of fine aggregate is weighed and a known volume of methylene blue is
added. The slurry is mixed thoroughly and the solution is filtered to remove any particles.
The change in concentration of methylene blue is then determined with the colorimeter.
In comparisons to standard MB tests, such as AASHTO TP 57, the improved MB test
provides an excellent correlation as shown in Figure 2. In this figure, the effect of adding
different amounts of sodium montmorillonite (Na-mont) to a clean silica sand with a
particle size passing the No. 100 (1.18mm) sieve is shown.

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 Silica sand passing No. 100 with 0, 1, 2, 4% doped Na-mont.
4.5
y = 1.0217x
4
R2 = 0.9997

AASHTO TP 57 [% Na-mont. eq]

3.5

2.5

1.5

0.5

0
0 0.5 1 1.5 2 2.5 3 3.5 4 4.5
Improved MB test [% Na-mont. eq]

Figure 2. Comparison between a modified AASHTO TP 57 and improved MB

method.
It should be pointed out that the comparison here is made with model clays. Real
aggregate systems may deviate slightly from the curve.
Concrete performance evaluation. Normal concrete was produced with each sand using
the mix design given above. Initially, all three sands were tested at a water-to-cement
ratio (w/c) of 0.53. Afterwards, the w/c was altered if necessary to adjust the slump of
each mix to a value of 170 mm +/- 10 mm. In addition to the slump, the air and
compressive strength at 4, 7 and 28 days were measured.

Test results and discussion

Sand cleanliness. The results from the sand equivalent and methylene blue tests are
given in Table 3.
Table 3. Sand cleanliness results.

Sand sample SE [%] MBV [mg/g]

SAND A 91 0.08
SAND B 72 0.29
SAND C 72 2.18
SAND D 83 0.21
SAND E 83 0.72

Although SAND B, with 2% fine ground silica has the same SE as SAND C, with 1%
sodium montmorillonite, the MB values are different by an order of magnitude.
Similarly, SAND D and E have the same SE but different MB values. These are clear

2012 International Concrete Sustainability Conference  7  ©National Ready Mixed Concrete Association 
examples where the SE suggests that there is clay present, even though there is no
significant amounts according the MB test. As shown previously, the correlation between
the SE and MB values is not strong. More importantly, however, is the correlation
between fines content and concrete performance.
Concrete performance. Concrete results including slump, air and compressive strength
are given in Table 4.
Table 4. Concrete performance results.

4 day 7 day 28 day

Slump
Sand sample w/c Air [%] strength strength strength
[mm]
[MPa] [MPa] [MPa]
SAND A 0.53 165 2.0 22 25 35
SAND B 0.53 165 2.1 22 25 36
SAND C 0.53 13 1.2 20 20 32
SAND D 0.53 191 2.0 22 26 37
SAND E 0.53 76 2.5 21 25 35
SAND C 0.80 171 2.0 10 13 19

At equal w/c, the silica sand mix (SAND B), even with a relatively low SE (but
acceptable MBV), performs similar to the control (SAND A) in both slump and strength.
The difference in SE between SAND A (91%) and SAND B (72%) does not translate to a
large difference in slump or strength. On the other hand, SAND C, with the same SE but
higher MBV than SAND A (2.18 versus 0.08) has a much lower slump. A similar trend is
seen comparing SAND D and E to the control mix, SAND A. The MB test is able to
predict a harmful effect of the clay on the concrete performance. In this set of
experiments, the MB test predicts the negative effect on slump, where the SE does not.
It should also be noted that although the fines content (minus 75 microns) are similar,
SAND B is above the 5% limit and SAND C is below the 5% limit. Yet, SAND B seems
to have the same performance as the control, while SAND C has a large negative effect
on the concrete performance.
Furthermore, if water is adjusted to achieve the same workability as SAND A, then the
strength of SAND C suffers dramatically compared to SAND A. The presence of clay
increases water demand through absorption onto the clay (and within any interlayer
structure), while the silica sand is not nearly as absorbent. There are several articles
suggesting that if fines are used correctly (in terms of type and content), key properties
such as workability and strength can be improved through particle packing. The MB test
is a helpful predictive tool to determine types of fines that may improve or damage a
particular concrete mix.

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Conclusions
Through a simple set of experiments, the SE test was shown to be ineffective in
predicting effects of clay on concrete performance. The MB, however, demonstrates that
clay content measured does relate to concrete performance in terms of slump. Use of the
MB test would give higher confidence in selecting fines that can be used at higher
percentages for both manufactured and natural sands.

Acknowledgements
The authors would like to acknowledge Huy Bui in preparing the aggregate and concrete
results.

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Quire, D., Kowalski, T, and Hudson, B. (2003) “Discovering the Lost Aggregate
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