Accepted Manuscript

Recycling of marble dust as paste replacement forimproving strength,

microstructure and eco-friendliness of mortar

L.G. Li, Z.H. Huang, Y.P. Tan, A.K.H. Kwan, H.Y. Chen

PII: S0959-6526(18)33365-1

DOI: 10.1016/j.jclepro.2018.10.332

Reference: JCLP 14734

To appear in: Journal of Cleaner Production

Received Date: 03 January 2018

Accepted Date: 30 October 2018

Please cite this article as: L.G. Li, Z.H. Huang, Y.P. Tan, A.K.H. Kwan, H.Y. Chen, Recycling of
marble dust as paste replacement forimproving strength, microstructure and eco-friendliness of
mortar, Journal of Cleaner Production (2018), doi: 10.1016/j.jclepro.2018.10.332

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Graphical abstract:

Water

Marble dust 80
Cement

28-day cube strength (MPa) .

MD added as
70 paste replacement
Aggregate

Cement replacement method 60

Water MD added as
50
cement replacement
Marble dust Paste
Cement
40
450 550 650 750 850 950
3
Cement content (kg/m )
Aggregate

Paste replacement method

 ACCEPTED MANUSCRIPT

28/7/2018

Recycling of marble dust as paste replacement for

improving strength, microstructure and eco-friendliness of mortar

L. G. Li1*, Z. H. Huang1, Y. P. Tan1, A. K. H. Kwan2 and H. Y. Chen1

1 Guangdong University of Technology, Guangzhou, China.
2 The University of Hong Kong, Hong Kong, China.

Abstract: Marble waste is generated in a fairly large quantity in the world and has
been causing serious environmental problems. Usually, the marble waste is reutilized
as cement replacement or aggregate replacement in concrete production. But these
two methods of utilization have some drawbacks. In this study, an alternative method,
called the paste replacement method, in which marble dust (MD) is added to replace
an equal volume of paste without changing the mix proportions of the paste, was
proposed, and a number of mortar mixes with different amounts of MD added as
either paste replacement or cement replacement were produced for testing of
workability, compressive strength and microstructure. It was found that the addition
of MD as paste replacement would improve the strength and microstructure of the
concrete produced. More importantly, the paste replacement method is better than the
cement replacement method in cement content reduction and waste utilization,
leading to greater reductions in the carbon footprint (which is mainly from the cement
content) and the amount of waste to be disposed.

Keywords: carbon footprint; filler technology; green mortar/concrete; marble waste;

microstructure of material; waste recycling.

_________________________________________________________________________________
* Corresponding Author. Tel: +86 020 39322527, E-mail: ligu@gdut.edu.cn (L. G. Li)

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1. Introduction

In the reuse of a solid waste for mortar/concrete production, depending on

whether the waste would react chemically to produce gel, the waste may be classified
into cementitious waste and inert waste. Fly ash, blast-furnace slag and silica fume are
the most common cementitious wastes and have now become precious supplementary
cementitious materials in mortar/concrete production (Farahani et al., 2015; Özbay et
al., 2016; Wu and Ye, 2017). Other wastes, such as rock dust, old concrete, waste
glass, seashell waste and certain mine tailings, are not inherently cementitious and are
therefore inert wastes (Sprung and Siebel, 1991; Poppe and De Schutter, 2005).
Nevertheless, it has been found that the incorporation of these inert wastes can
enhance the performance of mortar/concrete in certain ways (Singh et al., 2016;
Alyamac et al., 2017; Chen and Poon, 2017; Tam et al., 2007).

Marble is a metamorphic rock containing a large amount of calcium carbonate

and small amounts of silica, feldspar, iron oxide, mica and fluorine (Topcu et al.,
2009). Since ancient times, marble has been commonly used as a building material for
cladding and flooring. Nowadays, over 50% of the marble in the world is quarried
from four countries, namely, Italy, China, India and Spain, with individual annual
productions in the year 2014 of approximately 3.5, 2.8, 1.7 and 1.0 million tons,
respectively (Ministry of Industry, Energy and Mines, Republic of Tunisia, 2014;
Rana et al., 2015). China is the second largest producer of marble in the world and the
production of marble plank was 350 million m2 in 2015 (China Stone Material
Association, 2016). However, the amount of marble waste generated during the
extraction process can be as much as 80% of the total volume of stone extracted
(Hebhoub et al., 2011). As a non-biodegradable waste material, such a large quantity
of marble waste would permanently occupy a large area of land for disposal and
seriously damage the morphology, ecology, hydrology and fertility of soil, and the
air-suspended portion can even cause respiratory, visual and skin disorders (Rana et
al., 2015). Usually, the marble waste is reutilized as cement replacement or aggregate
replacement in mortar/concrete production. These two methods of using marble waste
are herein called the cement replacement method and the aggregate replacement
method, respectively.

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By the cement replacement method, the marble waste is added to replace a

portion of cementitious materials, as illustrated in Figure 1(a). For instance, Topcu et
al. (2009) used marble dust (MD) as binder (cement + fly ash) replacement to produce
self-compacting concrete (SCC) and found that the workability of SCC has not been
affected up to a MD content of 200 kg/m3. Corinaldesi et al. (2010) added MD to
replace part of cement and found that due to its high fineness, the MD powder can
improve the cohesiveness of fresh mortar and concrete. Soliman (2013) pointed out
that cement replacement by MD up to 5% can enhance the compressive strength,
tensile strength and Young’s modulus of concrete. Bacarji et al. (2013) investigated
the rheological and mechanical properties of concrete containing marble and granite
residues as cement replacement, and carried out analysis to quantify the influence of
cement replacement. Talah et al. (2015) added MD as partial substitute of cement up
to 15% to produce high-performance concrete (HPC) and revealed that the addition of
such amount of MD can improve the chloride and oxygen resistances of HPC. Rana et
al. (2015) found that 10% of the cement in concrete can be substituted by marble
slurry with the strength maintained and durability enhanced.

By the aggregate replacement method, the marble waste is applied to replace a

portion of fine and/or coarse aggregate, as illustrated in Figure 1(b). For instance,
Corinaldesi et al. (2010) showed that 10% substitution of fine aggregate in mortar by
MD yielded maximum compressive strength if a superplastisizer was added to
maintain the same workability level. Gencel et al. (2012) used marble waste to
replace both fine aggregate and coarse aggregate up to 40% by mass, and pointed out
that marble waste is a good aggregate substitution for producing concrete paving
blocks. André et al. (2014) added marble industry waste as coarse aggregate
replacement to produce concrete and demonstrated that it is feasible to use this solid
waste as coarse aggregate. Gameiro et al. (2014) revealed that the addition of marble
sand as aggregate could reduce the water permeability of concrete. Sadek et al. (2016)
have recently used MD to replace fine and coarse aggregates in SCC, and found that
the optimum MD content was 200 kg/m3.

However, both these two methods of adding marble waste have certain
drawbacks. For the cement replacement method, a high cement substitution rate

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would generally cause substantially reduction of strength, thus rendering the actual
effectiveness in cement content and carbon footprint reductions rather limited (Topcu
et al., 2009; Bacarji et al., 2013; Rana et al., 2015). For the aggregate replacement
method, although the use of marble waste as aggregate has beneficial effect on waste
recycling and environmental protection, the cement content and carbon footprint
would not be reduced. Hence, the current situation is not entirely satisfactory. Ideally,
a better method that replaces a larger amount of cement without any adverse effect on
strength, reuses a larger amount of MD for waste minimization, and at the same time
improves the performance of concrete should be developed.

Recently, an alternative method, called the paste replacement method, was

proposed by the authors’ research group. By this method, the inert fillers or waste
materials are used as paste replacement (replacement of an equal volume of paste
without changing the mix proportions of the paste so that the water/cementitious
materials ratio of the paste would remain unchanged), as illustrated in Figure 1(c). In
previous studies, the authors’ research group had proved that adding limestone fines
by this method would allow substantial reductions of cement content and carbon
footprint, and at the same time, also increase the strength, durability and dimensional
stability of concrete (Chen and Kwan, 2012; Kwan et al., 2013; Li and Kwan, 2015;
Li et al., 2017). Since the filler does not need to be cementitious, in theory, this
method should be applicable also to other inert fillers or waste materials (Li et al.,
2018a; Li et al., 2018b). However, the different fillers and waste materials may have
different particle size distributions, particle shape and mechanical properties, and
therefore the actual effectiveness of their additions as paste replacement to reduce the
cement content and improve the performance of concrete still needs to be separately
evaluated.

In the study presented herein, the paste replacement method and cement
replacement method of utilizing MD in concrete production were compared by
producing a number of trial mortar mixes with different amounts of MD added either
as paste replacement or as cement replacement for testing of their workability, cube
strength and microstructure. In the comparison, the relative effectiveness of the two

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different replacement methods in cement content reduction, waste utilization, strength

improvement and microstructure densification were evaluated.

2. Material and test methods

2.1 Raw materials

The cement used was an ordinary Portland cement of strength class 42.5
complying with the Chinese Standard GB175-2007 (Chinese Standard, 2007), the fine
aggregate used was a river sand with maximum size of 1.18 mm, moisture content of
0.16% and water absorption of 1.10%, and the superplasticizer (SP) added was a
polycarboxylate-based SP with a solid mass content of 20%. The relative densities of
cement, river sand and SP were measured as 3.08, 2.58 and 1.03, respectively.

The marble dust (MD) was provided by a stonework factory in Yunfu city, a
famous hometown of stoneware products in China. It was generated as a waste during
cutting, shaping and polishing of marble, and collected by a settling basin, as shown
in Figure 2. In recent years, due to tight control on waste disposal, stonework factories
have to pay large sums of money to dump the MD to landfills. Moreover, it is causing
the sustainability problem of rapidly consuming the limited capacities of landfills
because it is not easy to find new sites for landfills. A more fundamental approach
should be to reutilize the MD as a raw material in manufacturing or construction.

The MD was wet and contained some gravel and debris, as shown in Figure
3(a). To dry and reduce the variation in quality of the MD, simple treatment was
carried out as follows: first, the MD was heated in an oven at 105 ºC for 8 hours to
remove the water; then, a 0.15 mm sieve was used to mechanically sieve away the
particles larger than 0.15 mm. After such treatment, the MD became a white dry
powder, as shown in Figure 3(b). The sieving removed about 5% of the mass of the
MD (in other words, about 5% by mass of the MD supplied was larger than 0.15 mm).
Finally, the MD was measured to have a relative density of 2.70.

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2.2 Mix proportions

First of all, a series of mortar mixes with different amounts of MD added as

paste replacement and various water/cement (W/C) ratios were produced for testing.
For every mortar mix, the paste volume (volume of water and cement, expressed as a
percentage of volume of mortar) plus MD volume (volume of MD, expressed as a
percentage of volume of mortar) was fixed at 60%. The MD volume was set equal to
0%, 5%, 10%, 15% and 20%, and the respective paste volume was set equal to 60%,
55%, 50%, 45% and 40%, i.e. 60% minus the MD volume, such that the sum of the
paste volume and MD volume remained at 60% of the volume of mortar. With the
paste volume plus MD volume fixed, the fine aggregate volume was also fixed at 40%
of the volume of mortar. It should be noted that when the MD was added, the W/C
ratio was not changed, and for each set of mortar mixes with a given MD volume, the
W/C ratio was varied from 0.40 to 0.55 in increments of 0.05.

Then, to compare the effects of adding MD as paste replacement and adding

MD as cement replacement, another eight mortar mixes with different amounts of MD
added as cement replacement and various W/C ratios were also produced for testing.
For these mortar mixes, the paste volume plus MD volume was also fixed at 60%.
When MD was added as cement replacement, the cement volume was reduced by the
same amount such that the sum of the cement volume and the MD volume remained
constant. The MD volume was varied among 0%, 5%, 10%, 15% and 20% of the
initial cement volume (i.e. the cement volume before replacement) and the respective
cement volume was set equal to 100%, 95%, 90%, 85% and 80% of the initial cement
volume. It should be noted that when MD was added, the water volume was not
changed but the W/C ratio would be increased. The initial W/C ratio, i.e. the W/C
ratio before the addition of MD, was set at either 0.40 or 0.55.

Details of the mortar mixes are presented in Table 1. Each mortar mix was
assigned a code of X-Y-Z, in which X denotes the mortar type with names of NM
(normal mortar with no MD added), PR (mortar with MD added as paste replacement)
and CR (mortar with MD added as cement replacement), Y denotes the initial W/C
ratio and Z denotes the MD volume (as a percentage of mortar volume in PR mixes or

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as a percentage of initial cement volume in CR mixes).

Unlike the other mix parameters, the SP dosage (in terms of liquid mass of SP
by mass of cement plus MD) was not pre-determined. Instead, trial mixing was
carried out, in which the SP was added to the mortar in small increments until a flow
spread of 200 to 300 mm was achieved, and then the SP dosage determined by trial
mixing was applied in the formal tests.

2.3 Measuring PSD, SEM image and XRD pattern

A laser diffraction particle size analyzer (Malvern Mastersizer 2000) was used
to measure the particle size distribution (PSD) of the cement and MD, whereas the
mechanical sieving method was used to measure the PSD of the fine aggregate.
Moreover, the scanning electron microscopy (SEM) test via a Hitachi S-3400N-II was
used to study the micro-morphology of the MD particles and the hardened mortar
samples, and the X-ray diffraction (XRD) test via a Rigaku D/MAX-Ultima IV was
used to determine the chemical composition of the MD.

2.4 Measuring flow spread

The workability of each mortar mix was measured in terms of flow spread (the
average diameter of the patty formed after the slump cone was lifted) by a mini slump
cone test developed by Okamura and Ouchi (2003). The mini slump cone used has a
base diameter of 100 mm, a top diameter of 70 mm and a height of 60 mm. In actual
measurement, the diameters in two perpendicular directions were measured and the
average taken as the test result.

2.5 Measuring cube strength

After the mini slump cone test, the mortar was remixed and then cast into
three 100 mm cube moulds. The cubes were covered with plastic sheets and kept in
the laboratory after casting, demoulded at 24 hours and cured in lime-saturated water
at 272 °C until the time of testing. The compressive strength of each mortar cube

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was tested at the age of 28 days by using a Matest electro-hydraulic servo-controlled

compression testing machine. From each mortar mix, three cubes were cast and tested
at the same time. The average compressive strength of the three cubes was taken as
the cube strength of the mortar mix.

3. Test results

3.1 PSD, SEM image and XRD pattern

The PSDs of the cement, MD and fine aggregate are plotted in Figure 4. From
the figure, it can be seen that both the cement and MD have continuous graded PSDs.
The mean particle size of the MD is closed to that of the cement, but the particle size
range of the MD is wider. In other words, there are some MD particles finer than the
cement grains and some MD particles coarser than the cement grains. The reason may
be that marble has a Mohs hardness of only about 3 and therefore is not a hard rock.
So during the polishing process, some of the MD particles are ground to finer size
than cement.

The SEM image and XRD pattern of the MD are presented in Figures 5(a) and
5(b), respectively. From the SEM image, it is observed that the MD particles are
angular in shape due to the cutting, shaping and polishing processes in their
production. From the XRD pattern, it is evident that the MD used is typical marble
composed mainly of CaCO3, CaO and Ca2SiO4.

3.2 Cement content

The cement contents of the PR mortar mixes (with MD added as paste

replacement) and the CR mortar mixes (with MD added as cement replacement) are
tabulated in the third column of Table 1 and plotted against the MD volume for
different W/C ratios in Figures 6(a) and 6(b), respectively. From these results, it is
obvious that the cement contents decreased as the W/C ratio increased.

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To evaluate the effectiveness of adding MD as paste replacement or cement

replacement in reducing the cement content, the percentage reductions in cement
content due to the addition of MD are tabulated in the last column of Table 1. It is
obvious that in both the PR and CR mortar mixes, the percentage reduction in cement
content was generally larger when the MD volume was larger. For instance, in the PR
mortar mixes, as the MD volume increased from 5% to 20%, the percentage reduction
in cement content increased from 8.4% to 33.3% and in the CR mortar mixes, as the
MD volume increased from 5% to 20%, the percentage reduction in cement content
increased from 5.0% to 20.0%. These percentage reductions in cement content were
independent of the initial W/C ratio.

More importantly, comparing the reduction in cement content when the MD

was added as paste replacement with that when the MD was added as cement
replacement, it is evident that the addition of MD as paste replacement was more
effective in reducing the cement content than the addition of MD as cement
replacement. For example, by adding 20% MD as paste replacement (note that in such
case, the MD content is expressed as a percentage of mortar volume), the cement
content could be reduced by up to 33.3%, but by adding 20% MD as cement
replacement (note that in such case, the MD content is expressed as a percentage of
initial cement volume), the cement content could be reduced by only 20.0%.

3.3 SP dosage and flow spread

The SP dosage needed for each mortar mix to achieve the required workability
of flow spread within 200 to 300 mm is listed in the second column of Table 2 and
plotted against the MD volume for the PR mortar mixes and the CR mortar mixes in
Figures 7(a) and 7(b), respectively. Although the SP was added until the required
workability was achieved, the actual achieved flow spread in the formal tests varied
slightly. For reference, the measured flow spread of each mortar mix is presented in
the third column of Table 2 and plotted against the MD volume for the PR mortar
mixes and the CR mortar mixes in Figures 8(a) and 8(b), respectively. It is noted that
the measured flow spread of the mortar mixes ranged from 202 to 300 mm.

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From these results, it can be seen that for both the PR mortar mixes and the
CR mortar mixes, at a given MD volume, the SP dosage was generally lower at a
higher initial W/C ratio. Such observed phenomenon was expected because as the
W/C ratio increased, the water content also increased and thus less SP was needed to
achieve the required workability.

On the other hand, it can also be seen that at a given initial W/C ratio, the
change of SP dosage was dependent on whether the MD was added as paste
replacement or cement replacement. For instance, at a W/C ratio of 0.55, when the
MD was added as paste replacement, increasing the MD volume from 0% to 20%
substantially increased the SP dosage from 0.10% to 1.50%, whereas when the MD
was added as cement replacement, increasing the MD volume from 0% to 20% just
slightly increased the SP dosage from 0.10% to 0.12%. Hence, the addition of MD as
paste replacement demands a higher SP dosage than the addition of MD as cement
replacement. Such observed phenomenon may be explained by the following reasons.
When the MD was added as paste replacement, the powder content (cement plus MD)
increased and the water content decreased simultaneously as the MD volume
increased. Consequently, the water/powder ratio decreased and more SP dosage was
needed to achieve the required workability as the MD volume increased. On the other
hand, when the MD was added as cement replacement, the powder content remained
more or less the same and the water content was not changed. Therefore, in such case,
the increase of MD volume had less effect on the SP dosage needed.

Furthermore, it should be noted particularly that for the PR mortar mixes,

increasing the MD volume from 0% to 15% just gradually increased the SP dosage,
but increasing the MD volume from 15% to 20% dramatically increased the SP
dosage. The reason may be that when the MD volume was increased to 20%, the
mortar became too difficult to mix and too sticky to flow. So a much larger amount of
SP was needed to achieve the required workability. Therefore, from the perspective of
avoiding a very high SP dosage, the MD volume for paste replacement should
preferably be limited at 15%.

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3.4 Cube strength

The average 28-day cube strength results of the mortar mixes are tabulated in
the fourth column of Table 2 and plotted against the MD volume for the PR mortar
mixes and the CR mortar mixes in Figures 9(a) and 9(b), respectively. Moreover,
error bar for each concrete mix has been added in the figures to show the range of
strength results. From these results, it is obvious that the cube strength decreased as
the W/C ratio increased. This observed variation in cube strength is reasonable
because the strength of mortar or concrete is well known to be governed mainly by
the W/C ratio and is generally lower at a higher W/C ratio.

More importantly, it is noted that the variations of cube strength with MD

volume were not quite the same in the PR mortar mixes and the CR mortar mixes. In
the PR mortar mixes, at a W/C ratio of 0.40, increasing the MD volume from 0% to
20% increased the cube strength from 59.6 to 71.6 MPa by 20.1%, whereas at a W/C
ratio of 0.55, increasing the MD volume from 0% to 20% increased the cube strength
from 39.5 to 53.3 MPa by 34.9%. However, in the CR mortar mixes, at an initial W/C
ratio of 0.40, increasing the MD volume from 0% to 5% increased the cube strength
from 59.6 to 59.9 MPa by only 0.5%, and increasing the MD volume from 0% to 20%
decreased the cube strength from 59.6 to 47.9 MPa by 19.6%, whereas at an initial
W/C ratio of 0.55, increasing the MD volume from 0% to 10% increased the cube
strength from 39.5 to 40.4 MPa by only 2.3%, and increasing the MD volume from
0% to 20% decreased the cube strength from 39.5 to 33.8 MPa by 14.4%.

To more systematically evaluate the effects of MD volume on strength in the

two different cases of adding MD as paste replacement and adding MD as cement
replacement, the percentage changes in 28-day cube strength due to the addition of
MD are tabulated in the last column of Table 2. From these tabulated values, it can be
seen that adding MD as paste replacement without changing the W/C ratio would
always produce a positive change in cube strength (positive change means increase)
and within the range of mix parameters covered in the present study, the cube strength
increases with the MD volume up to a MD volume of at least 20%. Conversely,
adding MD as cement replacement without changing the water volume would only

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produce a slight positive change in cube strength up to a MD volume of 5%, and

could produce a negative change in cube strength (negative change means decrease) if
the MD volume is increased to 10% or higher. Hence, when adding MD as cement
replacement without changing the water content, the MD volume should be limited at
10%. The negative change in cube strength in such case is due to the excessive
increase in effective W/C ratio arising from the constant water volume and decreasing
cement volume when the MD volume keeps on increasing to beyond 10%.

3.5 Microstructure of mortar

The SEM images of three mortar samples, NM-0.40-0 (with no MD added),

PR-0.40-20 (with 20% MD added as paste replacement) and CR-0.40-20 (with 20%
MD added as cement replacement), are presented in Figures 10(a), 10(b) and 10(c),
respectively. These three mortar samples all have the same initial W/C ratio of 0.40
(note that the effective W/C ratio of PR-0.40-20 remained at 0.40, whereas the
effective W/C ratio of CR-0.40-20 was actually higher than 0.40 due to the reduction
in cement volume without changing the water volume).

From Figure 10(a), it is seen that in the mortar sample with no MD added,
some fairly large crystals were formed and the microstructure was rather loose with
many large voids embedded inside.

In contrast, from Figure 10(b), it is obvious that in the mortar sample with MD
added as paste replacement, much fewer large crystals were formed and the texture
was more dense and compact. One possible reason was that with MD added as paste
replacement, the water content was decreased but the powder content was increased
causing the water/powder ratio to decrease and the water films coating the powder
particles to become thinner and easier to be filled up with the gel products generated
by cement hydration.

Lastly, from Figure 10(c), it is observed that in the mortar sample with MD
added as cement replacement, some large crystals were formed and the microstructure
was fairly loose with a lot of small voids embedded inside. The possible reasons were

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that with MD added as cement replacement, the water content and powder content
remained more or less the same but the cement content was reduced leading to a
significant increase in the effective W/C ratio and causing the amount of gel products
generated by cement hydration to become insufficient to fill up the space originally
occupied by the water volume. At the same time, due to the larger size range of MD,
some MD particles finer than the cement grains filled into the voids between cement
grains, making the voids in the mortar with MD added as cement replacement
significantly smaller than those in the mortar with no MD added.

4. Discussions on test results

Overall, the test results revealed that adding MD as paste replacement could
reduce the cement content by up to 33.3% and at the same time increase the strength
by more than 20%. It is only that with MD added as paste replacement, the SP dosage
would significantly increase, especially when the MD volume is higher than 15%. On
the other hand, the traditional way of adding MD as cement replacement could reduce
the cement content by only about 10% if the cube strength is not to be adversely
affected and any further reduction of the cement content by adding more MD as
cement replacement would substantially decrease the strength.

To better depict and compare such simultaneous changes in cement content

and strength in the two different cases of adding MD as paste replacement and adding
MD as cement replacement, the cement content and cube strength of the PR mortar
mixes and CR mortar mixes are plotted in the same graphs for W/C = 0.40 and W/C =
0.55 in Figures 11(a) and 11(b), respectively. It is evident from these graphs that the
paste replacement method is a more effective way of utilizing the MD to reduce the
cement content and improve the strength. Since the reduction in cement content
would lead to a lower carbon footprint, the paste replacement method would also
more effectively improve the eco-friendliness of the mortar produced.

The filler technology of adding MD as paste replacement (as a filler to replace

an equal volume of paste), which increases the strength while reduces the cement

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content, is a promising way of producing green mortar/concrete. This possibility is

still new to some researchers and deserves further in-depth investigation. Whilst the
increase in strength may be attributed partly to the densification of the microstructure,
some further explanations may be given as follows:
(1) Adding MD as paste replacement would not change the W/C ratio whereas
adding MD as cement replacement would increase the effective W/C ratio.
(2) Both the cement grains and the MD particles are much finer than the fine
aggregate particles, and thus would fill into the voids in the fine aggregate to
improve the packing density and refine the pore structure (Powers, 1968;
Zhang et al., 2011; Kwan et al., 2012; Li and Kwan, 2014; Li et al., 2017).
Such filling effect is larger in the case of adding MD as paste replacement than
in the case of adding MD as cement replacement because the combined
cement plus MD volume is larger in the case of paste replacement.
(3) Some of the very fine MD particles could act as nuclei for precipitation of
CSH and thus increase the degree of cement hydration (Soroka and Setter,
1977; Poppe and de Schutter, 2005). This nucleation effect exists in both the
cases of paste replacement and cement replacement. It is only that in the case
of cement replacement, the adverse effect of excessive increase in effective
W/C ratio at large MD volume would counteract the beneficial nucleation
effect, thus causing the strength to decrease.
(4) In the case of paste replacement, the addition of more SP to achieve the
required workability would help to better disperse the cement grains and MD
particles to allow more uniform mixing and better compaction during casting
(Li and Kwan, 2015; Ling and Kwan, 2015; Li et al., 2017). This effect is
insignificant in the case of cement replacement.

5. Discussions on eco-friendliness

The recycling of MD in mortar/concrete production has two major benefits in

eco-friendliness, i.e. environmental sustainability. Firstly, the consumption of MD in
mortar/concrete, which is a widely used construction material, would substantially
decrease the amount of MD to be disposed to landfills. The dumping of MD to

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landfills has been causing rapid depletion of the limited landfill capacity, especially in
densely populated areas where it is difficult to find new sites for landfills. Due to the
rapid depletion of the limited landfill capacity, stonework factories have to pay high
fees for dumping the MD to landfills. Recycling of MD would help to mitigate the
environmental problem of waste disposals.

Secondly, the addition of MD to mortar/concrete would reduce the cement

content needed for production. The cement content is the main contributor to the
carbon footprint of mortar/concrete production (Purnell and Black, 2012; Yang et al.,
2015). More than 90% of the carbon footprint of mortar/concrete is from the cement
content (the manufacture of 1.0 ton of cement generates about 0.9 ton of carbon
dioxide). The reduction in cement content due to the addition of MD would
significantly reduce the carbon footprint and thus improve the environmental
sustainability. Although the heating needed to dry the MD before usage and the
increase in SP dosage would contribute to some carbon footprints, these are relatively
small compared to that of the cement content (the heating of MD up to 105 ºC for
drying consumes much less energy than the heating up to 1500 ºC during manufacture
of cement and the carbon footprint of SP contributes only several percent).

From this research, it was found that with MD added as paste replacement, up
to 20% MD by volume of the mortar (equivalent to 548 kg/m3) may be added to the
mortar to reduce the cement content by 33.3%, as shown in Table 1. However, the SP
dosage would increase quite dramatically when the MD volume is increased to higher
than 15%. In practice, therefore, it may be better to limit the MD volume at 15%
(equivalent to 411 kg/m3), in which case, the cement content would be reduced by
25.1%. On the other hand, with MD added as cement replacement, up to 10% MD by
volume of the original cement content (equivalent to 74 kg/m3 at a W/C ratio of 0.40
and 61 kg/m3 at a W/C ratio of 0.55) may be added to the mortar to reduce the cement
content by 10.0%, as shown in Table 1. Hence, in terms of both waste utilization and
carbon footprint reduction, the paste replacement method is more effective than the
cement replacement method.

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6. Conclusions

To explore a more effective method of reusing marble dust (MD) in mortar

and concrete, the particle size distribution, SEM image and XRD pattern of a typical
MD were analyzed and a series of mortar mixes with varying MD volume added as
paste replacement or cement replacement and different initial W/C ratios were made
for flow spread measurement, 28-day cube strength measurement and microstructure
imaging. Based on the test results, the following conclusions are drawn:
(1) The MD obtained has a continuously graded particle size distribution and an
angular shape, and is composed mainly of CaCO3, CaO and Ca2SiO4.
(2) The addition of MD as paste replacement would densify and improve the
microstructure of the hardened mortar, whereas the addition of MD as
cement replacement could cause deterioration of the microstructure.
(3) The addition of MD as paste replacement and the addition of MD as cement
replacement would both significantly reduce the cement content of mortar.
(4) In the case of paste replacement, the addition of MD up to 20% by volume of
mortar would reduce the cement content by 33% and increase the strength by
more than 20%. However, the SP demand would significantly increase,
especially at MD volume higher than 15%. If the MD volume is limited at
15% to avoid large increase in SP dosage, then there would be 25% reduction
in cement content and around 15% increase in strength.
(5) In the case of cement replacement, the addition of MD to reduce the cement
content by up to 5% has little effect on the strength, but further addition of
MD to reduce the cement content by more than 10% would decrease the
strength. Nevertheless, there is little effect on the SP demand. If the MD
volume is limited at 10% to avoid decrease in cube strength, there would
only be 10% reduction in cement content.
(6) The paste replacement method is a more promising way of producing a
higher performance and more eco-friendly mortar or concrete due to the
following advantages: greater reutilization of waste; lower cement content
and carbon footprint; and improved strength and microstructure.

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Acknowledgements

The authors gratefully acknowledge the financial support provided by

National Natural Science Foundation of China (Project No. 51608131), Natural
Science Foundation of Guangdong Province (Project No. 2015A030310282),
Guangdong Province Project on Application-Oriented R&D and Transformation of
Major Scientific and Technological Achievements (Project No. 2017B020238006),
Science and Technology Planning Project of Guangzhou City (Project No.
201607010329 and 201704030057), and Guangdong University of Technology via its
“One-Hundred Young Talents Plan” program (Project No. 220413508), and the raw
materials provided by Mr Yangsheng Chen of Yunfu Hongyuan Concrete Co. Ltd.
and Mr Shilin Huang of Yunfu Qijie Stone Co. Ltd.

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Figures

Figure 1 The marble waste addition methods

Figure 2 Marble dust generated in a stonework factory

Figure 3 MD supplied and MD after treatment

Figure 4 Particle size distributions of cement, marble dust and fine aggregate

Figure 5 SEM image and XRD pattern of MD

Figure 6 Cement content versus MD volume at different W/C ratios

Figure 7 SP dosage versus MD volume at different W/C ratios

Figure 8 Flow spread versus MD volume at different W/C ratios

Figure 9 Cube strength versus MD volume at different W/C ratios

Figure 10 SEM micrographs of mortar mix at 28 days

Figure 11 Cube strength versus cement content at different W/C ratios

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Water Water

Marble Cement Cement

waste

Aggregate Marble Aggregate

waste

(a) Cement replacement method (b) Aggregate replacement method

Water

Marble Paste
waste
Cement

Aggregate

(c) Paste replacement method

Figure 1 The marble waste addition methods

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(a) Shaping and polishing processes of marble block

Marble dust

(b) Marble dust on site

Figure 2 Marble dust generated in a stonework factory

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(a) MD supplied

(b) MD after treatment

Figure 3 MD supplied and MD after treatment

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100
Cumulative percentage passing (%) .

80
Cement Marble dust

60

40 Fine
aggregate

20

0
0.1 10 1000
Particle size (μm)

Figure 4 Particle size distributions of cement, marble dust and fine aggregate
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(a) SEM image of MD

6000
Ca2SiO4
5000 CaO
CaCO3
4000
I (CPS)

3000

2000

1000

0
20 30 40 50 60 70
2θ (°)

(b) XRD pattern of MD

Figure 5 SEM image and XRD pattern of MD

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900
. W/C = 0.40
W/C = 0.45
800
Cement content (kg/m3 )

W/C = 0.50
W/C = 0.55
700

600

500

400
0 5 10 15 20
MD volume (%)
(a) MD added as paste replacement

900
W/C = 0.40
W/C = 0.55
.

800
Cement content (kg/m3 )

700

600

500

400
0 5 10 15 20
MD volume (%)

(b) MD added as cement replacement

Figure 6 Cement content versus MD volume at different W/C ratios

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4.0

W/C = 0.40
W/C = 0.45
3.0
W/C = 0.50
SP dosage (%) .

W/C = 0.55

2.0

1.0

0.0
0 5 10 15 20
MD volume (%)
(a) MD added as paste replacement

4.0
W/C = 0.40
W/C = 0.55
3.0
SP dosage (%) .

2.0

1.0

0.0
0 5 10 15 20
MD volume (%)
(b) MD added as cement replacement

Figure 7 SP dosage versus MD volume at different W/C ratios

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500
W/C = 0.40
W/C = 0.45
Flow spread (mm) .

400 W/C = 0.50

W/C = 0.55

300

200

100
0 5 10 15 20
MD volume (%)
(a) MD added as paste replacement

500
W/C = 0.40
W/C = 0.55
400
Flow spread (mm) .

300

200

100

0
0 5 10 15 20
MD volume (%)
(b) MD added as cement replacement

Figure 8 Flow spread versus MD volume at different W/C ratios

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Strength (MPa) . 80

60

40 W/C = 0.40
W/C = 0.45
W/C = 0.50
W/C = 0.55
20
-5 0 5 10 15 20 25
MD volume (%)
(a) MD added as paste replacement

80
W/C = 0.40
W/C = 0.55
Strength (MPa) .

60

40

20
-5 0 5 10 15 20 25
MD volume (%)
(b) MD added as cement replacement

Figure 9 Cube strength versus MD volume at different W/C ratios

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(a) NM-0.40-0 (b) PR-0.40-20

(c) CR-0.40-20

Figure 10 SEM micrographs of mortar mix at 28 days

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80
W/C = 0.40
28-day cube strength (MPa) .

70 MD added as
paste replacement

60

MD added as
50 cement replacement

40
450 550 650 750 850 950
3
Cement content (kg/m )
(a) W/C = 0.40
60
W/C = 0.55
28-day cube strength (MPa) .

MD added as
50 paste replacement

40

MD added as
cement replacement
30

20
350 450 550 650 750 850
3
Cement content (kg/m )
(b) W/C = 0.55

Figure 11 Cube strength versus cement content at different W/C ratios

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1 28/7/2018
2
3 Recycling of marble dust as paste replacement for
4 improving strength, microstructure and eco-friendliness of mortar
5
6 L. G. Li1*, Z. H. Huang1, Y. P. Tan1, A. K. H. Kwan2 and H. Y. Chen1
7 1 Guangdong University of Technology, Guangzhou, China.
8 2 The University of Hong Kong, Hong Kong, China.
9
10
11 Highlights:
12
13  Recycling of marble dust as paste replacement in mortar/concrete is proposed.
14  Such usage of marble dust would decrease waste disposal and carbon footprint.
15  Moreover, such usage would also improve strength and microstructure of mortar.
16  Such usage also allows up to 33% reduction in cement content.
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28/7/2018
Tables

Table 1 Mix proportions of mortar mixes

Percentage
Marble Fine
Mix Water Cement reduction
dust aggregate
no. (kg/m3) (kg/m3) in cement
(kg/m3) (kg/m3)
content (%)
NM-0.40-0 333 832 0 1032 -
NM-0.45-0 350 778 0 1032 -
NM-0.50-0 365 731 0 1032 -
NM-0.55-0 379 689 0 1032 -
PR-0.40-5 305 762 137 1032 8.4
PR-0.45-5 321 713 137 1032 8.4
PR-0.50-5 335 670 137 1032 8.4
PR-0.55-5 347 631 137 1032 8.4
PR-0.40-10 277 693 274 1032 16.7
PR-0.45-10 292 648 274 1032 16.7
PR-0.50-10 304 609 274 1032 16.7
PR-0.55-10 316 574 274 1032 16.7
PR-0.40-15 250 624 411 1032 25.1
PR-0.45-15 263 583 411 1032 25.1
PR-0.50-15 274 548 411 1032 25.1
PR-0.55-15 284 516 411 1032 25.1
PR-0.40-20 222 555 548 1032 33.3
PR-0.45-20 233 519 548 1032 33.3
PR-0.50-20 244 487 548 1032 33.3
PR-0.55-20 252 459 548 1032 33.3
CR-0.40-5 333 790 37 1032 5.0
CR-0.55-5 379 654 31 1032 5.0
CR-0.40-10 333 749 74 1032 10.0
CR-0.55-10 379 620 61 1032 10.0
CR-0.40-15 333 707 110 1032 15.0
CR-0.55-15 379 585 92 1032 15.0
CR-0.40-20 333 666 147 1032 20.0
CR-0.55-20 379 551 122 1032 20.0

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Table 2 Test results of mortar mixes

28-day Percentage
SP Flow
Mix cube change in
dosage spread
no. strength 28-day cube
(%) (mm)
(MPa) strength (%)
NM-0.40-0 0.40 246 59.6 -
NM-0.45-0 0.37 273 49.2 -
NM-0.50-0 0.24 261 41.9 -
NM-0.55-0 0.10 243 39.5 -
PR-0.40-5 0.60 280 63.6 +6.7
PR-0.45-5 0.50 279 58.6 +19.1
PR-0.50-5 0.36 233 49.3 +17.7
PR-0.55-5 0.26 218 42.4 +7.3
PR-0.40-10 0.70 251 66.5 +11.6
PR-0.45-10 0.60 255 60.8 +23.6
PR-0.50-10 0.45 230 51.2 +22.2
PR-0.55-10 0.40 245 43.8 +10.9
PR-0.40-15 0.90 220 68.7 +15.3
PR-0.45-15 0.80 249 64.0 +30.1
PR-0.50-15 0.62 260 54.4 +29.8
PR-0.55-15 0.50 202 44.7 +13.2
PR-0.40-20 3.60 283 71.6 +20.1
PR-0.45-20 2.90 287 66.8 +35.8
PR-0.50-20 2.20 293 57.0 +36.0
PR-0.55-20 1.50 300 53.3 +34.9
CR-0.40-5 0.30 288 59.9 +0.5
CR-0.55-5 0.05 212 43.3 +9.6
CR-0.40-10 0.40 250 55.9 -6.2
CR-0.55-10 0.10 221 40.4 +2.3
CR-0.40-15 0.40 266 52.1 -12.6
CR-0.55-15 0.12 220 36.1 -8.6
CR-0.40-20 0.42 222 47.9 -19.6
CR-0.55-20 0.12 224 33.8 -14.4