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The use of waste mussel shells as an aggregate replacement in concrete

Conference Paper · September 2020

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 The use of waste mussel shells as an aggregate
replacement in concrete

C. A. Papadimitriou*, T. Anagnostopoulos, K. Anagnostopoulos, S.

Galinou – Mitsoudi

International Hellenic University, School of Engineering, Department of

Environmental Engineering, Sindos, 57400, Thessaloniki, Greece

*Corresponding author : chrysipapadimitriou@gmail.com

Abstract

Mussel culture is very important sector of the Greek agricultural economy with
an annual production of ~20000 t (2017, Eurostat). The majority of mussel
culture activities (80%) take place in the area of Central Macedonia, Thermaikos
Gulf NW Aegean Sea. In the area, local small scale industries process 12 t
mussels/day and produce unvalved fresh mussels which forward to the market.
Currently there is no legislation concerning the disposal of the mussel shells. In
the present project the feasibility of using shells as aggregates in the production
of concrete was investigated. In the present project the waste mussel shells were
dried and crushed into different aggregates ranging from coarse particulates to
powder.
Specimens were prepared by using various types of cements (CEM I 52.5N,
CEM IV/B (P-W) 32.5N and CEM II/A-M (W-L) 42.5R) and shells of different
size. Their 28-day compressive strength and elastic modulus was evaluated and
compared with the one of specimens made with compatible calcareous sand or
gravel. Waste mussel shells material showed characteristics, similar to limestone,
that enable them to be an inert material due to the high calcium oxide content.
However, proper treatment such as heating at high temperature and crushing to
achieve appropriate fineness are desirable for a better quality material. It was
shown that waste mussel shells could be utilized as a partial aggregate for
adequate workability and strength of concrete for non-structural purposes.

Keywords
calcium oxides, cement, concrete, waste mussel shells
1. INTRODUCTION

Every year, 6 to 8 million tons of waste crab, shrimp, oysters, mussels and lobster
shells are produced globally – about 1.5 million tons in Southeast [1]. In
developing countries, waste shells are often just dumped in landfill or the sea. In
developed countries, disposal can be costly. Yet shells harbor useful chemicals –
protein, calcium carbonate and chitin, a polymer similar to cellulose, but which
contains nitrogen. Mussel culture is very important sector of the Greek
agricultural economy with an annual production of ~20000 t (2017, Eurostat).
The majority of mussel culture activities (80%) take place in the area of Central
Macedonia, Thermaikos Gulf NW Aegean Sea. In the area, local small scale
industries process 12 t mussels/day and produce unvalved fresh mussels which
forward to the market. The production of completely unvalved mussels is taking
place only in Greece and thus there is an added value to the product by producing
vast quantities of waste shells that can be used in various environmental
applications [2]. Currently there is no legislation concerning the disposal of the
mussel shells.
The construction sector requires the use of vast quantities of raw/virgin materials
derived from natural resources. However in the last decade intensive efforts have
been made to introduce in concrete mixture activities, by products and wastes
from various industrial, agricultural or other alternative sources. Originating from
the fishery industry, seashell waste, such as oyster shells, mussel shells, and
scallop shells, among others, is available in huge quantities in certain regions,
and is usually dumped or landfilled without any reuse value. The characteristics
of different types of seashell waste, as well as the effects of incorporating the
seashells on the fresh and hardened properties of concrete, are discussed. The
material characteristics suggest that, similar to limestone, seashell waste could be
an inert material due to the high calcium oxide content. However, proper
treatment such as heating at high temperature and crushing to achieve appropriate
fineness are desirable for a better quality material. It is shown in past research
that while seashell waste has been used as a replacement for both cement and
aggregate, there is still a lack of investigation concerning its durability, as well as
the actual influence of seashell powder as a cement replacement material. Despite
the reduction in the workability and strength, based on the review, it is suggested
that seashell waste could still be utilized as a partial aggregate at a replacement
level of up to 20% for adequate workability and strength of concrete for non-
structural purposes. The current trend in concrete engineering is shifting towards
the sustainability aspect due to the depletion of natural concrete- making
materials as well as the environmental impact arising from the utilization of these
materials. Hence, there is an increased need of applying sustainable practices in
concrete production through the use of recycled waste materials as substitutes for
conventional materials in concrete. For this purpose, a number of studies have
been carried out to utilize wastes originating from different sources, such as
construction and demolition waste [3,4], and from a variety of industries
including steel [5], agricultural [6–8], glass [9], and rubber [10], among others.
These wastes are available in huge volume in certain countries, and, hence, have
the potential to be reused in large-scale concrete production. The utilization of
waste materials in concrete could moderate the problem of excessive
consumption of conventional materials as well as reduce the amount of
wasteshells generated. In the present project the feasibility of using mussel shells
as aggregates in the production of concrete was investigated, the results of the
study are of particular importance for Greece and especially the area of
Thessaloniki, where vast amounts of mussel shells are disposed under no
regulation in close proximity to RAMSAR and NATURA 2000 protected site of
Axios. The investigation of reuse or utilization of waste shells can attribute to the
decision making upon the sustainable management practices in the specific area.

2. MATERIALS AND METHODS

For the purpose of this study, three types of Portland cement (code-named CEM I
52.5 N, CEM II/A-M (W-L) 42.5 R and CEM IV/B (P-W) 32.5 N according to
EN 197-1) were selected. The compositions of these cements are presented in
Table 1 both in terms of oxides and in terms of the raw materials utilized for their
production.

Table 1.
Composition of cements and mussel shells.

Oxides (%) Cement type Mussel shells

Components I II/A-M IV/B Parameter Concentration
(%)
Si2O3 19.38 19.60 29.99 Organic content 7.5 %
Al2O3 4.28 5.90 11.22 Dry content 99.1%
Fe2O3 3.24 3.50 3.83 Kjeldahl Nitrogen 0.57 %
CaO 64.11 60.40 47.92 Ca (as CaCO3) 97.1 %
MgO 3.43 2.20 2.14 K 148.8 mg/kg
K2O 0.57 0.60 0.95 Mg 1660.2 mg/kg
Na2O 0.17 0.42 0.38 Cd 0.1 mg/kg
Na2Oeq 0.55 0.94 1.1 Cr 1.1 mg/kg
SO3 3.09 3.20 2.6 Cu 37.4 mg/kg
LOI 3.73 6.32 2.56 Pb 0.6 mg/kg
Zn 2.8 mg/kg
Clinker 90.3 80 58 Ni 0.2 mg/kg
Limestone 4.7 6.00 2 P 152.8 mg/kg
Pozzolan 0 7.30 20
Fly ash 0 5.40 18
Gypsum 5 5 2

For the preparation of natural aggregate concretes (reference concretes) and

mussel shell concretes, natural and waste mussel shell aggregates were used.
Natural aggregates came from crushed limestone. Mussel shell aggregates were
produced by hydration of waste mussel shells in an oven at 110oC for 24h, and
afterwards by crushing and sieving the dry material. The size fractions used for
both natural or mussel shell aggregates were a sand fraction of 1.19-2.38 mm,
and two gravels, with a 2.38-4.76 mm fraction, and a 4.76-12.7 mm fraction (Fig.
1). The composition of mussel shells is presented in Table 1.
All the studied concretes were prepared with a constant water/cement (w/c) ratio
of 0.5. The details of the mixing proportions of the different concretes are given
inTable2.The preparation of concrete specimens, curing and storage followed the
instructions of ASTM C192-18. The assessment of unconfined compressive
strength and elastic modulus of the different concrete mixes was performed at
28days of curing on cubic specimens (150mmx50mmx50mm) under a constant
strain rate of 0.0043 mm/mm/sec. An Instron servohydraulic (model 4500KPX J4
Static Hydraulic Universal Testing System) compression testing machine was
used for all the compression tests. It incorporates a linearly variable differential
transformer (LVDT) and a load cell linked to a data logger-computer for the
 recording of stress-strain during the test. The elastic modulus was calculated from
the elastic part of the compressive stress-strain curve according to ASTM C469-
10.

(a) (b) (c)

Figure 1.
Mussel shell fractions; (a) Gravel 4.76/12.7 mm; (b) Gravel 2.38/4.76 mm;
and (c) Sand 1.19/2.38 mm.

Table 2.
Mix proportions and notations of the modules.

Water/ Water Cement Coarse gravel Coarse gravel Sand Type of cement
Cement (kg/m3) (kg/m3) aggregates aggregates aggregates
ratio (kg/m3) (kg/m3) (kg/m3)
12.7> d > 4.76 4.76> d> 2.38> d > 1.19
Notation* (mm) 2.38(mm) (mm)
S1 0.5 249 498 1451 - - CEM I 52.5 N
S2 0.5 259 518 - 1475 - CEM I 52.5 N
S3 0.5 298 596 - - 1414 CEM I 52.5 N
S4 0.5 249 498 1451 - - CEM II/A-M (W-L)
42.5 R
S5 0.5 259 518 - 1475 - CEM II/A-M (W-L)
42.5 R
S6 0.5 298 596 - - 1414 CEM II/A-M (W-L)
42.5 R
S7 0.5 249 498 1451 - - CEM IV/B (P-W) 32.5 N
S8 0.5 259 518 - 1475 - CEM IV/B (P-W) 32.5 N
S9 0.5 298 596 - - 1414 CEM IV/B (P-W) 32.5 N
M1 0.5 405 810 760 - - CEM I 52.5 N
M2 0.5 285 570 - 1129 - CEM I 52.5 N
M3 0.5 285 570 - - 1114 CEM I 52.5 N
M4 0.5 405 810 760 - - CEM II/A-M (W-L)
42.5 R
M5 0.5 285 570 - 1129 - CEM II/A-M (W-L)
42.5 R
M6 0.5 285 570 - - 1114 CEM II/A-M (W-L)
42.5 R
M7 0.5 405 810 760 - - CEM IV/B (P-W) 32.5 N
M8 0.5 285 570 - 1129 - CEM IV/B (P-W) 32.5 N
M9 0.5 285 570 - - 1114 CEM IV/B (P-W) 32.5 N
*Letters S and M denote a natural aggregate concrete and a mussel aggregate concrete, respectively

Each of the reported compressive strength and elastic modulus values correspond
to the average value of at least three specimens that have strength values that
deviate no more than 5% from the average value of all tested specimens made
from the same concrete mixture.
Porosity of concrete specimens was estimated with the use of vacuum saturation
technique conforming to ASTM C 1202-19.

3. RESULTS AND DISCUSSION

It is well known that the porosity is a crucial parameter that influences the
strength of porous materials, such as concrete. Table 3 presents the porosity of
the reference and mussel shell concretes. It is clearly seen that the porosity of all
mussel concrete specimens is very similar (slightly higher) to the one of reference
concrete specimens. Thus, in this study, the investigation of the potential
difference between the strength of natural aggregate and mussel concretes is
based solely on the cement type and amount, and particle size of aggregate in
relation with the quality of aggregate utilized for concrete mixes.

Table 3.
Porosity of different concretes.

Notation Porosity (%)

S1 9.6
S2 9.7
S3 9.4
S4 8.25
S5 8.5
S6 8
S7 10.7
S8 10.6
S9 12.5
M1 11.8
M2 12.1
M3 12.7
M4 8.8
M5 8.76
M6 8.5
M7 13.1
M8 12.7
M9 14.2

Figures 2 and 3 present the compressive strength and elastic modulus,

respectively, of the reference and mussel concretes obtained at 28 days of curing.
From these results, it can be seen that the mechanical parameters decreased for all
concretes containing gravel or sand mussel. Nguyen et al. (2013) reported the
same conclusion. A possible explanation for the aforementioned results is that the
low strength of mussel aggregate can strongly influence the overall mechanical
behavior of the material [11]. Another possible explanation is the reduced
strength of cement paste-mussel aggregate due to low strength bonds due to the
presence of chitin in nacre layer, which as organic polymer decreases the pull
force of inorganic compounds of cement agglomerates [15, 16].
The presence of weak interfacial zones or cracks, undoubtedly harm the
mechanical properties of the composite [12]. Garcia et al. (2017) performed
scanning electron microscopy analysis on specimens of mussel structural
concrete and showed that the interface between the outer part of shell and cement
paste had some little cracks and a high presence of pores, whereas the interfacial
zone of the inner part of shell (nacre layer) demonstrated an absolute lack of
bond, showing high porosity in form of cavities, however it should be underlined
that the differences in the particulate matters and the drying methods between the
studies can exhibit variabilities in the amount of chitin presence. Two significant
factors that determine the presence of chitin is the age and the species of the
mussels used. In the present study it was observed that particles of the larger
diameter showed decreased ability in forming bonds, such as agglomeration or
sedimentation, on the outer or inner surface of mussel, however further studies
will be conducted in order to investigate the mechanisms of bonding and the
inhibiting factors effecting them.

Figure 2.
Compressive Strength (MPa) of the specimens.
Figure 3.
Elastic modulus (GPa) of the specimens.
In general, the decrease of compressive strength and elastic modulus of mussel
concretes ranged from 16.1 to 39.8 % and 17.4 to 39.1 %, respectively (Table 5).
Specifically, the cement type affected significantly the strength parameters of all
mussel mixes. The use of CEM II/A-M (W-L) 42.5 R was found to result in less
decrement of strength, 16.1 to 31 % and 17.4 to 22 % for compressive strength
and elastic modulus, respectively, whereas mussel concretes prepared with
cement type CEM IV/B (P-W) 32.5 N appeared to have the larger decrement in
strength, 31 to 39.8 % and 31.1 to 39.1 % for compressive strength and elastic
modulus, respectively.

Table 5.
Reduction of strength parameters of mussel shell concretes.

Compressive Elastic modulus

Notation strength (%) (%)
M1 31.9 28.9
M2 26.3 29.7
M3 25.6 23.1
M4 31 22
M5 21.4 21.6
M6 16.1 17.4
M7 31 35.9
M8 37.9 31.1
M9 39.8 39.1

It has long been established that the strength of concrete is related not only to the
hydrates of cement paste and their strength development but also to the porosity.
An inspection of the porosity test results indicates that the utilization of CEM
II/A-M (W-L) 42.5 R had a more pronounced effect on the reduction of porosity
for both reference and mussel concretes, a fact that is attributed to the
incorporated pozzolanic substances. The most effective action of this type of
cement is clearly seen in the case of M5 and M6 mussel concretes containing
almost the same amount of cement with the reference ones, which demonstrated
limited strength reduction ranged from 16.1 to 21.4 % and 17.4 to 21.6 % for
compressive strength and elastic modulus, respectively.
The test results also demonstrated that the aggregate fraction plays an important
role in the strength development of mussel concretes. The most impressive
observation was that mussel concretes (code named M1, M4 and M7) made with
the coarser gravel aggregate (4.76 – 12.7 mm fraction) showed strength values
lower than the one of reference concretes with much less cement content, for all
types of cement. An explanation for this result is the one proposed by Garcia et
al. (2017), who stated that the flat and flaky shape of the mussel aggregates,
especially the one of the mussel gravel, act as a barrier to the bleeding water
which increases the water to cement ratio in the downward face of the shell,
resulting in a weaker bond between the two phases (cement paste-aggregate), and
hence, in a worst concrete strength. This hypothesis of aggregate size effect on
concrete strength is corroborated by the experimental results obtained for the
finer fraction (sand mussel concretes M3 and M6), which exhibited the lower
decrements in compressive strength and elastic modulus when cement types of
CEM I 52.5 N and CEM II/A-M (W-L) 42.5 R were used.
4. CONCLUSIONS

This project studied the use of mussel shells as a total replacement of aggregates
in concrete. Experimental tests performed on different mussel concrete specimens
showed that their strength was lower than the one of natural aggregate concretes
and depended strongly on the aggregate size and cement type. The results lead to
establishing that a fine fraction of mussel shells when combined with a complex
type cement of high strength and containing pozzolan and ground limestone
could give a concrete with strength properties comparable to the conventional
one and can be used for non structural purposes.

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