18/6/23, 21:21 Preliminary electrochemical cementation of high volume fly ash mortars - ScienceDirect

Construction and Building Materials

Volume 122, 30 September 2016, Pages 54-62

Preliminary electrochemical cementation of high volume fly ash

mortars
Juan Lizarazo-Marriaga , Fredy García , Camilo Higuera

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Abstract

This paper summarizes a research about the electrochemical activation of the cementitious properties of
fly ash. Taking into account that in recent years there have been various environmental issues associated
with the production of Portland cement (PC), the use of Fly Ash (FA) has been promoted in the production
of concrete. Traditionally, the use of fly ash has been possible through its blending with Portland cement
and as a geopolymeric cementitious material. In this research, a third technique for fly ash activation,
known as electro-mutagenesis, was investigated. This treatment consisted in the late hydration of fly ash
after the migration of ions from an external alkaline solution, by applying an electric field across the
hardened mortar. Solutions of sodium hydroxide and sodium silicate with different molar concentrations
were used as a source of alkaline ions. The electrical treatment was applied in many mortar samples using
high volume proportions of fly ash, a constant water to binder ratio, and a fixed aggregate content. After
treatment, the compressive strength, the ultrasonic pulse velocity, and the microstructure of the mortar
matrices were investigated. Results showed that the alkaline ions migrated into the hardened mortar
through the permeable capillary pores, reacted with the un-hydrated fly ash and mutated in new
hydration phases, producing an improvement in the physical properties of mortar.

Introduction

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18/6/23, 21:21 Preliminary electrochemical cementation of high volume fly ash mortars - ScienceDirect

Nowadays, environmental issues associated with the production of Portland cement (PC) are in the middle
of a global debate. It is estimated that the CO2 released during cement clinkering is around 0.7 to 0.9 tons
per ton of PC, meaning that the cement industry generates around 7% of total CO2 emissions worldwide [1],
[2]. For that reason, and because of the growing concrete demand, research on alternative materials has
increased. Among those alternative materials, fly ash (FA) appears to be as one of the most industrially
used, which is a by-product of thermal generation in coal power stations [3].

FA as a cementitious material has been used through “direct activation” using PC, in which the usual
replacement percentages range from 15 to 25% [4]. Additionally, in recent years geopolymers have become
popular, in which FA hydration is accomplished through a chemical “alkaline activation”. This chemical
process allows the transformation of a material with a partially or fully amorphous structure, in stable
cementitious compounds [5]. FA is a silicon-aluminous material, which reacts in presence of an alkali
hydroxide solution, producing synthetic silicon-aluminous solids, which can achieve similar
characteristics of PC hydrates [3], [6].

There are several chemical activators that can be employed with FA; however, the combination of sodium
hydroxide (NaOH) and sodium silicate (Na2SiO3) has been successfully reported in literature. In this case,
the sodium hydroxide generates the dissolution of FA in alumina (Al) and silicon (Si), which are the main
precursors of the compounds produced in the hydration process. During the dissolution process, the
sodium silicate acts as a catalyst, increasing the reactions velocity [3], [7].

Electrochemical treatments in hardened concrete or mortar are based on electromigration, which can be
defined as the transport of ionic species under the influence of an electric field. Ions must move through a
tortuous path defined by the interconnection of capillary pores of the material, so, the transport equations
are defined similarly to the equations of transport in porous medium [8]. The general law governing the
ionic movements in cementitious materials is known as the Nernst–Planck equation [9].
where Ji is the flux of species i [mol/m2/s], Di is the diffusion coefficient of
species i [m2/s], ci is the ionic concentration of species i in the pore fluid [mol/m3], x is the distance [m], R
is the gas constant [8.31 J/mol/°K], T is the absolute temperature [°K], zi is the electrical charge of specie i, F
is the Faraday constant [9.65 × 104 Coulomb/mol], and E is the electrical potential [V].

Recently, a new process of electromigration has been used to mitigate damage and densify cementitious
matrices. This technique corresponds to the electrodeposition of nanoparticles within the capillary pores
of cementitious materials [10], [11], [12]. It has been reported that if in a reinforced concrete structure an
electric current is applied between the steel reinforcement (cathode) and an outer electrode (anode), it is
possible to lead the electrodeposition of external nanoparticles that could serve as a physical barrier and
prevent the entry of gases or contaminants within concrete [13], [14].

Electrodeposition is a novel and promising technique because it can help in many durability issues. It also
improves other physical properties such as the compressive strength and density. That increase is related
to the porosity reduction within the material during the electrochemical treatment, which is provided by
the pozzolanic materials that migrate into concrete. The driving electrical forces produce late hydration
products. In literature, this process is better known as electro-mutagenesis [15].

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18/6/23, 21:21 Preliminary electrochemical cementation of high volume fly ash mortars - ScienceDirect

Based on a preliminary research [16], a more detailed research program was carried out regarding the
electrochemical activation of high volume fly ash mortars. This paper summarizes the results of that
experimental study about the activation process of FA by applying an electrochemical method. The
treatment consisted on the electrical migration of alkali ions within hardened mortar samples previously
cast using high volume FA. For the experimental setup, cells with external reservoirs containing sodium
hydroxide and sodium silicate solutions, with different molar concentrations, were used. After the
electrochemical process, the compressive strength, the ultrasonic pulse velocity and the microstructure
were assessed.

Section snippets

Raw materials

All mortar mixes were cast using natural sand and a constant aggregate content. Fig. 1 shows the size
distribution for the aggregate used in this research. Fig. 2 shows the physical appearance of the aggregate,
with individual particles viewed through SEM at a magnification of 34×. From X-ray fluorescence, it was
determined that the natural sand (aggregate) was mainly siliceous holding a 98% SiO2 content. The physical
properties of aggregates are summarized in Table 1.

Commercial hydraulic ASTM C1157 ↗…

Voltage evolution

The voltage measured on samples subjected to electrochemical treatments was related to the mortar
resistivity and the external electric current applied according to Ohm’s Law. As the current through the
mortar samples was constant, the voltage evolved. Fig. 7 shows the voltage evolution of mortar samples
during the electrochemical treatment. It is possible to note that samples with higher cement content, (60%
fly ash + 40% Portland cement) have the highest initial voltage compared with samples…

Chemical electro-mutagenic activation theoretical model

Based on the results of the previous tests, an initial qualitative model of the fly ash electrochemical
activation process was developed, which approximates the physical interactions involved. Nowadays, the
research in this subject is in progress, in order to determine quantitative descriptions of the
electrochemical alkaline activation, much further research work is necessary.

Fig. 11 shows the preliminary conceptual model of the electrochemical activation process proposed in this
research. This …

Conclusions

Based on aforementioned results and commentaries, the following conclusions can be drawn:
• The chemical electro-mutagenic activation has been researched successfully with an experimental set
of mortar samples and tests. As a result, a theoretical model of the chemical electro-mutagenic

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18/6/23, 21:21 Preliminary electrochemical cementation of high volume fly ash mortars - ScienceDirect

activation process has been proposed.…

• According to the results achieved, it is possible to activate the fly ash as a cement material by a chemical
electro-mutagenic activation process.…

• The electrochemical activation…

Acknowledgement
This work was supported by COLCIENCIAS and National University of Colombia-Bogotá, Project Young
Researchers 2013-Call 617.…

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There are more references available in the full text version of this article.

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…For these reasons, and because of the growing demand for concrete, research on supplementary cementitious materials
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Fly ash (FA) is a powdery substance discharged by power plants after burning coal or other fossil raw
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properties of building materials will undergo deterioration at high temperatures. Therefore, in this study,
the influence of heat treatment at high temperatures on FA cement mortar is examined in relation to the
color and thermal conductivity changes. Color changes are an apparent indicator, for example, of the

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18/6/23, 21:21 Preliminary electrochemical cementation of high volume fly ash mortars - ScienceDirect

variation in moisture content. Thermal conductivity ( ) is an important parameter for evaluating the heat
transport properties of materials. Mass loss and density also affect thermal conductivity. In this study, 15 FA
cement mortar samples are made from mixtures that contain 3 different FA replacement percentages: 10%,
20% and 40%, for a total of 45 samples. The samples undergo heat treatment at temperatures that range
from room temperature to 800 °C before testing is carried out. A color meter and a thermal conductivity
tester are used to obtain the color parameters L∗, a∗, b∗ and thermal conductivity, respectively. The samples
are also sprayed with a phenolphthalein reagent after treatment to qualitatively observe the changes in pH.
It is found that a temperature range of 400–600 °C is critical in which the pH of the mortar decreases due to
carbonization and the decomposition of calcium hydroxide, which lead reduced lifespan of the FA cement
mortar. The thermal conductivity also decreases at higher temperatures, and is linearly correlated with the
density ratio. The experimental results show that the FA percentage has a considerable influence and
therefore, there could be an optimum FA percentage.

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…Hence, in this study, according to our previous work, two kinds of solid wastes were used as the main raw materials.
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For the purpose of building energy-saving, a novel one-piece wall ceramic board was prepared by using fly
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…The production of one ton of OPC requires 4 GJ of energy and emits approximately 1.35 billion tons of CO2 into the
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