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Advances in the Production of a Cement Substitute from
Fermentation Residues
Journal: Energy Sources, Part A: Recovery, Utilization, and Environmental Effects
Manuscript ID UESO-2019-1904
Manuscript Type: Original Article
Date Submitted by the
Author:
08-Oct-2019
Complete List of Authors: Maroušek, Josef; The Institute of Technology and Business in České
Budějovice
Maroušková, Anna; The Institute of Technology and Business in České
Budějovice,
Kůs, Tomáš; The Institute of Technology and Business in České
Budějovice
Keywords:
fermentation residues, pyrolysis, particulate matter, bioeconomy,
developing countries
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Energy Sources, Part A: Recovery, Utilization, and Environmental Effects
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Title:
Advances in the Production of a Cement Substitute from Fermentation Residues
Authors:
Josef Maroušek*, Anna Maroušková, Tomáš Kůs
Abbreviation (all):
Institute of Technology and Business in České Budějovice
Contact:
* corresponding author (josef.marousek@gmail.com, +420 777 987 683)
Abstract:
The amount of fermentation residues from biogas stations is rising rapidly worldwide.
Nevertheless, farmers are losing their interest in its incorporation into soil since the level of
nutrients as well as the agrochemical value of the organic matter present is low. Unlike
combustion (carried out in the presence of oxygen), the product of which is ash, pyrolysis
(without oxygen) turns biowaste into a highly porous carbonaceous material that can
substitute cement, one of the most energy-intensive mass-produced materials in the world.
This practice is booming in developing countries. Due to saving and inexperience, farmers or
local communities do not apply the technologies to utilize or filter the hazardous gaseous
products of pyrolysis. However, these contain high levels of particulate matter (PM) that
absorbs hazardous cocktails and facilitates their spread to the surroundings. An inexpensive
and easily producible shower cooler was designed and analyzed in full operation. The results
obtained suggest that the proposed solution can significantly reduce a wide range of PM sizes,
creating preconditions for reducing negative impacts on the environment as well as health of
locals.
Keywords:
fermentation residues; pyrolysis; particulate matter; bioeconomy; developing countries
Introduction:
Biogas production, in addition to food industry and biorefining technologies, produces huge
amounts of fermentation residues worldwide (Maroušek et al., 2018). The application of
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fermentation residues into arable land is raising economic and agronomic concerns among
farmers because the level of nutrients is low (some 3 % in total) and these must first undergo
mineralization via soil biota (slow and lossy process) to become available for plant nutrition
(Vochozka et al., 2017). Furthermore, the agrochemical value of the organic matter in
fermentation residues is disputed (Kolář et al., 2008) which altogether results in soil
degradation, in particular worsening of the water retention capacity (Smetanová et al., 2013).
There are growing reservations towards the landfilling of biowaste since it is considerably
bulky and its subsequent biodegradation worsens the stability of landfills, not to mention the
unnecessary production of greenhouse gases (Chavez et al., 2019).
The building industry and, particularly, the cement industry are among the most significant
emitters of CO2 in the world (Stehel et al., 2018). Ordinary concrete typically contains about
12% of cement (Salas et al., 2016). The global production of cement has grown rapidly in
recent decades; it is the third–largest source of anthropogenic emissions after fossil fuels and
land use change (Andrew, 2018). Cement plants release some 7% of global CO2, while 900 kg
of CO2 is emitted per 1.000 kg of cement. Its cumulative emissions from 1928 to 2016 were
39.3 ± 2.4 Gt CO2, 66 % of which have occurred since 1990. However, such a picture is far
from complete; batching, mixing, transport, placement, consolidation, finishing and,
especially, waste management are not considered in these estimations (Salas et al., 2016). At
the same time, concrete industry is one of the largest industrial consumers of fresh water
(Maroušek et al., 2019a; Guo et al., 2017). In addition, producing a ton of Portland cement,
the most common hydraulic cement, requires about 4 GJ of energy, making it one of the most
energy-intensive mass-produced material on the globe (Malhotra, 1999). To make matters
worse, the cement manufacturing process produces millions of tons of cement kiln dust each
year, contributing to respiratory and pollution health risks (Huntzinger and Eatmon, 2009).
Emissions from cement production (typically NOx) react with O3 and volatile organic carbons
(VOCs) to form secondary particulate matter (PM). At ambient temperature and with an
excess of O2, NO is oxidized to NO2 (toxic by inhalation and causing irritation to the human
eye, nose and throat) which is a precursor to the hazardous HNO3 (Seangkiatiyuth et al.,
2011).
There are two main aspects of cement production that result in a significant environmental
burden. The first is the chemical reaction involved in the production of the main component
of cement, clinker, as carbonates (largely limestone, CaCO3) are decomposed into oxides
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(largely lime, CaO) and CO2 by the addition of heat (Boden et al., 2017). It should be noted
that the calcination process (driving off CO2 from CaCO3 to form CaO) accounts for roughly
half of the CO2 emitted, while the remaining carbon results from energy usage during the
production process (Huntzinger and Eatmon, 2009). The second source of emissions is the
combustion of fossil fuels to generate the significant energy required to heat the raw
ingredients to well over 1000 °C (preferably above 1400 °C), and these “energy” emissions,
including those from purchased electricity, could add a further 60 % on top of the process
emissions (Andrew, 2018). Furthermore, mining large quantities of raw materials such as
limestone and clay and fuel such as coal often results in extensive deforestation and soil
degradation (Vochozka et al., 2017; Mehta, 2001).
Benhelal et al. (2013) proposed three strategies of CO2 reduction, including energy saving,
carbon separation and storage, as well the use of alternative materials. In the case of energy
saving approaches, moving from a wet to a more efficient dry process with a calciner has
since then reduced up to 50% of the required energy and mitigated almost 20% of CO2
emissions, but other options are not widely known (Salas et al., 2016). Modern cement plants
tend to have high energy efficiency and the scope for reducing CO2 emissions by further
efficiency improvements was found to have little environmental saving in comparison to the
dry process (Barker et al., 2009). Economic challenges (40 € t–1 of CO2 avoided for a
European cement plant and 23 € t–1 for a plant located in Asia, Barker et al., 2009) present
considerable obstacles to implementing carbon capture and storage processes in cement plants
(Maroušek et al., 2019b). As far as alternative materials are concerned, fly ash, blast furnace
slag, palm oil waste, recycled concrete, zeolite and other materials have been used for
manufacturing blended cement (Salas et al., 2016). A plethora of experiments have shown
that the incorporation of raw biomass into concrete results in inconsistent mechanical
properties (Britt and Kangas, 2016). Many have experimented with biomass ash that is more
homogeneous (Matalkah et al., 2016). Biomass ash, however, like fossil ash, produces round
conglomerates, which show little chemical reactivity due to their minimalist surface and thus
tend to degrade the quality of concrete (Katare and Maduwar, 2017).
Following the above, most attention has recently been paid to charred biowaste (also known
as biochar) and its abilities to substitute cement (Gupta et al., 2018). Experimental results
suggest that the addition of biochar reduces the initial setting time and significantly improves
the early compressive strength of mortar. Biochar addition can impart ductility to mortar
under flexure, although flexural strength was not significantly influenced. Water penetration
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and sorptivity of mortar was significantly reduced due to the addition of biochar, indicating
higher impermeability in biochar-added mortar. It was also found that the addition of treated
biochar results in significantly higher mechanical strength and improved permeability. The
published findings show that 5% replacement of cement (by weight) by biochar improved the
28–day compressive strength of mortar by about 10%. However, the flowability of biochar–
mortar is reduced with a higher replacement rate. According to Choi et al. (2012), biochar
tends to absorb and hold a significant part of mixing water, thus resulting in a stiffer mix. The
physically absorbed water in biochar is later released during the hardening of mortar and can
contribute to internal curing. Roberts et al. (2009) state that depending on the type of
feedstock and preparation conditions used, biochar has the potential for reducing net
greenhouse gas emissions by about 870 kg CO2 per ton of dry feedstock, of which 62 – 66%
are realized from carbon capture and storage by the biomass feedstock of the biochar. It was
repeatedly and independently reported (Stehel et al., 2018; Katare and Maduwar, 2017;
Vochozka et al., 2017) that the addition of 1 % of biochar prepared at 800 °C improved the
modulus of rupture and fracture energy of cement by up to 61%. The study suggests that
biochar can act as micro-aggregates and improve the compressive strength, bending strength
and fracture energy of cement. The improvement in fracture energy due to the introduction of
biochar has been attributed to the tortuosity of the crack path. Biochar particles introduce
inhomogeneity in the matrix and attract crack paths towards them. The biochar particles have
the ability to absorb energy before failure, which improves fracture energy and bending
strength.
There is a wide consensus that biochar from fermentation residues has the potential for
successful deployment as an additive or substitute of cement, which would also promote
waste recycling and sequester high volume carbon in civil infrastructure. Nevertheless, during
biowaste pyrolysis, a large number of reactions take place in parallel and in series, including
dehydration, depolymerisation, isomerization, aromatisation, decarboxylation and charring,
altogether resulting in various solid, liquid and gaseous components. There is an increasing
demand for pyrolysis oil (free flowing organic liquid mixture, which generally consists of a
great amount of water and hundreds of organic compounds, such as acids, alcohols, ketones,
aldehydes, phenols, ethers, esters, sugars, furans, alkenes, nitrogen compounds and
miscellaneous oxygenates as well as solid particles, Razaei et al., 2014) while special devices
(flash pyrolysis) are being designed exactly for its production and subsequent upgrading (Kan
et al., 2016). Gases released from biomass pyrolysis consist of CO2, CO, H2, low carbon
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number hydrocarbons such as CH4; C2H6; C2H4 and C3H8, and small amounts of other gases,
such as NH3, NOx, SOx and alcohols of low carbon numbers. In terms of health effects,
especially the Particulate Matter (PM) plays a key role as it captures and drifts the VOCs
through the air over long distances (Madureira et al., 2016). PM10 refers to PM of
aerodynamic diameter above 10 μm, furthermore PM5, PM2.5 and PM1 for smaller (and thus
more reactive) diameters are established. Even in low concentrations (at the edge of
detection), the presence of PM and VOCs can lead to significant impacts on respiratory
health, such as low lung function, asthma and bronchitis. Many studies have shown that PM is
also contaminated with heavy metals and other hazardous pollutants such as polycyclic
aromatic hydrocarbons (PAHs) that can directly enter the body through inhalation, dermal
contact and oral ingestion exposure pathways (Wei et al., 2015). In particular, the smallest
PM is of increasing concern because it can be easily inhaled deep into the lungs (Khan et al.,
2010). As reviewed by Hossain and Davies (2013), pyrolysis gas has multiple potential
applications, such as production of individual gas components, including CH4, H2 or other
VOCs, or in production of liquid biofuels through synthesis. However, all of these require
sophisticated and costly equipment that is completely beyond the economic reality of small
farms and communities running the majority of biogas stations worldwide. Thus, for
economic reasons, most of the small pyrolysis units operating worldwide do not contain any
filtration device.
Hypothesis was build, whether the current situation can be improved by designing
undemanding shower cooler of the pyrolytic gas (se shown in Fig. 1) that would be
incorporated to the pyrolysis unit.
Methodology:
Fermentation residues were obtained from the Nedvědice biogas station (Czech Republic).
The technological design and the corresponding processing parameters of the biogas station as
well as the feedstock properties are traceable in Maroušek (2013). Fermentation residues were
kept at 4°C until analyzed on biochemical properties according to Kolář et al. (2008), the
results being stated in Tab. 1. An analysis of nutrients and heavy metals was carried out
according to Ratajová (2014) and is summarized in Tab. 2. The fermentation residues
(average particle size of 0.9 mm) were mechanically dewatered by a single helix press
(PHARMIX, s.r.o, Czech Republic), which operates at 16 revolutions per minute (rpm),
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representing a backpressure tension of 650 N that resulted in dewatering to 43 % volatile
solids (VS). The mechanically dewatered fermentation residues were subjected to the
continuous (150 kg hr–1) standardized UHL–07 pyrolysis unit (Aivotec, s.r.o., Czech
Republic). In brief, the pyrolysing apparatus consists of the entrance hopper equipped with an
inner vertical slow motion helix. The slowly rotating helix continuously compresses the
biowaste down into the mechanical turnstile located at the bottom of the hopper. The turnstile
provides a minimum air leakage to minimize combustion and related ash formation. The
turnstile leads to the pyrolysis chamber made up of a thick-walled refractory horizontal wide
cylinder, where the material is exposed to the external source of heat (for more construction
details see Hašková, 2017). 400 kg of dewatered residues were fed into the reactor and
pyrolysed at 250, 300, 350, 400 and 450 °C each (speed of the horizontal helix that is
responsible for the hydraulic retention time was set to 0.4 Hz, which corresponds to the delay
of the feedstock in the pyrolysis chamber for approximately 6 minutes), while the pyrolysis
gas was analyzed using the SPS30 PM sensor (Sensirion AG, Switzerland), which operates on
the laser-based scattering principle and is capable of detecting PM at 10; 5; 2.5; 1 and 0.5 µg
m-3) every second. Two groups of experiments (with and without the shower cooler, Fig. 1)
were performed. Statistics was carried out using the ZunZunSite3 software (zunzun.com)
where the fitting target is the lowest sum of the squared absolute error.
Results and Discussion:
Hawken et al. (2013) pointed out that only a negligible amount of all materials actually ends
up in the desired products, with most of the virgin materials returned to the environment as
harmful solid, liquid, and gaseous wastes. Mardoyan and Braun (2015) highlighted that it is
advisable to close the loops in extraction and manufacturing and turn biowaste into valuable
products. Almost two decades ago, Mehta (2001) predicted that an alternative concrete system
provides a model for the future, making concrete mixtures that shrink less, crack less, and
would be far more durable and resource-efficient than conventional Portland-cement concrete.
According to Škapa and Vochozka (2019) this prediction is coming true and charred biowaste
is the answer.
With regard to Tab. 1 and 2, it can be stated that the biochemical properties of the
fermentation residues used during the experiments are in good agreement with other literature
world-wide (Stehel et al., 2018), in particular with reports from developing countries (Kolář et
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al., 2008) where the cement substitute is currently produced most intensively (Matalkah et al.,
2016). This finding is a good prerequisite for the generalization the following knowledge.
Data plotted into Fig. 2 shows many remarkable and so far unpublished findings. It is firstly
observed that at lower temperatures, pyrolytic gas contains mostly medium-sized and bigger
particles and with increasing temperature, its amount is decreasing. The available literature
does not provide a reliable explanation for this phenomenon (Matalkah et al., 2016; Salas et
al., 2016; Rezaei; Roberts et al., 2009). It is hypothesized that lower temperatures are not
sufficient to release the finest particles; however, such a hypothesis requires more
experiments. In contrast, it can be deduced from the visualized data that the amount of the
finest PM increases with higher temperatures. Following the available literature
(Seangkiatiyuth et al., 2011; Huntzinger and Eatmon, 2009), one might conclude that higher
temperatures of the pyrolysis process could thus be more environmentally harmful (Madureira
et al., 2016), since these smallest particles reach the deepest parts of the respiratory system,
where they are most biologically harmful (Hossain and Davies, 2013; Khan et al., 2010).
Although such an observation requires further examination, it can be assumed that this is not
the case in the instance of pyrolysis gases - at the same time, it can be assumed that thermal
degradation of VOCs occurs at higher temperatures; therefore, the finest PM could be with
decreased levels of absorbed hazardous substances (Madureira et al., 2016; Khan et al., 2010).
With regard to the application of the shower cooler (PM data plotted into Fig. 3), the most
important of all is the fact that there has been a significant reduction in the PM released regardless
the PM size, the quantities are no longer in thousands but in hundreds. Data
visualization also reveals that bubbling and subsequent showering of pyrolysis gas via water
relatively efficiently captures large and medium PM, and its quantities remain relatively
unchanged regardless of the process temperature. This is in line with latest high-end filtration
units (Andrew, 2018; Hossain and Davies, 2013); which, however, are unaffordable in
developing countries. Nevertheless, the finest PM penetrates more easily through the showers.
Increasing the volume of dispersed water did not show a significant increase in its removal
either. It is worth noting that increased temperature also increases the amount of the finest PM
released, which is in agreement with Fig. 2. If, however, the above-stated hypothesis
regarding the reduction of harmful substances at higher operating temperatures proved valid,
this partial drawback would not be so important (Kan et al., 2016; Madureira et al., 2016).
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Hawken et al. (2013) claim that: 1) humans mine or grow or harvest materials whose daily
flow per person averages 20 times the person’s weight; 2) at least 93 % of this massflow is
lost in extraction and manufacturing, with no more than 7 % getting into products; 3) 6/7 of
those products, by mass, are consumer goods that are thrown away after a single or no use; 4)
thus, only 1 % of the original mass is retained in durable products; 5) of the material in those
durable products, only about 1/50 later returns to produce more value, either as compost or
from recycling and remanufacturing. Moreover, much of the waste is toxic. Following the
above, it is advisable to support the production of a cement substitute from fermentation
residues via the application of simple shower coolers as depicted in Fig. 1. Provided it is
equipped with a centrifugal pump for water (800W should provide the performance of 1.5 to 2
m3h-1 and the pressure of 0.4 MPa, operating with water at a temperature of up to 90°C) and
ventilator that operates some 200 m3h-1, the pressure loss in the shower cooler showed to be
some 250 Pa. In the developing world, this construction can be realized within 1 month for an
estimated $ 1,000.
Conclusion:
An undemanding shower cooler design was designed that allows reducing the amounts of PM
released during the pyrolysis of fermentation residues into a cement substitute by one decimal
place. There is a certain threshold where an increased intensity of pyrolytic gas washing no
longer results in increased PM captures. The finest PM is the most difficult to capture via the
showering technique. There is an indirect assumption that the finest PM that is formed during
pyrolysis at higher temperatures is less dangerous provided that higher temperatures break
down some of the hazardous compounds that are trapped on the PM.
Acknowledgement:
The authors would like to express their thanks to the Institute of Technology and Business in
České Budějovice, which supported the research through the grant SVV201903 (Technoeconomic
and environmental assessment of the use of liquid pyrolysis products in civil
engineering). At no stage did the Institute interfere with the work or its publication.
References:
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VS COD LP RP pH
69 ± 7 2 088 ± 105 9 ± 2 24 ± 4 7.7 ± 0.2
Tab. 1: Biochemical analysis of fermentation residues, where: VS = volatile solids (%); COD
= chemical oxygen demand (mg L-1); LP1 = labile pool of carbon (%); resistant pool of
carbon (%), all n = 12; α = 5.
As Cd Cr Cu Hg Mo
0.21 ± 0.15 ND 15.52 ± 1.64 12.09 ± 1.57 ND ND
Ni Pb Zn Ca Mg(MgO) P(P2O5)
2.43 ± 0.47 1.02 ± 0.63 31.10 ± 3.16 23.44 ± 6.91 16.75 ± 3.39 48.95 ± 4.77
Tab. 2: Analysis of fermentation residues on heavy metals and nutrients, where Ca is
expressed as CaO; Mg as MgO and P as P2O5, all n = 12; α = 5.
Fig. 1: Schema of the shower cooler, where: A= pyrolysis gas inlet pipe; B= water washing; C
= water showering; D = removal of scrubbed pyrolysis gas; E = water recycling; F = fan to
maintain pressure.
Fig. 2: Visualization of PM analyses obtained from standardized UHL–07 pyrolysis unit that
was not equipped with the shower cooler, where: the optimal fitting equation was found z = a
+ bx^0y^1 + cx^0y^2 + dx^1y^0 + fx^1y^1 + gx^1y^2; fitting target of lowest sum of
squared absolute error = 2.53E+04 a = -4.93E+01 b = 1.02E+02 c = -7.67E+00 d = 2.18E+00
f = -7.53E-01 g = 5.34E-02; degrees of freedom (error) = 14; degrees of freedom
(regression)= 5 Chi-squared: 25366.65; R-squared: 0.95; p-value: 6.44e-09; root mean
squared error = 35.61
Fig. 3: Visualization of PM analyses obtained from standardized UHL–07 pyrolysis unit that
was equipped with the shower cooler, where: the optimal fitting equation is the same as in
Fig. 2; fitting target of lowest sum of squared absolute error = 1.32E+04 a = 1.14E+01 b = -
0.51E+04 c = 1.24E+02 d = -0.31E-02 f = -2.09E+03 g = -2.44E-01; degrees of freedom
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(error) = 14; degrees of freedom (regression)= 5 Chi-squared: 12.30; R-squared: 0.96; pvalue:
3.03e-19; root mean squared error = 12.05.
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Fig. 1: Schema of the shower cooler, where: A= pyrolysis gas inlet pipe; B= water washing; C = water
showering; D = removal of scrubbed pyrolysis gas; E = water recycling; F = fan to maintain pressure.
128x296mm (96 x 96 DPI)
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Visualization of PM analyses obtained from standardized UHL–07 pyrolysis unit that was not equipped with
the shower cooler, where: the optimal fitting equation was found z = a + bx^0y^1 + cx^0y^2 + dx^1y^0
+ fx^1y^1 + gx^1y^2; fitting target of lowest sum of squared absolute error = 2.53E+04 a = -4.93E+01 b
= 1.02E+02 c = -7.67E+00 d = 2.18E+00 f = -7.53E-01 g = 5.34E-02; degrees of freedom (error) = 14;
degrees of freedom (regression)= 5 Chi-squared: 25366.65; R-squared: 0.95; p-value: 6.44e-09; root
mean squared error = 35.61
250x211mm (96 x 96 DPI)
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Visualization of PM analyses obtained from standardized UHL–07 pyrolysis unit that was equipped with the
shower cooler, where: the optimal fitting equation is the same as in Fig. 2; fitting target of lowest sum of
squared absolute error = 1.32E+04 a = 1.14E+01 b = -0.51E+04 c = 1.24E+02 d = -0.31E-02 f = -
2.09E+03 g = -2.44E-01; degrees of freedom (error) = 14; degrees of freedom (regression)= 5 Chisquared:
12.30; R-squared: 0.96; p-value: 3.03e-19; root mean squared error = 12.05.
259x218mm (96 x 96 DPI)
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