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Journal of Cleaner Production 180 (2018) 716e727

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Journal of Cleaner Production


journal homepage: www.elsevier.com/locate/jclepro

Life cycle assessment of defluoridation of water using laterite soil


based adsorbents
Vineet Kumar Rathore, Prasenjit Mondal*
Indian Institute of Technology Roorkee, Roorkee, 247667, Uttarakhand, India

a r t i c l e i n f o a b s t r a c t

Article history: The present study deals with the life cycle assessment (LCA) of defluoridation of water using thermally
Received 10 April 2017 treated laterite (TTL), acid treated laterite (ATL) and acid-base treated laterite (ABTL). The scope of LCA
Received in revised form study consists of cradle to grave approach (i.e., from the acquisition of raw materials to the management
18 January 2018
of spent adsorbent). Environmental impacts associated with the defluoridation process are interpreted
Accepted 21 January 2018
with the help of CML 2001 and TRACI methods using GaBi 6.0 software. All calculations are based on the
amount of adsorbent required to reduce fluoride concentration from 10 mg/L to 1.5 mg/L of 720 L water.
The results from life cycle impact assessment reveal that the overall impacts are highest for TTL followed
Keywords:
Fluoride
by ABTL and ATL. The fluoride adsorption capacity of adsorbents is found as the key factor influencing
Adsorption environmental impacts. Further, through sensitivity analysis, loading capacity of the vehicle and the
Surface modified laterite soil distance between the mining and the processing site are found to play important role in environmental
Life cycle assessment degradation, which can be reduced by selecting a vehicle with lower loading capacity due to its higher
Groundwater fuel economy.
© 2018 Elsevier Ltd. All rights reserved.

1. Introduction adsorption has gained most interest due to its low initial cost, low
energy requirement, simplicity of design and possibility to reuse
Groundwater contamination with various types of organic and the spent adsorbent via regeneration. Further, most of the adsor-
inorganic pollutants has posed a serious threat on human health bents reported for the remediation of high fluoride-containing
around the world. Prolonged consumption of water containing an water are based on aluminum and iron due to their high affinity
excess amount of fluoride may lead to many types of diseases like towards it (Jagtap et al., 2012).
bone and skeletal fluorosis and mottling of teeth (Jagtap et al., Natural clays and soils show good capability for scavenging
2012). The maximum permissible limit for fluoride in drinking many types of pollutants from water including fluoride (Vinati
water is 1.5 mg/L as per the guidelines of World Health Organiza- et al., 2015). Various types of clays and natural geological mate-
tion (WHO, 2011). rials like laterite soil (Sarkar et al., 2006), mechanochemically
The presence of fluoride in groundwater is reported in many activated kaolinites (Meenakshi et al., 2008), lanthanum modified
countries like India, China, Mexico, Argentina, Pakistan, Ethiopia, bentonite clay (Kamble et al., 2009) have been studied by different
Egypt, Saudi Arabia, Niger, USA etc. (Jadhav et al., 2015). China and researchers for the removal of fluoride from water. Surface modi-
India are the two most affected countries with nearly 35 and 26 fication of adsorbents has also attracted considerable attention in
million people respectively at fluoride risk (Jadhav et al., 2015). order to increase the adsorption capacity and selectivity of the
Many fluoride remediation techniques based on ion exchange, adsorbents (Maiti et al., 2011). Based on the above background, for
reverse osmosis, chemical reduction, electrodialysis, distillation, the present study, locally available laterite soil is chosen as the raw
biological processes, and adsorption have been reported by many material for adsorption of fluoride as it possesses a high amount of
researchers (Jagtap et al., 2012). Among these techniques, iron and aluminum. Further, in order to improve the adsorption
capacity of raw laterite soil, its surface is modified by three different
types of treatments viz. thermal treatment, acid treatment, and
* Corresponding author. Department of Chemical Engineering, Indian Institute of acid-base treatment. The adsorption capacities of these surface-
Technology Roorkee, Roorkee, Uttarakhand, 247667, India. modified adsorbents have been studied for removal of fluoride
E-mail addresses: vinchdch@iitr.ac.in (V.K. Rathore), pmondfch@iitr.ac.in
and reported elsewhere (Rathore et al., 2016).
(P. Mondal).

https://doi.org/10.1016/j.jclepro.2018.01.176
0959-6526/© 2018 Elsevier Ltd. All rights reserved.
V.K. Rathore, P. Mondal / Journal of Cleaner Production 180 (2018) 716e727 717

Surface modification increases the cost of the adsorption pro- amount of adsorbent required to reduce the fluoride concentration
cess and produces many environmental consequences. Thus, to get of 720 L of water from 10 mg/L to 1.5 mg/L. Selection of 720 L water
a suitable adsorbent for sustainable utilization, the life cycle anal- as a basis is based on the idea of developing a water filtration unit
ysis of the adsorbent is important, which not only considers the containing the present adsorbent, which can successfully work for
economic aspect but also includes the system thinking and concept 60 days to meet the drinking water requirement of a family with 4
of sustainability (Montalembert et al., 1992). Recently, in 2015, the members assuming 3 L of drinking water consumption per capita
LCA of activated alumina, aluminum oxide amended wood char, per day.
bone char, and alum based adsorbents, which are relatively costlier Patel et al. (2015) conducted an extensive investigation on the
than laterite soil based adsorbent for fluoride removal has been quality of groundwater in Ambagarh Chouki block, Rajnandgaon
reported by Yami et al. (2015). The study of LCA reported by Yami district, Chhattisgarh, India, by taking the samples from around 146
et al. (2015) was based on adsorbents having different origins and sites, including tube wells of Public Health Engineering Department
raw materials with respect to the present study. Moreover, in the (PHED), Government of Chhattisgarh, India and dug wells in 22
study by Yami et al. (2015), only normalized impacts are reported villages. The concentration of fluoride in the groundwater in that
and hence it is difficult to compare their environmental impacts area is reported between 3.7 mg/L to 27 mg/L along with other
with those of the present adsorbents. impurities including arsenic, with an average fluoride concentra-
The aim of LCA in the present paper is to evaluate impacts that tion of ~10 mg/L. There are many other states in India (e.g., Andhra
arise due to various processes including mining of the raw material, Pradesh, Gujarat, Uttar Pradesh, Tamil Nadu, Madhya Pradesh etc.)
transportation, physical and chemical processing and finally man- where the concentration of this contaminant is also observed above
agement of the spent adsorbent by solidification in the form of clay permissible limit (Jagtap et al., 2012). Due to this fact and consid-
bricks. The objective of this study is to provide a better under- ering the scenario, the initial concentration of fluoride in the water
standing of environmental impacts associated with fluoride ad- to be treated has been taken as 10 mg/L for the present study.
sorbents through the quantification and comparison of impacts. The scope of the present study includes all the stages starting
Moreover, the present manuscript can also help in understanding from the mining/collection of raw laterite soil to final disposal in
the intensity of impacts of the most important factors under the form of clay bricks. The usage phase is excluded from the study
different scenario through sensitivity analysis and selecting the and it is assumed that the total waste emissions associated with
most suitable option to lower the impacts of the overall process. this stage are negligible. The life cycle diagram of the adsorbent is
given in Fig. 1.
Based on the above-mentioned diagram it is important to clearly
2. Method define the system boundaries of the process. The system bound-
aries for the LCA of presently considered adsorbents are presented
2.1. Goal and scope of study through Fig. 2 (a) to (c).

The goal of present study is to perform LCA and compare the


2.2. Preparation of adsorbents
environmental impacts of three types of adsorbents prepared from
a locally/easily available natural material. The raw material for
2.2.1. Preparation of thermal treated laterite soil (TTL)
remediation of fluoride containing water was also selected such
For preparing TTL, raw laterite soil was crushed in a jaw crusher
that it is available easily in many parts of India and globally. The LCA
so as to make particles of proper size (1e1.7 mm diameter particle
of the materials was performed as per the protocol of the Inter-
size) and then it was thoroughly washed several times with tap
national Organization for Standardization (ISO 14040:2006, ISO
water and subsequently with distilled water in order to remove all
14044:2006), which consists of four phases: (1) Defining the goal
the dust, clay and other organic matters present on the surface of it.
and scope of problem, (2) Life cycle inventory analysis, (3) Life cycle
Then the laterite soil was heated in a hot air oven at 105  C for 6 h.
impact assessment, and (4) Interpretation of results (ISO
This material was assigned as thermally treated laterite soil.
14040:2006).
The present study addresses the problem of groundwater
contaminated with an excess quantity of fluoride and its treatment 2.2.2. Preparation of acid treated laterite soil (ATL)
with the help of soil based adsorbent. Soil, being a natural and very For preparing ATL, 50 g thermally treated laterite soil was added
low-cost raw material, makes it economically feasible and safe for in an excess quantity of 2N HCl (200 ml) and the solution was
the environment. The basis of all the calculations is defined as the heated at 70  C for 3 h with thorough agitation on a magnetic

Fig. 1. Life cycle diagram of adsorbent.


718 V.K. Rathore, P. Mondal / Journal of Cleaner Production 180 (2018) 716e727

stirrer. Thereafter, the solution was heated at 110  C without stir-


ring so as to distill the excess free HCl (approximately 60%). The acid
treatment of the laterite is also helpful in the development of
positive charge on its surface due to the inclusion of Hþ ions of acid
on the adsorbent surface, which facilitates the adsorption of F ions
from the solution (Maiti et al., 2010). Finally, the solution was
allowed to cool to room temperature and the solid mass was
separated from the solution by filtration, washed several times with
distilled water till the pH of the wash water reached to ~7 and was
dried in hot air oven at 110  C. This material was assigned as acid
treated laterite soil.

2.2.3. Preparation of acid-base treated laterite soil (ABTL)


For preparing ABTL, 200 ml of 2N HCl was added to 50 g ther-
mally treated laterite soil and the solution was heated at 70  C for
3 h with thorough agitation on a magnetic stirrer. Thereafter, the
solution was heated at 110  C without stirring so as to distill the
excess free HCl (approximately 60%). Then 200 ml distilled water
was added to this followed by addition of base (in the form of 4N
NaOH solution). It was added dropwise at room temperature under
constant stirring and the final pH of the mixture was adjusted to
nearly 6.5. The addition of base was done in order to hydrolyze the
iron and aluminum ions leached out during acid treatment to the
slurry, in the form of respective metal hydroxides (Maiti et al.,
2011). The so formed metal hydroxides were then allowed to pre-
cipitate over the residual laterite mass at the bottom by keeping the
mixture undisturbed for 24 h and the clear liquid forming at the top
was decanted. The mixture was further washed several times with
distilled water till the wash water was free from chloride ions.
Residual chloride in wash water was determined by titrating it with
AgNO3 in presence of potassium chromate with phenolphthalein as
indicator. Finally, the solid mass was filtered. The filtrate was dis-
carded and the residue, i.e., solid mass was kept in the oven to dry
at 110  C. The dried mass was assigned as acid-base treated laterite
soil.
Characterization of the adsorbents and details of studies related
to the determination of optimum conditions for the maximum
removal of fluoride with the help of ABTL as adsorbent has been
reported elsewhere (Rathore et al., 2016) and are found as pH 6,
adsorbent dose 20 gm/L, contact time 300 min, initial fluoride
concentration 10 mg/L and temperature 25  C.

2.3. Life Cycle Inventory analysis

Life Cycle Inventory (LCI) analysis provides quantitative infor-


mation about energy and raw material requirements, environ-
mental emissions and wastes generations in each step included in
the system boundaries. LCI takes the help of process flow diagrams
developed in the goal and scope section. The main emphasis in this
section is given on identification and quantification of the energy
and material used.
In the present case the main energy consuming factors were
collection of laterite soil from the site, transportation of raw laterite
from the mining site to the processing site, preliminary treatment
(e.g. size reduction, washing and drying), surface modification with
chemicals (in the case of acid treated and acid-base treated soil)
and final disposal of spent adsorbent. The manual collection of soil
on the site is considered. After the collection, the laterite was
transported for preliminary operations like crushing, screening,
washing, and other treatments.
Fig. 2. System boundary for TTL (a), ATL (b) and ABTL (c).
A life cycle impact analysis of inputs and outputs of materials
and energy during raw material acquisition, material processing
V.K. Rathore, P. Mondal / Journal of Cleaner Production 180 (2018) 716e727 719

and chemical treatment and disposal of the fluoride adsorbents i. Mining/collection of raw laterite from the site is assumed to
was obtained using two different methods namely, Centrum voor be carried out through human labor and not with the help of
Milieukunde, Leiden 2001 (CML 2001) and Tool for Reduction and any type of mechanical drillers or excavating machines. Thus,
Assessment of Chemicals and other Environmental Impacts the possible emissions associated with this step are
(TRACI). Life cycle models were built with the help of GaBi 6.0 neglected.
software and the impacts associated with each of the processes ii. The transportation of quarried out raw laterite soil is carried
were evaluated with the help of GaBi professional database 2016. out with the help of diesel engine trucks. Further, the average
All the inputs and emissions were calculated on the basis of transportation distance from the mining site to the pro-
appropriate material and energy balances. Due to lack of avail- cessing site is assumed as 5 km.
ability of data for Indian conditions for some of the processes, all iii. All the laterite soil collected is assumed to have uniform
the data presented in the study are given according to German physical and chemical composition. Therefore, any pre-
context except the transportation data which is presented in Global processing of the raw laterite to convert it into a usable
(GLO) context. A similar practice has been used by other re- form is not considered.
searchers also (Cavalett et al., 2013). The adsorption capacity of any iv. Heating of the laterite samples for drying after washing steps
adsorbent is an important factor in determining its applicability in and while giving it acid treatment is assumed to be carried
adsorption process as well as its environmental impacts. The ad- out in hot air ovens having a capacity to dry up to 50 kg of
sorbents having high adsorption capacity is required in less quan- material at a time and the calculations related to emissions
tity to treat any stipulated amount of water and vice versa. This from these processes are done accordingly.
factor can also be useful in the approximation of environmental v. It is assumed that during acid-base treatment step (for pro-
impacts. The fluoride adsorption capacity of any adsorbent at an ducing ABTL), the effluent does not consist of any leftover
equilibrium dissolved fluoride concentration of 1.5 mg/L (referred acid or base. This assumption is based on the fact that during
to hereafter as Q1.5, with units of mg F/g adsorbent) is a crucial the acid-base treatment, all the leftover acid is neutralized by
factor for comparing the magnitude of environmental impacts, the NaOH. Further, the amount of HCl and NaOH used in the
because the quantity of adsorbent required for fluoride removal process is very less. Thus, the environmental impacts asso-
(the functional unit) is governed by the fluoride adsorption ca- ciated with the synthesis of these chemicals are not
pacity. The value of Q1.5 can be determined as (Yami et al., 2015): considered.
  vi. The application step of the adsorbent for treating water is
Q1:5 mg=g ¼ Qmax bCe=ð1 þ bC Þ (1) assumed not to contribute significantly towards any of the
e impacts and therefore this step is also not considered.
vii. Losses in the mass of laterite soil in the form of undersized
where, Qmax is the Langmuir maximum adsorption capacity of particles and water vapors generating during drying and
adsorbent (mg/g), Ce is the concentration at equilibrium (i.e., surface modification of laterite are assumed not to produce
1.5 mg/L) and b is Langmuir adsorption constant. The amount of any significant impact on the environment and human
adsorbent required for reducing the concentration of fluoride to health.
desired concentration can be calculated from the values of Q1.5 viii. The environmental impacts imparted by the refinery for
using Eq. (2): producing diesel, which has been used for the transportation
of raw laterite is not considered. This is due to the fact that
Total mass of the adsorbent required ðgÞ ¼   ðC0  Ce ÞV=Q the LCA of production of diesel fuel from the crude oil is
1:5
(2) beyond the scope of the present study and should be carried
out separately.
where, C0 is the initial concentration of fluoride (i.e., 10 mg/L), Ce is ix. Biogas from biomass has been selected for generating elec-
the equilibrium concentration of fluoride (i.e., 1.5 mg/L) and V is the tricity for sintering the bricks made from spent adsorbent
volume of solution (i.e., 720 L). The values of Qmax, b, and Q1.5 (as and clay as it is assumed that biomass is available in abun-
calculated) are reported in Table 1. dant quantities in developing countries like India (web link
For preparing 55.63 kg TTL, 38.25 kg ATL, and 27.81 kg ABTL, the 2) and it would not be economically feasible to use electricity
amount of raw laterite required were found as approximately from grid mix. Moreover, the usage of direct burning of
382 kg, 310 kg, and 370 kg respectively. Further, for producing the materials like coal and other fossil fuels is also avoided as it
adsorbents, the energy requirements and loss of laterite during may result in even higher impacts to the environment.
each treatment steps are shown through Figs. S1eS3.

2.4. Assumptions 2.5. Impact assessment methodology and categories considered

The following assumptions were made for the present LCA Different life cycle impact assessment methods may lead to
study: distinct results in terms of values, impact categories, units etc.

Table 1
Langmuir isotherm constants for different adsorbents and their total mass required to lower the concentration of fluoride from 10 mg/L to 1.5 mg/L in 720 L water.

Adsorbent Langmuir isotherm constants Q1.5 (mg/g) Total mass of adsorbent required for treating 720 L of water (in kg)

ABTL Qmax ¼ 0.52 mg/g 0.22 27.81


b ¼ 1.50 L/mg
ATL Qmax ¼ 0.40 mg/g 0.16 38.25
b ¼ 0.44 L/mg
TTL Qmax ¼ 0.27 0.11 55.63
b ¼ 0.51 L/mg
720 V.K. Rathore, P. Mondal / Journal of Cleaner Production 180 (2018) 716e727

(Monteiro and Freire, 2012). Therefore, in order to interpret the on environmental impacts under different impact categories (in-
environmental impacts, two different methods viz. CML 2001 and dicators) for TTL, ATL and ABTL are shown in Figs. 3 (a), 4 (a) and 5
TRACI have been used in the present study. The main purpose of (a), respectively which are calculated by CML 2001 method. As
considering two different impact assessment methodologies is to evident from these figures, transportation of raw materials (by the
compare the results obtained through these methodologies and to truck trailer) and management of the spent adsorbents (with
verify their consistency for the present system. Characterization electricity from biogas) together contribute to more than 90% of the
factors of these two methodologies may vary as these are based on impacts for all the indicators except abiotic depletion potential
different geographical conditions. Therefore, a consistency in re- (ADP) elements. In this case (for ADP elements) contribution of the
sults of the environmental impacts interpreted by the above- truck trailer is not available and only electricity from biogas and
mentioned methodologies may ascertain their application in In- grid mixes are contributing to impacts. It is obvious as the truck is
dian context also. operated by diesel, which is a fossil fuel and hence it contributes
Both the methods follow midpoint oriented approaches that ADP fossils in spite of ADP elements (which is generally associated
characterize the impact categories based on the impacts that are with extraction of metals and their remaining reserves) as shown in
directly caused by emitted pollutants. In brief, the midpoint Figs. 3 (a), 4 (a), and 5 (a). It is interesting to note that the trend in
approach assesses the environmental impacts at intermittent stage the contribution of different operations on different impact cate-
of the cause-effect chain in the form of indicators like carbon di- gories for TTL and ATL are similar, however, for ABTL it is different
oxide (CO2), climate change, chlorofluorocarbon (CFC) for ozone for many impact categories such as ADP fossils, human toxicity
depletion, nitrogen oxides (NOx) for eutrophication, sulfur dioxide potential (HTP) and marine aquatic ecotoxicity potential (MAETP).
(SO2) for acidification, etc. On the other hand, end-point approach In the case of ABTL; ADP fossils, HTP and MAETP have significant
evaluates the environmental impacts at the areas of protection contributions from electricity production through grid mixes along
(AoP) level such as human health, ecosystem, and resource (Dong with electricity production from biogas. This is due to the fact that
and Ng, 2014). Moreover, the midpoint results are more compre- for the ABTL, surface modification of more mass of raw laterite soil
hensive to cover possible environmental interventions, while the is needed as compared to TTL and ATL, which in turn consumes
endpoint approach may neglect some aspects in deriving the more coal to produce required electricity for grid mixes. Further, a
damage indicators (Bare and Gloria, 2006). larger amount of wastes is produced during surface modification in
The advantage of selecting mid-point oriented approaches is case of ABTL, which accounts for higher values of HTP and MAETP.
that they are often better in predicting the results in the cause- From Figs. 3 (b), 4 (b), and 5 (b), it is evident that when impacts
effect chain between stressors (e.g., air quality, water quality, are calculated with TRACI method for TTL and ATL, the contribution
extreme temperature) and endpoint of the process. of transportation of raw materials (truck trailer) and management
The CML 2001 methodology for life cycle impact assessment is of the spent adsorbents (electricity from biogas) on the different
developed by the Institute of Environmental Sciences at the Uni- indicators are also more than 90%, however, for ABTL it is less than
versity of Leiden in the Netherlands. This methodology for life cycle 90% for the indicators like Ecotox Air, and Human Health Non
impact assessment is one of the most widely accepted methodol- Cancer air. In this case, other operations like electricity from grid
ogies (Trudewind et al., 2014) and primarily uses European data to mix play a significant role due to the addition of more drying step in
derive its impact factors (Cavalett et al., 2013). It groups the LCI case of ABTL production, unlike other adsorbents. Since, electricity
results into categories according to themes like common mecha- production emits acutely toxic gasses into the air, the values of
nisms (e.g. climate change) or groupings (e.g. ecotoxicity) (Web link Ecotox Air as well as Human Health Non-Cancer air are influenced
2). Due to its midpoint oriented nature, it models the problems at by electric grid mix. It is interesting to note that in the case of TRACI,
an early stage in the cause-effect chain, allowing a more trans- for ABTL, one extra contributor (Rest) is observed (Fig. 5b), which is
parent assessment and limiting the uncertainties (Monteiro and probably due to the use of more number of treatment steps and
Freire, 2012). material loss.
On the other hand, TRACI is an impact assessment methodology From Figs. 3e5, it seems that the contribution of different op-
developed by the US Environmental Protection Agency. Like other erations on the four common indicators such as GWP, AP, EP, and
life cycle impact assessment methodologies, TRACI is also primarily ODP are similar, although a slight variation in the contributions on
a midpoint approach but differs from the CML 2001 methodology AP is observed for all the adsorbents. This may be due to the vari-
as the data in the former one comes primarily from North American ation in the database in different methods.
sources (Zhou et al., 2011).
Both CML 2001 and TRACI methods include five similar impact 3.2. Normalization of data
categories, but they are represented by different indicators. For
example, human health is represented by Human Toxicity Potential The normalized value of the impacts of different categories for
(HTP) in CML 2001, while TRACI further divides it into three sub- TTL, ATL, and ABTL obtained through CML 2001 and TRACI methods
categories including carcinogenic, non-carcinogenic, and respira- are shown in Fig. 6 (a) and (b), respectively. From Fig. 6 (a), it is
tory impact potentials to better reflect the local health concerns evident that the indicator values (CML 2001) are maximum either
and regulatory focus (Zhou et al., 2011). Thus, the selection of for TTL or ABTL in most of the cases. The impacts of ATL are in
impact indicators is important for meaningful comparison of the between TTL and ABTL. To produce the stipulated amount of TTL
CML 2001 and TRACI methods. (55.63 kg), which is required to treat 720 L of fluoride contaminated
water, approximately 382 kg raw laterite is required. The trans-
3. Results and discussion portation of large quantities of raw laterite requires combustion of
fossil fuels, which produces greenhouse gases and consequently
3.1. Overview gives higher values of ODP, ADP (both elemental and fossil), FAETP
and TETP in impact assessment by CML 2001 method. Compara-
The contribution of different operations such as transportation tively less amount of raw laterite is required to produce sufficient
of raw materials (truck trailer), crushing of raw laterite (electricity amount of ATL for treating the same amount of water, so it creates
from grid mix 2) drying of adsorbents (electricity from grid mix 1) less impact in these categories. Similarly, the requirement of raw
and management of the spent adsorbents (electricity from biogas) laterite for the production of ABTL for the treatment of the same
V.K. Rathore, P. Mondal / Journal of Cleaner Production 180 (2018) 716e727 721

Fig. 3. Assessment of impacts by TTL estimated by CML 2001 (a) and TRACI (b) method.

amount of water is also high as a considerable amount of laterite Water. The highest contribution of ATL in these categories is
soil is lost during the chemical processing steps. Moreover, both observed due to the usage of HCl acid for surface modification of
energy and chemicals are needed for the surface modification of laterite soil. Although HCl is used for ABTL also, it is further
raw laterite to produce ABTL, which leads to its large contribution neutralized by the base and thus the contribution of ABTL on these
in the form of GWP, AP, EP, HTP, and MAETP in impact assessment indicators is less than ATL.
by CML 2001 method. On the basis of the above discussion, it seems that the overall
Further, almost similar trends are observed in impact assess- environmental impacts of TTL, ATL, and ABTL as determined by the
ment by TRACI method also for all the adsorbents (Fig. 6 (b)). The LCA study, follows the following order TTL > ABTL > ATL. It can be
TTL shows maximum impacts in several categories, which include explained by the fact that the adsorption capacity of TTL is very
GWP, AP, EP, Ecotox Soil, Ecotox Water, Human Health Cancer Air small as compared to ABTL (50% as compared to ABTL), therefore, it
and Smog Air. Similarly, ABTL shows maximum impacts in Ecotox accounts for usage of large quantity (382 kg) of raw materials to
Air, Human Health Criteria Air, and Human Health Non Cancer Air, produce sufficient quantity (55.63 kg) of adsorbent to treat 720 L of
whereas, ATL shows maximum impacts in remaining categories water. Further, in post adsorption process, about 55.63 kg of spent
like ODP, Human Health Cancer Soil, Human Health Cancer Water, adsorbent needs to be immobilized in the form of clay bricks (as it is
Human Health Non Cancer Soil and Human Health Non Cancer assumed that there is no loss in adsorbent mass during the
722 V.K. Rathore, P. Mondal / Journal of Cleaner Production 180 (2018) 716e727

Fig. 4. Assessment of impacts by ATL estimated by CML 2001 (a) and TRACI (b) method.

defluoridation process). It is observed that more laterite soil is the Q1.5 values of the present adsorbents are highly competitive to
required for the production of the required amount of ABTL than those of the previously reported adsorbents. The Q1.5 values for
that of ATL to treat 720 L water. The requirement of more amount of laterite soil, mechanochemically activated kaolinites, lanthanum
raw laterite for ABTL is due to some additional treatment steps for modified bentonite clay were reported as 0.098, 0.117 and
its production than ATL. On the other hand, it is observed that the 0.038 mg F/g respectively whereas, as for TTL, ATL and ABTL these
specific uptake of three adsorbents for fluoride increases in the values are 0.11, 0.16 and 0.36 mg F/g respectively. Further, no LCA
following order ABTL > ATL > TTL. Considering both environmental study was carried out for these adsorbents to assess their envi-
impacts and specific uptake, ABTL is found to be a suitable adsor- ronmental implications.
bent for fluoride removal from the contaminated water. It is also
able to reduce the fluoride concentration below 1.5 ppm from 3.3. Sensitivity analysis
initial fluoride concentration of 10 ppm as reported elsewhere
(Rathore et al., 2016). Sensitivity analysis was conducted in order to identify and
Comparing the present adsorbents with laterite soil, mecha- evaluate the process steps with maximum contributions on various
nochemically activated kaolinites, lanthanum modified bentonite impact categories as well as to find out the alternative options to
clay on the basis of their fluoride adsorption capacity at an equi- decrease the impacts varying their input values. For carrying
librium dissolved fluoride concentration of 1.5 mg/L, it seems that sensitivity analysis, the impacts to the environment and human
V.K. Rathore, P. Mondal / Journal of Cleaner Production 180 (2018) 716e727 723

Fig. 5. Assessment of impacts by ABTL estimated by CML 2001 (a) and TRACI (b) method.

health were quantified through CML 2001 method for all the ad- 1. A truck trailer having 5 ton carrying capacity and the distance
sorbents. On reviewing the quantified data of initial LCI analysis, it between the mining site and the processing site is assumed as
was observed that the transportation of the raw material was one of 5 km.
the major contributors in the impact categories like GWP, acidifi- 2. A truck trailer having 5 ton carrying capacity and the distance
cation potential and eutrophication potential due to emission of between the mining site and the processing site is assumed as
greenhouse gases and other gases like SOx, NOx etc., as indicated in 10 km.
the report of GaBi 6.0 software. Therefore, various options were 3. A truck trailer having 12.4 ton carrying capacity and the distance
considered to lower the impacts due to transportation step by between the mining site and the processing site is assumed as
varying the loading capacity of the truck trailer and the assumed 5 km.
distance between the mining site and the processing site. In the 4. A truck trailer having 12.4 ton carrying capacity and the distance
originally considered scenario, a truck trailer of 27 tons capacity between the mining site and the processing site is assumed as
was selected and the distance between the mining site and the 10 km.
processing site was assumed as 5 km. Alternatively, various other 5. A truck trailer having 17.3 ton carrying capacity and the distance
scenarios were considered, which are as follows: between the mining site and the processing site is assumed as
5 km.
724 V.K. Rathore, P. Mondal / Journal of Cleaner Production 180 (2018) 716e727

Fig. 6. Impact comparison using CML 2001 (a) and TRACI (b) method. The y-axis value for the adsorbent that had the maximum impact in each category was set equal to 100%, and
other values were normalized to this maximum value.

6. A truck trailer having 17.3 ton carrying capacity and the distance through these figures, on comparing the alternative scenarios with
between the mining site and the processing site is assumed as the originally presented scenario, a decrease in the impacts is
10 km. observed in all the above mentioned three categories when the
distance of carrying load is kept 5 km. In the case of a vehicle having
The carrying capacities of the vehicles were selected from the 5 ton loading capacity and transportation distance as 5 km, the
database of the GaBi 6.0 software and the other properties of impacts reduced to nearly 50% and by increasing the transportation
emissions were kept similar to the originally considered scenario distance of 10 km, it had almost similar impact as compared to
(like the composition of diesel used as fuel, emission standard of original scenario in all the three categories.
the vehicle was taken as Euro IV etc.). Moreover, for the present case, maximum amount of raw ma-
A comparison between initial results of LCI analysis under terial required is 382 kg for the synthesis of sufficient adsorbent (in
different scenarios is shown through Fig. 7 (a) to (c). As shown case of TTL) for the treatment of stipulated amount (720 L) of
Fig. 7. Comparison of effect of variation in transportation capacity of the truck trailer and the transportation distance on the global warming potential (a), acidification potential (b)
and eutrophication potential (c) under different scenarios.

Table 2
Total impact caused by each treatment step as per the CML 2001 method.

GWP 100 years (kg AP (kg SO2 EP (kg ODP, steady state (kg ADP elements (kg ADP fossil FAETP (kg HTP (kg DCB MAETP (kg TETP (kg DCB
CO2 equi.) equi.) phosphate R-11 equi.) Sb equi.) (MJ) DCB equi.) equi.) DCB equi.) equi.)
equi.)

TTL 14.67 0.1 2.25  102 2.57  1010 2.60  107 1.05  102 1.13  101 1.09 9.70  102 2.21  101
ATL 11.09 0.07 0.02 1.79  1010 1.86  107 73.45 0.08 0.76 674.46 0.154
ABTL 11.93 0.08 0.02 1.27  1009 1.12  107 64.29 0.06 1.02 2712.05 0.11
726 V.K. Rathore, P. Mondal / Journal of Cleaner Production 180 (2018) 716e727

contaminated water and a truck trailer having a default capacity of

Smog Air
5 tons would be sufficient to carry enough raw material to last for

(kg O3
equi.)
synthesis of 13 batches of TTL adsorbent. Similarly, a higher number

1.95
1.47
1.55
of batches of ATL (~16) and ABTL (~13.5) can be synthesized from 5
tons of raw laterite soil. By using light engine vehicles, the emis-

Human Health Human Health Human Health

Water (cases)
sions are less due to their high fuel economy and hence lesser

Non-Cancer Air Non-Cancer Soil Non-Cancer

6.82  109
4.05  108
2.92  108
emissions (Sivak and Schoettle, 2012; National Research Council,
2010).
More alternatives for the transportation of raw material like
railway or by air were not considered as the distance between the
7.10  107 mining site and the processing site is assumed to be very less (5 km)
4.88  106
3.5  106
and hence it cannot be economically feasible to use these.
(cases)

The total impact caused by each of the treatment steps under


original scenario (using a truck trailer of 27 tons capacity and the
distance between the mining site and the processing site taken as
5 km) is also given in Tables 2 and 3.
(cases)

4. Conclusion
3.44

6.03
2.4

In the LCA of defluoridation process, using three different ad-


Health Cancer Health Cancer Cancer Water Criteria Air (kg

sorbents made from raw laterite soil for the treatment of fluoride
Human Health Human Health

PM10 Equi.)

9.84  103

contaminated water, the environmental impacts are found to be


proportional to raw material requirement and inversely propor-
0.001
0.011

tional to the adsorption capacity of the adsorbent, which is in


agreement with the observations reported by Yami et al. (2015).
Normalization of impacts revealed that TTL produces maximum
2.10  109
1.43  108
1.02  108

impacts in few categories (ODP, ADP (minerals and fossils), FAETP


(cases)

and TETP) primarily due to larger amount of raw materials whereas


the ABTL produces maximum impact in other categories (GWP, AP,
EP, HTP, and MAETP) due to greater number of treatment steps and
1.13  109
7.79  109
5.58  109

use of chemicals when assessment is done with CML 2001 method.


Soil (cases)

Almost similar patterns of impacts are observed when the impacts


Human

are calculated with TRACI method. Sensitivity analysis of the ad-


sorbents revealed that most of the impacts to the environment and
human health are caused by transportation and production of
6.82  1010
8.93  109

5.00  109
Air (cases)

electricity from biogas. Moreover, as observed by Yami et al. (2015)


Human

also that in order to reduce the environmental and human impact,


the adsorption capacity of the adsorbents should be increased and
transportation of the raw materials should be minimized. The
Water (PAF
m3day/kg) m3day/kg) m3day/kg)

sensitivity analysis of the present LCA study revealed that the


Ecotox Air Ecotox Soil Ecotox

environmental impacts may be reduced by using a vehicle having


1.47
1.03
0.74

lower carrying capacity and reducing the distance between the


mining site of the raw laterite and the processing site.
(PAF

2.86
1.99
1.42

Acknowledgement
Total impact caused by each treatment step as per the TRACI method.

The authors acknowledge PE International, Germany for


providing GaBi 6 software for students and teachers along with
(PAF

2.30  102 2.74  1010 0.12


1.87  109 0.08
1.37  109 0.14

databases of various countries to estimate the impacts to the


environment and human health. The authors are also thankful to
Ministry of Drinking Water and Sanitation, Government of India, for
ODP (kg
CFC-11

providing financial support (project number: MRD-623-CHD) and


equi.)

Indian Institute of Technology Roorkee, Roorkee (India) for


providing facilities and resources for carrying out this study.
AP (kg Hþ EP (kg N
equi.)

0.02
0.01

Appendix A. Supplementary data

Supplementary data related to this article can be found at


(kg CO2 moles
equi.)

6.34
4.68
4.98

https://doi.org/10.1016/j.jclepro.2018.01.176.
equi.)

TTL 14.68
ATL 11.09
ABTL 11.93

References
GWP
Table 3

Bare, J.C., Gloria, T.P., 2006. Critical analysis of the mathematical relationships and
comprehensiveness of life cycle impact assessment approaches. Environ. Sci.
Technol. 40 (4), 1104e1113.
V.K. Rathore, P. Mondal / Journal of Cleaner Production 180 (2018) 716e727 727

Cavalett, O., Chagas, M.F., Seabra, J.E., Bonomi, A., 2013. Comparative LCA of ethanol District, Chhattisgarh, northeastern India. Appl. Water Sci. 1e10. https://doi.org/
versus gasoline in Brazil using different LCIA methods. Int. J. Life Cycle Assess. 18 10.1007/s13201-015-0355-2.
(3), 647e658. Rathore, V.K., Dohare, D.K., Mondal, P., 2016. Competitive adsorption between
Dong, Y.H., Ng, S.T., 2014. Comparing the midpoint and endpoint approaches based arsenic and fluoride from binary mixture on chemically treated laterite.
on ReCiPeda study of commercial buildings in Hong Kong. Int. J. Life Cycle J. Environ. Chem. Eng 4 (2), 2417e2430.
Assess. 19 (7), 1409e1423. Sarkar, M., Banerjee, A., Pramanick, P.P., Sarkar, A.R., 2006. Use of laterite for the
Jadhav, S.V., Bringas, E., Yadav, G.D., Rathod, V.K., Ortiz, I., Marathe, K.V., 2015. removal of fluoride from contaminated drinking water. J. Colloid Interface Sci.
Arsenic and fluoride contaminated groundwaters: a review of current tech- 302 (2), 432e441.
nologies for contaminants removal. J. Environ. Manag. 162, 306e325. Sivak, M., Schoettle, B., 2012. Eco-driving: strategic, tactical, and operational de-
Jagtap, S., Yenkie, M.K., Labhsetwar, N., Rayalu, S., 2012. Fluoride in drinking water cisions of the driver that influence vehicle fuel economy. Transport Pol. 22,
and defluoridation of water. Chem. Rev. 112 (4), 2454e2466. 96e99.
Kamble, S.P., Dixit, P., Rayalu, S.S., Labhsetwar, N.K., 2009. Defluoridation of drinking Trudewind, C.A., Schreiber, A., Haumann, D., 2014. Photocatalytic methanol and
water using chemically modified bentonite clay. Desalination 249 (2), 687e693. methane production using captured CO2 from coal-fired power plants. Part Iea
Maiti, A., Basu, J.K., De, S., 2010. Removal of arsenic from synthetic and natural Life Cycle Assessment. J. Clean. Prod. 70, 27e37.
groundwater using acid-activated laterite. Environ. Prog. Sustain. Energy 29 (4), Vinati, A., Mahanty, B., Behera, S.K., 2015. Clay and clay minerals for fluoride
457e470. removal from water: a state-of-the-art review. Appl. Clay Sci. 114, 340e348.
Maiti, A., Basu, J.K., De, S., 2011. Chemical treated laterite as promising fluoride World Health Organization, 2011. Guidelines for Drinking Water Quality, fourth ed.
adsorbent for aqueous system and kinetic modeling. Desalination 265 (1), World Health Organisation, Geneva.
28e36. Yami, T.L., Du, J., Brunson, L.R., Chamberlain, J.F., Sabatini, D.A., Butler, E.C., 2015. Life
Meenakshi, S., Sundaram, C.S., Sukumar, R., 2008. Enhanced fluoride sorption by cycle assessment of adsorbents for fluoride removal from drinking water in East
mechanochemically activated kaolinites. J. Hazard Mater. 153 (1), 164e172. Africa. Int. J. Life Cycle Assess. 20 (9), 1277e1286.
Montalembert, M.R., Gregersen, H.M., Oram, P., Spears, J., Gregersen, H.M., Oram, P., Zhou, J., Chang, V.W.C., Fane, A.G., 2011. Environmental life cycle assessment of
1992. Report of the United Nations Conference on Environment and Develop- reverse osmosis desalination: the influence of different life cycle impact
ment. United Nations Conference on Environment and Development, Río de assessment methods on the characterization results. Desalination 283,
Janeiro, Brasil. 227e236.
Monteiro, H., Freire, F., 2012. Life-cycle assessment of a house with alternative
exterior walls: comparison of three impact assessment methods. Energy Build.
47, 572e583. Weblinks
National Research Council, 2010. Technologies and Approaches to Reducing the Fuel
Consumption of Medium-and Heavy-duty Vehicles. National Academies Press. http://www.solidworks.com/sustainability/sustainable-design-guide/appendix-c-
Patel, K.S., Sahu, B.L., Dahariya, N.S., Bhatia, A., Patel, R.K., Matini, L., Sracek, O., the-hannover-principles.htm. (Accessed 9 April 2017).
Bhattacharya, P., 2015. Groundwater arsenic and fluoride in Rajnandgaon http://mnre.gov.in/mnre-2010/offgrid/biogas-2/. (Accessed 16 September 2017).