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Green Chemistry
PAPER
Cite this: Green Chem., 2013, 15, 3337
Received 8th July 2013,
Accepted 9th September 2013
DOI: 10.1039/c3gc41338a
www.rsc.org/greenchem
Life cycle assessment of surfactants: the case of an
alkyl polyglucoside used as a self emulsifier in
cosmetics
Jérôme Guilbot,*
a
Sébastien Kerverdo,
b
Alain Milius,
b
Rémi Escola
c
and
Fredrik Pomrehn
d
Purpose: Cetearyl glucoside and cetearyl alcohol are an alkyl polyglucoside composition (APG) widely
used in personal care as an efficient and versatile self-emulsifier. This ingredient is considered as green
thanks to its vegetable origin and to its manufacturing process complying with the 12 rules of Green
Chemistry. Beyond these general criteria, the rising environmental concern among consumers encourages
manufacturers to provide quantifiable measures highlighting the real impacts of a product on the
environment. In order to respond to this need, the aim of this work was to study, from an environmental
point of view, the contribution of the use of APG in a cosmetic cream (raw materials, glucosylation
process, formulation process, chemical inputs, energy, transport, waste management, end use, and recy-
cling) and to assess several potential improvements to decrease its global impacts. Materials and
methods: The methodology used was the life cycle assessment (LCA) according to the ISO 14-040 stan-
dard. Two approaches were chosen: (a) from the cultivation of vegetable raw materials to the final use
by consumers and recycling (from cradle to grave) and (b) from the cultivation of vegetable raw materials
to the production of APG (from cradle to gate). The two corresponding functional units were defined as
follows: (a) the preparation of a cosmetic oil in water emulsion having suitable stability and allowing the
face hydration of a consumer during 1 year and (b) the preparation of 1 t of packaged APG in a plant
located in the South of France. To comply with these two functional units, the life cycle was divided into
4 phases (gate to gate): the agricultural and transformation phase A, the chemical process phase B, the
formulation process phase C and finally the end use phase D. The life cycle inventory data collected were
based either on bibliographical sources or on direct industrial data. Seven impact categories were
selected for their relevance (ozone depletion, global warming, mineral resources, petrochemical
resources, eco-toxicity, acidification/eutrophication, and water consumption). For each significant
environmental impact, sensitivity assessments were carried out to identify potential improvements
regarding the two functional units. Results and discussion: The results show that the formulation process
phase C and the end use phase D are the main key issues of the cosmetic cream life cycle. Their respective
environmental contributions are between 15 and 51% and between 30 and 77% depending on the
impact category. Regarding the formulation step, the two most contributing parameters are the emul-
sion oil and the cream packaging. The impacts of oil are directly linked to the quantity involved (20% in
the cream) and also to the cultivation conditions of the plant from which the oil is extracted. A sensitivity
study on the nature of the packaging highlights that glass is much better than PET. As far as the end use
of the cream is concerned, the main impacting parameter is the purchasing by the consumer (between
33 and 77%). It was clearly proved that APG has relatively low impacts when it is formulated at 5% in a
a
SEPPIC, 127, Chemin de la Poudrerie, 81100 Castres, France.
E-mail: jerome.guilbot@airliquide.com
b
SEPPIC, 22, Terrasse Bellini –Paris La Défense, 92800 Puteaux, France.
E-mail: sebastien.kerverdo@airliquide.com, alain.milius@airliquide.com
c
ECO2 Initiative, 119-121, Rue Damrémond Bât. D, 75018 Paris, France.
E-mail: remi.escola@eco2initiative.com
d
LURGI, Lurgiallee 5, 60439 Frankfurt am Main, Germany.
E-mail: fredrik.pomrehn@airliquide.com
This journal is © The Royal Society of Chemistry 2013 Green Chem., 2013, 15, 3337–3354 | 3337
cosmetic cream (between 4 and 24%). Despite this low contribution, the environmental profile of APG
was examined and indicated the high impacts of the cetearyl alcohol (more than 80% by weight in APG).
For instance, the carbon footprint of APG directly depends on the cultivation mode of the palm trees
and, according to the land use change, it can vary between 1.9 and 49.8 t CO
2
eq. per t of APG. The
impacts directly due to the glucosylation process are between 2 and 12%, mainly coming from the trans-
port of raw materials and waste management. Conclusions: The present LCA gave a precise picture of the
role that APG plays in the environmental profile of a cosmetic emulsion. The next step may be to
compare its impacts with those of other surfactants that also respond to the first functional unit in order
to functional unit in order to confirm the green status of this kind of biosurfactant. Finally, improvements
in APG processing and use can also be brought about and all levels of the production chain are relevant:
raw material suppliers (fatty alcohol quality and transport), APG manufacturers (utilities consumption
follow-up, waste management and transport), finished cosmetic product formulators (packaging) and
final consumers (transport mode).
1 Introduction
Cosmetics are used to clean the skin and to improve its
appearance. In the past, basic materials such as animal and
vegetable oils or soaps were used. In the last few decades,
more elaborate materials have been developed to increase the
efficiency of cosmetics. Among these new materials, excipients
allow the formulation of several materials with a suitable
galenic (lotions, emulsions, ointments, sticks with pleasant
textures, etc.) and actives impart biological properties to the
formulations (slimming, moisturizing, tanning, whitening,
anti-ageing properties, etc.).
As far as excipients are concerned, one of the most impor-
tant kinds of molecules are surfactants
1a
which are character-
ized by an amphiphilic structure with both a polar head and a
lipophilic tail (Fig. 1).
In the literature,
1b
many studies introduce surfactants as
cationic, anionic, amphoteric (zwitterionic) or neutral com-
ponents depending on the charge borne by the polar head.
However, other classifications regarding their geometric struc-
ture do exist.
Surfactants are usually represented as in Fig. 1 with one
polar head and one hydrocarbon tail but it is also possible to
find surfactants with one hydrophilic head and two or three
lipophilic chains (bicatenary or tricatenary surfactants) or with
one hydrocarbon chain ending at each extremity with one
polar moiety (bolaform derivatives)
2,3
or with two monocatenary
amphiphilic entities linked together by a sort linker (Gemini
structures).
4
Surfactants (Fig. 2) can also be differentiated thanks to
their hydrophilic lipophilic balance (HLB). This physico-
chemical parameter is defined by assessing the size of the
polar head compared to the number and the length of the
hydrocarbon chain(s). The higher the HLB is, the bigger the size
of the polar head is and, as a consequence, the higher the
water solubility of the surfactant is. Obviously, although the
HLB concept is less and less used by formulators in the cos-
metic field, this parameter remains an interesting tool for the
design of new surfactants and for the prediction of their final
application properties.
Due to the presence of both a polar head and a lipophilic
tail, surfactants are able to lower the interfacial tensions of two
phases (liquid–liquid, liquid–gas and liquid–solid) inducing
original physico-chemical properties such as auto-organization
(Fig. 3).
5
The most famous one is the formation of micelles in
water which can help formulators to dissolve lipophilic raw
materials in aqueous solutions (fragrance or lipophilic surfac-
tants for example).
6
Surfactants can also stabilize mixtures of
oil and water to achieve oil in water (O/W) or water in oil (W/O)
emulsions.
7
A last example of surfactant applications is the
Fig. 1 Schematic representation of a surfactant.
Fig. 2 Various geometric structures of a surfactant.
Fig. 3 Auto-organization of surfactants (illustrations).
Paper Green Chemistry
3338 |Green Chem., 2013, 15, 3337–3354 This journal is © The Royal Society of Chemistry 2013
preparation of liposomes used for the encapsulation and the
vectorization of active principles to well defined targets (DNA
transfection for instance).
This ability for interfacial organization is consequently very
useful in many areas and especially in the cosmetic field,
where surfactants are generally involved in formulations as
foaming, emulsifying, thickening, solubilizing, wetting or tex-
turizing agents. Cationic derivatives are mostly used for their
conditioning properties in hair care whereas anionic
8
and
amphoteric derivatives are found in toiletry formulations
thanks to their detergent and foaming properties. As they are
not charged, the non-ionic surfactants are obviously mild to
the skin, explaining their uses in leave-on products.
The need for surfactants in cosmetics has not been dis-
cussed so far. Nevertheless, even if the major part of surfac-
tants still comes from synthetic raw materials, the increasing
sustainability trends of our society lead to the design of bio-
surfactants complying with the 12 Green Chemistry Principles
9
and inducing as little impact as possible on the environment.
10
Indeed, the petrochemical raw materials that play the role
of the polar head of the surfactant (ethylene or propylene
oxides, sulfates, sulfonates and quaternary ammoniums) can
now be substituted by hydrophilic vegetable raw materials
such as sugars (the saccharose, also called sucrose, coming
from sugar beet or sugar cane, the D-glucose coming from
wheat or corn starch or the D-xylose contained in hemicellu-
loses of wood)
11
or protein derivatives (hydrolysates, peptides
or amino acids).
As far as the lipophilic chains are concerned, the use of
fatty acids, alcohols or methyl esters coming from oleochemis-
try (coconut, castor, rapeseed, soybean, palm or palm kernel
oils for instance) is now largely preferred
12
to the use of
olefins obtained by paraffin cracking or by ethylene or propyl-
ene oligomerization, alkyl benzene chains or fatty alcohols
issued from the Ziegler or oxo processes.
13
The valorization of these natural raw materials allows the
design and the development of new surfactants that are more
or less renewable (the polar head and the lipophilic chain can
have a natural origin or only one part of the surfactant) and
characterized by good toxicological and ecological profiles
(skin irritation, biodegradability, bioaccumulation, daphnia/
fish/algae eco-toxicities). On the industrial scale,
1a
the most
representative bio-surfactants are (Fig. 4) alkyl polyglucosides
or APG (polar head based on D-glucose),
14
alkyl polyxylosides
or APX (polar head based on D-xylose),
15
sorbitan esters, sac-
charose esters,
16
glucamides and lipo amino acids or LAA.
17,18
Today, APGs are probably the best example of 100% bio-
based surfactants available on the market. They are produced
from renewable raw materials, oleochemical fatty alcohols and
crystallized D-glucose. The process to achieve them is quite
efficient (one step process). Their applications are huge as
their hydrocarbon chain length can vary from C-4 to C-8 (solu-
bilizing and detergent properties), from C-8 to C-12 (foaming
properties) and from C-14 to C-22 (emulsifying properties).
2 Goal and scope definition
2.1 Objectives
The first aim of this study was to analyze the part of the
environmental impacts induced by the use of APG in a cos-
metic cream. This global approach, “from cradle to grave”
(from cultivation of vegetable raw materials to final use by con-
sumers), allowed us to provide a full picture of the role played
by this kind of excipient in the sustainability of a cosmetic
cream.
19
This picture will be a very interesting tool to after-
wards compare with other kinds of surfactants ( from petro-
chemistry for instance). The second goal was focused on the
production of APG with a “from cradle to gate”approach.
Aside from the results of the first approach, this part of the
work provided some information to identify which improve-
ments could be brought about to reduce the environmental
impacts of the APG process on the industrial scale.
In this context, the APG considered here is an O/W emulsi-
fier used in a personal care leave-on product, a moisturizing
cream.
20
The raw materials to manufacture this APG are
cetearyl alcohol and crystallized D-glucose coming respectively
from palm kernel oil and wheat starch. It is composed of 80%
of C-16/18 alcohol and 20% of C-16/18 glucoside (INCI name:
cetearyl alcohol and cetearyl glucoside). Hereafter in this
article, APG refers to this aforementioned mixture of fatty
alcohol and glucoside.
2.2 Functional units
The selection of the functional unit is a significant step as it
influences both the results and their analysis. Its choice
thereby depends on the goal(s) defined for the study. Regard-
ing the cradle to grave approach, the first functional unit
(FU 1) is the preparation of a cosmetic O/W emulsion having
suitable stability and allowing the face hydration of a consumer
for 1 year. To reach this functionality, the use of 584.0 g of
a moisturizing cream containing 29.2 g of APG is necessary.
The precise composition of the emulsion, the stability
Fig. 4 Chemical structures of bio-surfactants produced on the industrial scale.
Green Chemistry Paper
This journal is © The Royal Society of Chemistry 2013 Green Chem., 2013, 15, 3337–3354 | 3339
requirements, the daily application conditions and the
expected moisturizing effects are detailed in Sections 3.7 and
3.8. As far as the cradle to gate approach is concerned, the
second functional unit (FU 2) is the production of 1 t of pack-
aged APG in a plant located in the South of France.
2.3 Description of the system selected in this study
The system process was divided into 4 main phases, the first
one being subdivided into 4 subphases:
•Agricultural and transformation phases A:
○Production of the lipophilic raw material from palm
tree:
–Phase A-1: Palm cultivation →fresh fruit bunches
(FFB).
–Phase A-2: Oil extraction and refining →refined palm
kernel oil (RPKO).
–Phase A-3: Transesterification of RPKO and hydrogen-
ation →cetearyl alcohol.
○Production of the hydrophilic raw material from wheat:
–Phase A-4: Wheat cultivation →crystallized D-glucose.
•Chemical process phase B:
○Linkage of these two raw materials according to
Fischer’s glucosylation and leading to the amphiphilic
structure →APG manufacture.
•Formulation process phase C:
○Preparation of a moisturizing O/W emulsion →cos-
metic cream fabrication.
•End life phase D:
○Use of the final cosmetic cream by a consumer and
recycling.
The localization of these different phases were defined pre-
cisely (Fig. 5): Malaysia or Indonesia for phases A-1 and A-2,
Germany for phase A-3, the North of France for phase A-4, the
South of France (Castres) for phases B and C and, finally, Paris
area for phase D. The transport modes and the distances taken
into account were detailed in the life cycle inventories.
The system boundaries are summarized in Fig. 6. The
weights mentioned correspond to FU 1.
The FU 2 system boundaries include phases A and B. The
weights have to be multiplied by 34.246 × 10
3
.
3 Life cycle inventory (LCI)
3.1 Data quality and simplifications
High quality data are essential to make a reliable evaluation in
a LCA analysis and the bibliographical work is very time con-
suming. The LCI data for phases A-1, A-2, A-4 and D being
based on available literature, all the references mentioned
throughout the article are listed at the end in the last section
of this paper.
The LCI data regarding phase A-3 are issued from collabor-
ation with the Lurgi Company which is specialized in the
scale-up of industrial processes and has significant experience
in transesterification and hydrogenation reactions on the plant
scale. In the present study, the impacts due to the hydrogen-
ation catalyst were not taken into account.
The LCI data for phase B were obtained by on-site measure-
ments at Castres by means of an industrial control system,
supervisory control and data acquisition (follow-up of water,
electricity, gas and nitrogen consumption, solid waste weight-
ing, waste water control with chemical oxygen demand (COD)
measurements, etc.).
The LCI data for phase C are based on the knowledge of the
general practices implemented by well known formulators in
the cosmetic field.
Information regarding the manufacture of primary raw
materials such as natural gas, chemicals,
21
electricity, fuel,
packaging, etc., was obtained from databases (mainly the Eco-
invent database) and also from the literature.
Finally, the different wastes for recycling from phases
A-1 and A-2 were not taken into account in this study and 3
Fig. 5 World localization of the different phases of the studied system.
Paper Green Chemistry
3340 |Green Chem., 2013, 15, 3337–3354 This journal is © The Royal Society of Chemistry 2013
co-products from wheat cultivation (germ, bran and gluten)
were not allocated.
3.2 Agricultural and transformation phase A-1: production of
FFB
The cetearyl fatty alcohol used for the production of APG is
derived from the oleochemistry field, and more particularly
from the palm field.
Palm oil is the most widely traded oil in the vegetable oil
market.
22–29
When we talk about the palm industry, it is
important to distinguish two kinds of oils: refined palm oil
(RPO) and refined palm kernel oil (RPKO). The first one,
obtained from the mesocarp of the fruit, is the most important
in terms of tonnage (about 41 millions of tons mainly dedi-
cated to food applications). It mainly contains triglycerides
with palmitic and oleic chains. By contrast, the second one
comes from the kernel contained in nuts which can be con-
sidered as a byproduct of palm oil mills.
30,31
This PKO is
characterized by triglycerides mainly composed of lauric
chains (Table 1). For this reason and on the basis of the
coconut oil, it is also called “lauric oil”which is very useful for
the production of foaming surfactants.
Fig. 6 System boundaries of the LCA study.
Green Chemistry Paper
This journal is © The Royal Society of Chemistry 2013 Green Chem., 2013, 15, 3337–3354 | 3341
Surprisingly, despite its high levels of palmitic and oleic
chains, RPO is not used to achieve cetearyl alcohol while
RPKO is.
The productivity of an oil palm plantation depends on
many factors (Table 2) such as the palm variety, cultivation con-
ditions, harvesting modes, soil nature, the use of fertilizers,
herbicides or pesticides, etc.
32,35–37
In this study, it was con-
sidered that the palms of the Elaeis guineensis variety are
planted in Malaysia or Indonesia on undegraded areas. The
type of soil was chosen according to the mean repartition
defined in Malaysia:
33,34
61% of primary forest, 31% of intact
meadow and 8% of non-degraded peat land. The most
common fertilizers applied in the oil palm plantations are
muriate of potash (KCl), ammonium sulphate ((NH
4
)
2
SO
4
),
kieserite (MgSO
4
·H
2
O) and rock phosphate (Ca
5
(PO
4
)
3
F and
Ca
5
(PO
4
)
3
OH).
38
In this study, it was considered that all the
crop inputs (fertilizers, herbicides, insecticides, fungicides
and rodenticides) are imported and brought to plantations by
transoceanic freight ship (5000 km). The water need of oil
palms is about 200–250 l of water per tree per day and 300–350 l
during the hot periods.
39
The main part of this water is
brought by rains and atmospheric humidity (tropical climate)
and only 0.7 l per tree per day was considered to come from
irrigation.
3.3 Agricultural and transformation phase A-2: production of
RPKO
The FFB, delivered to the palm oil mill (50 km by lorry), are
received at the FFB hoppers and transferred into sterilization
cages. This sterilization step loosens the individual fruits from
the bunch and also deactivates the enzyme which causes the
breakdown of the oil into free fatty acids (FFA). The sterilized
FFB are sent to a stripper where the fruits are separated from
the bunch. The bunches now free of attached fruits, known as
empty fruit bunches (EFB), are normally sent back to the plan-
tations for mulching as a fertilizer substitute. The fruits from
the stripper are then sent to a digester where they are con-
verted into a homogeneous oily mash by means of a mechan-
ical stirring process. The digested mash is then pressed using
a screw press to remove the major portion of crude palm oil
(CPO). After clarification, centrifugation and vacuum drying,
CPO is sent to refineries to lead to RPO. The nuts with the
pressed mesocarp fibres are separated at the fiber cyclone and
then cracked to produce kernels and shells. The kernels (∼5%
in FFB)
40
are shipped to kernel crushing plants to be processed
into crude palm kernel oil (CPKO), while the shells and
pressed mesocarp fibres are used as boiler fuel.
31,41
The main solid wastes from the milling processes are EFB,
pressed mesocarp fibres, shells and boiler ashes, while the
liquid wastes are palm oil mill effluents (POME) composed of
sterilization condensates and clarification waters.
35,42
The
gaseous emissions are from the boiler stacks and biogases
from the treatment ponds (mainly methane formed by anaero-
bic biodegradation of POME).
The next step consists of refining CPKO by a chemical
method.
43
CPKO is firstly degummed with phosphoric or citric
acid followed by an adsorptive cleansing in the presence of
bleaching earth. Then FFA and other undesirable volatiles
from the oil that it contains are stripped under vacuum in the
de-acidification and deodorization steps allowing the access
of RPKO.
Energy for CPKO processing is met by electricity from the
grid and fossil fueled boilers which produce steam from
municipal water. Steam is used to heat the oil during degum-
ming and earth bleaching, while live steam is injected into the
deodorizers during stripping of FFA and other undesirable
volatiles from the oil in the de-acidification and deodorization
steps. Liquid wastes from the refinery include waste water and
free fatty acid distillate (FFAD).
3.4 Agricultural and transformation phase A-3: production of
cetearyl alcohol
Before the transesterification and hydrogenation processes,
13
RPKO is transported from Malaysia or Indonesia to Marseille
by transoceanic freight ship (12 000 km) and then to Germany
by train (1100 km). A continuous transesterification of RPKO
Table 1 Triglyceride compositions of PO, PKO and coconut oil
R + 1 Palm oil Palm kernel oil Coconut oil
Caprylic C-8 : 0 / 3–10 6–9
Capric C-10 : 0 / 3–14 6–10
Lauric C-12 : 0 / 37–52 44–51
Myristic C-14 : 0 0–57–17 13–18
Palmitic C-16 : 0 32–47 2–98–10
Stearic C-18 : 0 2–81–31–3
Oleic C-18 : 1 40–52 11–23 5–8
Linoleic C-18 : 2 5–11 1–30–3
Table 2 Common cultivation conditions of palm trees in Malaysia or Indonesia
Palm cultivation conditions of this study
Tree density 142 palm trees ha
−1
FFB yield 19.4 t ha
−1
year
−1 24,36,37
RPO yield 3.71 t ha
−1
year
−1
RPKO yield 0.46 t ha
−1
year
−1
Biogenic carbon 7.7 t ha
−1
year
−1
N fertilizer 105 kg ha
−1
year
−1
P fertilizer 31 kg ha
−1
year
−1
K fertilizer 170 kg ha
−1
year
−1
Mg fertilizer 21 kg ha
−1
year
−1
S fertilizer 16 kg ha
−1
year
−1
Herbicides 2.4 kg ha
−1
year
−1
Insecticides 0.31 kg ha
−1
year
−1
Fungicides 13 g ha
−1
year
−1
Rodenticides 0.21 g ha
−1
year
−1
Irrigation water 0.7 l tree
−1
day
−1
Paper Green Chemistry
3342 |Green Chem., 2013, 15, 3337–3354 This journal is © The Royal Society of Chemistry 2013
with methanol in the presence of sodium hydroxide is selected
for this work (called the “methyl ester route”). This process is
the most economical process as it takes place at relatively low
operating temperature and pressure, has a high conversion of
more than 98% and involves direct conversion to methyl esters
in a relatively short reaction time. Nevertheless, the influence
of an alternative process using no methanol, the “wax ester
route”, on the environmental impact of the cetearyl alcohol
will be discussed in Section 5.4. After removing glycerin and
purification by rectification, the recovered methanol is recycled
and the C-8/14 methyl ester is split from the C-16/18 methyl
ester by distillation separation.
The last step is the continuous hydrogenation of the
C-16/18 methyl ester in the presence of hydrogen and a cata-
lyst.
44
This chemical transformation is generally carried out
under high temperature (250–300 °C) and high hydrogen
pressure (25–35 MPa) in a fixed bed trickle flow process. The
catalyst used consists mainly of copper–chromite (Cu–Cr)
oxide as a basic structure (not taken into account in this
study). The targeted C-16/18 alcohol is finally distilled to reach
a purity of more than 95%.
3.5 Agricultural and transformation phase A-4: production of
crystallized D-glucose
The crystallized D-glucose used for the manufacture of APG is
derived from wheat, and particularly from wheat starch.
The starches are carbohydrate polymers which form the
energy reserve in plants. The main sources of commercial
starches in Europe are maize, wheat and potatoes with smaller
quantities being derived from rice, barley and tapioca.
45
Chemically, starch consists of repeated sequences of gluco-
pyranosyl units. The number of repeat units varies from around
250 to 1000 and are linked in two ways (Fig. 7): a linear struc-
ture with only α-1,4 glycosidic bonds (amylose) and a branched
form with α-1,4 and α-1,6 glycosidic bonds (amylopectin).
Most commercial starches contain 20–30% amylose and
70–80% amylopectin.
46
The wheat cultivation (Table 3)
47–49
begins by sowing seeds
in autumn and finishes by harvesting in July or August. At this
stage, the main solid co-product is the straw which is valued in
mulching or animal feed. During the growth of the plant, ferti-
lizers, herbicides, pesticides and growing substances are used,
especially during winter months. These crop inputs are
brought to the plantation by lorry (500 km). The water need for
wheat growing is about 1000–1500 l of water per kg of wheat
(7200–10 800 m
3
ha
−1
year
−1
).
38,47
Depending on the country
and on the area, this water can come from either rain or irriga-
tion. In this study, a wheat plantation located in the North of
France was considered and the water irrigation was estimated
at around 317 m
3
ha
−1
year
−1
. Unlike the palm cultivation, the
mechanization is more important for the wheat cultivation
(tractors, trailed implements, combine harvesters, transport
from crops to the mill by lorry (100 km), etc.). The ADEME esti-
mates, in its 2003 Ecobilan,
50
that about 107 liters of fuel are
needed to cultivate 1 hectare of wheat.
After harvesting, the wheat grains are washed and ground
into flour. The wheat bran and optionally the wheat germs are
separated from flour by sifting. The flour is then mixed with
water to form a slurry from which the starch and the gluten
are separated. The resulting starch milk is totally hydrolyzed
either under chemical conditions or under enzymatic con-
ditions or both. The final work-up involves demineralization,
discoloration, concentration by evaporation and crystallization
to obtain anhydrous D-glucose.
51
3.6 Chemical process phase B: production of APG
The glucosylations according to Fischer’s conditions
52,53
are
acidic catalyzed balanced reactions involving crystallized
D-glucose dispersed in a molar excess of hydrocarbon alcohol.
They are generally carried out at about 105 °C for 4 to
6 hours.
1a,b
As described in Fig. 8, the chemical mechanism
comprises several well identified steps: activation of the
anomeric hydroxyl function, removal of the water, formation
of the “oxycarbenium ion”and nucleophilic attack of the
fatty alcohol either from the bottom or from the top leading
respectively to the anomers αand β.
At the end of glycosylation, the reaction medium is neutral-
ized with sodium hydroxide and un-reacted glucose is removed
by decantation and centrifugation. The last step is the shaping
Fig. 7 Chemical structure of starch.
Table 3 Common cultivation conditions of wheat in the North of France
Wheat cultivation conditions of this study
Grain yield 7.2 t ha
−1
year
−1a
Biogenic carbon ∼0tha
−1
year
−1
N fertilizer 184 kg ha
−1
year
−1
P
2
O
5
fertilizer 46 kg ha
−1
year
−1
K
2
O fertilizer 76 kg ha
−1
year
−1
Herbicides 0.9 kg ha
−1
year
−1
Insecticides 0.2 kg ha
−1
year
−1
Fungicides 0.3 kg ha
−1
year
−1
Growing substances 1.5 kg ha
−1
year
−1
Irrigation water 317 m
3
ha
−1
year
−1
a
http://lafranceagricole.fr.
Fig. 8 Mechanism of Fisher’s glucosylation.
Green Chemistry Paper
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of APG by pearlizing. Finally, APG is packaged in plastic bags
stored in 25 kg rigid cardboard.
Batches of 10.9 t of APG in a 25 m
3
vessel are supposed. For
that, it is necessary to involve 10.5 t of cetearyl alcohol and
1.4 t of crystallized D-glucose. The supplying of the raw
materials is done by lorry (∼1200 km for the cetearyl alcohol
coming from Germany to Castres and ∼900 km for the glucose
coming from the North of France to Castres). As the APG is
solid at room temperature (melting point ∼65 °C), the entire
process is carried out by heating in order to maintain the
product as a liquid. The heat is provided by steam produced by
a gas boiler (104 kg of steam per t of APG). Electricity is also
consumed, especially for pumps, stirring motors, the decanta-
tion device, etc., and this energetic input was estimated at
313 kWh per t of APG.
Water is needed during the entire process for the liquid
ring pumps, the flue gas scrubber of the decantation device,
the washing operations, etc. Its consumption is fixed at 1.4 m
3
per t of APG. The water necessary for cooling during the pear-
lizing operation is not taken into account because the device
works in a closed circuit system. Nitrogen is also necessary
(2.2 m
3
per t of APG) because, during the entire process, the
reaction medium is always maintained under a nitrogen
atmosphere in order to prevent coloration with oxygen from
the air.
The main outputs are glucose muds from the decan-
tation and centrifugation steps (∼76 kg per t of APG). They
are incinerated in a specific treatment plant at about
160 km from the production site. There are also liquid
aqueous effluents from the process and from the washing
operations (∼14 l per t of APG containing 3000 mg per l
of COD). All these effluents are transferred to a wastewater
treatment plant.
3.7 Formulation process phase C: production of a cosmetic
cream
Due to the huge diversity of cosmetic creams available in the
market, the type of formulation was not very easy to choose for
this study. Nevertheless, it seemed that an O/W moisturizing
emulsion was a suitable and representative model which
allowed the clear definition of FU 1: preparation of a cosmetic
O/W emulsion having good stability and allowing the face
hydration of a consumer during 1 year. Its composition is as
follows: 75% of water, 20% of an oil phase and 5% of APG.
Regarding the oil phase, it was considered that its environ-
mental profile was very similar to the RPKO one.
The emulsification process is quite simple and consists of
mixing the three components for about 2 h at 70 °C and under
vigorous agitation. After supplying the oil at Castres
(∼1000 km by lorry), this phase is carried out in a 2 t vessel.
The emulsion is stable if there is no phase separation after
3 months at room temperature and after 1 month at 45 °C.
The energy consumption for heating and stirring is estimated
at 85 kg of steam per t of cream (the same gas boiler as for the
glucosylation step) and at 6 kWh of electricity per t of cream.
The outputs are mud (70 kg per t of cream) and liquid waste-
water (10 l per t of cream with 3000 mg per l of COD).
Finally, the final cream is bottled in a 30 g jar made of 7 g
of PET and equipped with a tight fitting lid made of 5 g of alu-
minium. Each jar is packaged in a small cardboard box (5 × 5
× 5 cm) wrapped in a very thin PEHD film (100 µm). Conse-
quently, to reach FU 1 (584.0 g of cream), 19.5 jars are needed.
3.8 End life phase D: use of the cream during 1 year
The final use of the cream is its application on the skin of a
consumer. So, the cream does not have direct environmental
impacts as it penetrates through the skin. However, indirect
impacts have to be taken into account such as the supplying of
the cream to the store, the transport to buy it and the recycling
of the 19.5 jars.
For the supplying, 1000 km by a >32 t lorry and 100 km by a
3.5–7.5 t lorry were considered. As far as the purchasing act is
concerned, the choice of the distance and the transport mode
was based on studies carried out in 2004 by the Direction
Régionale de l’Equipement d’Ile de France.
54
Assuming that
the consumer bought 2 jars at each shopping trip, the global
distance of 100 km was taken into account (10 back to back
10 km distances) with the following modes: 60 km by an average
vehicle emitting 0.18 kg CO
2
eq. km
−1
and 40 km by a bus
emitting 0.10 kg CO
2
eq. km
−1
. As the consumer did not buy
only cosmetic jars, an allocation of about 15% was considered.
The recycling of the packaging was done by landfill (64% of
the package) and by incineration (36% of the package).
To check the efficiency of the cream, the moisturizing pro-
perties were assessed according to in vivo tests. The cream
was applied to the forearm of volunteers with normal skin
(2 × 0.8 g day
−1
according to the recommendations of the
Scientific Committee on Cosmetics products and Non Food
Products intended for consumers (SCCNFP 2006))
55
and the
hydration was measured at 22–24 °C thanks to a Corneometer
CM 820 (Courage & Khazaka). The cream was considered
efficient if the skin hydration had increased by more than 25%
90 min after the application.
3.9 Allocation procedure
In this study, not only APG and cosmetic cream are produced
(main products) but RPO, glycerin, C-8/14 methyl ester and
wheat straw are also obtained. Among the different possible
procedures, allocations based on weight were selected for RPO,
glycerin and C-8/14 methyl ester according to the following
ratios: 79% of RPO versus 21% of kernels at the palm oil mill
(first extraction) and 13% of glycerin versus 63% of
C-8/14 methyl ester versus 24% of C-16/18 methyl ester during
the transesterification and distillation steps. For the wheat
straw, an economical allocation was taken into account: 92%
of wheat grains versus 8% of wheat straw.
56
No allocation was
taken into account for germs, bran and gluten coming from
wheat.
Paper Green Chemistry
3344 |Green Chem., 2013, 15, 3337–3354 This journal is © The Royal Society of Chemistry 2013
Table 4 Global average inventory: general inputs and outputs for the use of 584.0 g of moisturizing cosmetic cream (FU 1)
Phases A-1 A-2 A-3 A-4 B C D
Crop inputs
Land
occupation
1.71 m
2
of
primary forest
0.008 m
2
0.87 m
2
of
intact meadow
0.22 m
2
of
intact peat land
Biogenic
carbon
2.2 kg CO
2
eq. 0 kg CO
2
eq.
Fertilizers 29.4 g of N 140.6 mg of N
8.7 g of P 36.0 mg of P, O
47.6 g of K 56.2 mg of K, O
5.9 g of Mg
4.5 g of S
Herbicides 672.0 mg 0.72 mg
Insecticides 86.8 mg 0.16 mg
Fungicides 3.7 mg 0.24 mg
Rodenticides 58.8 μg
Growth
substances
1.2 mg
Water 9.8 l 0.3 l
Process inputs
Mineral acid 89.5 mg of
H
3
PO
4
(refining)
2.1 mg of HCl
Mineral base 0.9 mg of NaOH 15.4 mg of NaOH
(neutralization)
18.1 mg
of MeO
−
Na
+
Bleaching
agent
1.3 g of
bleaching
earth
Catalyst Mineral acid
(hydrolysis)
57.9 mg
(glucosylation)
MeOH 50.0 g (17.2 g
recycled)
Hydrogen 7.8 × 10
−3
Nm
3
Nitrogen 1.0 × 10
−4
Nm
3
0.1 × 10
−3
Nm
3
0.03 N m
3
Tap water 9.3 l 11.8 l 0.04 l (washing,
pumps, scrubber)
0.48 l 21.1 l
Oil 116.8 g
Packaging
materials
73.1 g of rigid
cardboard
136.5 g of PET
27.5 g of plastic
bag
97.5 g of
aluminium
PEHD film
cardboard
Energy inputs
Electricity 0.41 × 10
−5
kwh 0.14 kWh 0.006 kWh 0.005 kWh 0.009 kWh
(pumps, stirring
motors, etc.)
0.408 kWh
Fuel 0.17 kWh
(tractor,
crusher)
0.04 kWh 0.02 kWh 0.9 × 10
−6
kWh
(tractors,
harvesters)
Steam 7.9 g 35.0 g 3.0 g (gas boiler) 49.6 g (gas
boiler)
Transport inputs
5000 km (crop
inputs by
transoceanic
freight ship)
50 km (FFB
to mill by
lorry)
12 000 km (RPKO
from Malaysia to
Marseille by
transoceanic
freight ship)
500 km (crop
inputs by lorry)
1200 km (fatty
alcohol from
Germany to
Castres by lorry)
1000 km (oil by
lorry)
1000 km (store
supplying by
>32 t lorry)
1100 km (RPKO
from Marseille to
Germany by
train)
100 km (wheat
grain to mill by
lorry)
900 km (glucose
from north of
France to Castres
by lorry)
160 km (mud
from Castres to
incineration
plant by lorry)
100 km (store
supplying by
3.5–7.5 t lorry)
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3.10 Inventory analysis for FU 1 and FU 2
The LCI of each phase of the system is summarized in Table 4.
The inputs and outputs correspond to FU 1 based on the
production and the use of 584.0 g of moisturizing
cream. Regarding FU 2 aimed at the production of 1 t
of packaged APG, the figures have to be multiplied by
34.246 × 10
3
.
4 Life cycle assessments (LCA) for the
cosmetic cream (FU 1) and APG (FU 2)
4.1 Selection of environmental impact indicators
In this study, seven impact indicators were chosen.
Ozone depletion (OD). High in the Earth’s stratosphere,
chemical processes maintain a balanced concentration of
Table 4 (Contd.)
Phases A-1 A-2 A-3 A-4 B C D
160 km (glucose
mud from
Castres to
incineration
plant by lorry)
9.2 km
(purchasing by
car)
6.1 km
(purchasing by
bus)
Product outputs
5423.0 g of FFB 127.9 g of
RPKO
27.8 g of C-16/18
alcohol
3.7 g of glucose 29.2 g of APG 584.0 g of cream
Co-products outputs
Allocated in
this study
1.0 kg of
RPO (food
oil)
16.7 g of glycerin Straw
(mulching,
animal feed)
80.7 g of C-8/
14 methyl ester
Not allocated
in this study
Germ
Bran
Gluten (food,
animal feed)
Waste to recycling
Felled old
trunks
(nutrient
source)
0.7 kg of
fibres (boiler
fuel)
87.4 g of PET
and 62.4 g of
aluminium (by
landfill)
Pruned fronds
(mulching)
1.3 kg of
EFB
(mulching,
fertilizer)
49.1 g of PET
and 35.1 g of
aluminium (by
incineration)
0.4 kg of
shells (boiler
fuel)
Boiler ashes
Waste to treatment
3647 g of
POME
Waste water 1.9 g of glucose
mud
(incineration)
40.1 g of mud
(incineration)
Waste water
25.1 g of
proteins
0.4 g of reaction
water
5.8 ml of waste
water
Waste water 0.41 ml of waste
water
FFAD
Air emissions
4393 g eq. of
CO
2
from land
use change
GHG from
POME
Water emissions
Cf LCI Schmidt
J.H. (2007) part
3, p. 114
1.23 mg of COD 17.4 mg of COD
Paper Green Chemistry
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ozone. This ozone layer protects the Earth by absorbing much
of the harmful ultraviolet radiation from the Sun. If a gas car-
rying bromine or chlorine atoms can stay in the atmosphere
long enough to reach the stratosphere, the ozone balance may
be threatened as free bromine and chlorine can accelerate the
breakdown of ozone. The Ozone Depletion indicator is
expressed in kg CFC-11 eq.
Global warming (GW) or the greenhouse effect (GHE). The
Earth’s climate is driven by the balance of energy or heat
added by the Sun and lost by the Earth. The primary energy
is lost through heat radiation, much like the heat you
feel coming from a stove. Several gases in the atmosphere,
called greenhouse gases (GHG), can reflect some of this heat
back to the Earth. This effectively warms the Earth and may
alter the climate over time as these gases increase in con-
centration. The Global Warming indicator is expressed in kg
CO
2
eq.
Mineral resources (MR). Taking into account their increas-
ing scarcity, surplus energy is needed to extract mineral raw
materials. The Mineral Resources indicator is expressed in
megajoules (MJ).
Petrochemical resources (PR). The same concept as for
mineral resources. The Petrochemical Resources indicator is
expressed in megajoules (MJ).
Eco-toxicity (EC). Quality ecosystem changes (fauna and
flora) due to emissions in water, air and soil. The Eco-toxicity
indicator is expressed in potentially affected fraction (PAF) per
m
2
per year.
Acidification/eutrophication (AC/EU). Natural rain is slightly
acidic due to the presence of various acids in the air that are
washed out by rain. However, a number of man-made emis-
sions are either acidic or they are converted to acid by pro-
cesses in the air. Examples of such emissions are sulfur
dioxide (which becomes sulfuric acid) and nitrogen oxide
(which becomes nitric acid). As a result, the acidity of rain can
be substantially increased. In a number of areas (such as large
areas of Sweden), the soil and water have a limited capacity to
neutralize these added acids. If water becomes too acidic, an
increasing number of aquatic species are harmed. If the soil
becomes too acidic, the ability of plants to grow and thrive is
harmed. The acidification indicator is expressed in potentially
disappeared fraction (PDF) per m
2
per year.
Aquatic plants and algae gradually fill in freshwater lakes
and estuaries over time in a natural process called eutrophica-
tion. This process is controlled by low concentrations of
certain nutrients (like phosphate and nitrogen) that the
plants and algae require to grow. Usually, phosphorus is the
limiting nutrient in freshwater and nitrogen in estuaries
and salt water. However, when humans release nutrients
like phosphate (agriculture ∼50%, human metabolism ∼20%,
industry ∼10%, detergents ∼10% and natural erosion ∼10%),
the process of eutrophication is accelerated. In the worst-
case scenario, the excess growth of plants and algae can
smother other organisms when they die and begin to decay.
The eutrophication indictor is also expressed in PDF per m
2
per year.
Water consumption (WC). Quantity of water needed to
perform the phase of the LCA. The water consumption indi-
cator is expressed in m
3
.
For each phase, the SimaPro version 7.3.2 was used for the
achievement of environmental impact assessment. The figures
listed hereafter were obtained thanks to different methods and
databases: Impact 2000+, Eco Indicator 1999 (MR and PR),
IPCC 2007 GWP 100 a (GW) and Eco-invent (WC).
4.2 Characterization results from cradle to grave (FU 1)
The allocated results to the global life cycle of the moisturizing
cream are shown in Table 5. The skin hydration of a consumer
during 1 year has a carbon footprint equal to 5.6 kg CO
2
eq.
and represents a consumption of water equal to 79.3 l. For
comparison purposes, these figures can be expressed by mean
impacts emitted by an average European person. The GW of
the moisturizing cream is equivalent to 0.2 day of an average
European person and the WC is equivalent to 0.6 day.
A breakdown of the contribution of the different phases
involved in the system is depicted in Fig. 9 in order to identify
the most contributing phase to the selected environmental
impact categories. Phases C and D which correspond
respectively to the formulation of the cream and to its use by a
consumer are the hot spots among all the impact categories
under assessment. Their contributions to the environmental
profile are 32% OD, 30% GW, 40% MR, 26% PR, 31% EC,
15% AC/EU and 51% WC for phase C and 63% OD, 47%
GW, 54% MR, 70% PR, 62% EC, 77% AC/EU and 30% WC for
phase D.
These results are in agreement with studies available in the
literature. The first one was on the environmental labeling of
shampoos, performed in 2009 by the Fédération des Entre-
prises de la BEAuté (FEBEA).
57
Its aim was to identify the
origins of the most important environmental impacts due to
the use of a cosmetic product. They concluded that between 85
and 95% of the impacts came from the use itself of the
shampoo. The second one, published in 2003 by Procter &
Gamble, dealt with the role of surfactants in the environ-
mental profile of detergents. The results showed that the use
conditions of a detergent were more important than the
nature of the surfactant. For instance, colder wash tempera-
tures during the consumer use phase would result in positive
contributions such as energy savings, reduced air emissions,
conservation of petroleum stocks and reduced waste.
19
Table 5 Impact assessment results associated with the use of 584.0 g of moist-
urizing cream (skin hydration during 1 year)
Impact categories Unit Value
Ozone depletion (OD) kg CFC-11 eq. 6.7 × 10
−7
Global warming (GW) kg CO
2
eq. 5.6
Mineral resources (MR) MJ 0.1220
Petrochemical resources (PR) MJ 8.14
Eco-toxicity (EC) PAF m
−2
year
−1
1.150
Acidification/eutrophication (AC/EU) PDF m
−2
year
−1
0.1040
Water consumption (WC) m
3
0.0793
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From a cradle to grave perspective, it is quite clear that the
impacts induced by the glucosylation process (phase B) as well
as by the production of lipophilic and hydrophilic raw
materials to achieve APG (phases A-1, A-2, A-3 and A-4) are
limited and between 4 and 24%.
4.2.1 Impact details of the formulation process phase
C. To understand why phase C is predominant during the
global life cycle of the cream, it was split according to its
inputs and outputs (Fig. 10). The majority of the impacts pro-
duced during the formulation process come from the oil of the
emulsion and the materials of the cream packaging (PET jars,
aluminium lid, cardboard and PEHD film). The oil represents
12% OD, 53% GW, 9% MR, 9% PR, 15% EC, 29% AC/EU and
24% WC. As already mentioned in the previous section, the
environmental profile of the oil was considered, in this study,
the same as RPKO used for the manufacture of the cetearyl
alcohol. As a consequence, the impacts of the oil are linked to
the cultivation of palm trees and the oil extraction processes
whose impacts are explained in more detail in Section 4.3.1
describing the FU 2 results.
The packaging represents 74% OD, 27% GW, 86% MR, 76%
PR, 75% EC, 49% AC/EU and 63% WC. These significant con-
tributions are due to the nature of the chosen materials almost
exclusively from the petrochemical field. The sensitivity of this
parameter is assessed in Section 5.1. To highlight the impor-
tance of packaging in the cosmetic field, it is interesting to
mention the software called “Winted”and recently developed
by Chanel in collaboration with EVEA. The objective of this
tool is to help formulators develop more eco-designed pack-
aging in order to improve the environmental profile of their
cosmetic products.
58
Finally, APG’s impacts are moderate, between 3% and 15%,
whereas waste’s ones are between 1 and 7%.
4.2.2 Impact details of the end life phase D. In the same
way as before, the relative contributions of the use and the end
life of the cream to selected impact categories are shown in
Fig. 11. Two main stages prevail: the cream itself mainly
because of the oil and the packaging as already concluded and
its purchasing.
Indeed, the purchasing is responsible for 63% OD, 53%
GW, 55% MR, 69% PR, 60% EC, 77% AC/EU and 33% WC.
These results are a consequence of the transport mode
selected for this work (9.2 km by car and 6.1 km by bus in
Paris) which corresponds to an average.
54
Of course, they can
be reduced if lower distances are taken into account and/or if
walking, cycling or public transport is preferred. In addition,
the purchasing impacts are higher than the supplying ones
because of the quantities of cream transported for each route.
4.3 Characterization results from cradle to gate (FU 2)
The allocated results to the production of 1 t of packaged APG
are summarized in Table 6. For instance, the corresponding
carbon footprint is 12.3 t CO
2
eq. per t of APG and the water
consumption is about 190 m
3
per t of APG. These figures are
equivalent to 481 days of an average European person for GW
and to 1391 days for WC.
A breakdown of the contribution of the different phases
involved in this FU 2 (A-3, A-4 and B) is depicted in Fig. 12 in
order to identify the most contributing phase to the selected
environmental impact categories.
It appears that the most contributing phase is the pro-
duction of the cetearyl alcohol far ahead of the production of
the glucose and the glucosylation process. Its contributions
are 82% OD, 97% GW, 85% MR, 82% PR, 77% EC, 85% AC/EU
and 81% WC. Regarding the crystallized glucose production,
its impacts are relatively limited and between 1 and 16%.
50
Despite the intensive conditions of the cultivation (high
Fig. 9 Relative contributions per phase to selected impact categories for the
use of 584.0 g of moisturizing cream.
Fig. 10 Relative contributions per input and output to selected impact cat-
egories for the formulation phase C.
Fig. 11 Relative contributions per input and output to selected impact cat-
egories for the end life phase D.
Paper Green Chemistry
3348 |Green Chem., 2013, 15, 3337–3354 This journal is © The Royal Society of Chemistry 2013
degree of mechanization, use of agrochemicals in high levels,
etc.), this hydrophilic raw material does not affect significantly
the environmental profile of APG because of the stoichiometry
involved during the glucosylation reactions: 963 kg of cetearyl
alcohol and 128 kg of glucose to achieve 1 t of APG.
The glucosylation process is responsible for 9% OD, 2%
GW, 8% MR, 12% PR, 8% EC, 11% AC/EU and 3% WC. This
contribution is certainly quite lower than the cetearyl alcohol
one but enough to be detailed in order to identify which para-
meters of the process could be improved.
4.3.1 Impact details of the cetearyl alcohol furniture
(phase A-3). Cetearyl alcohol manufacture is the source of a
large part of the impacts of APG because of the cultivation
mode of palm trees, the oil extraction/transformations and the
transport (Fig. 13). The crop inputs have an impact in all cat-
egories. This result is related to the application of fertilizers on
palm trees (NPK based fertilizers) as well as the diffuse emis-
sions from these agrochemical applications. In the figure
below, the cultivation energy was integrated with the crop
inputs but as the mechanization is not very developed in palm
plantations, the contribution of this parameter is very low.
The type of soil and vegetation upon which the oil palms
grow plays a major role in GW results. The land use change is
responsible for 8.0 kg CO
2
eq. per kg of cetearyl alcohol (64%)
and for 7.8 kg CO
2
eq. per kg of APG (64%). These results are
quite high and are probably overestimated because of the
drastic initial assumptions. Firstly, it was supposed that
the palms are grown on un-degraded soil. This situation is not
very realistic as it occurs only once at the beginning of the
plantation and as oil palm planting is very often carried out on
soils already degraded by other crops. Secondly, as mentioned
in the previous LCI, the soil repartition is 61% of primary
forest, 31% of intact meadow and 8% of non-degraded peat
land. According to the literature,
59,60
it is assumed that the
land use change of primary forest, intact meadow and non-
degraded peat land corresponds to respective CO
2
emissions:
25.1, 1.7 and 100.0 t eq. ha
−1
year
−1
. Taking into account the
removal of CO
2
from the atmosphere by the palm crop (bio-
genic CO
2
) which is considered equal to 7.7 t eq. ha
−1
year
−1
in this study,
61,62
the land use change of primary forests and
peat lands appears as a carbon release effect whereas the land
use change of meadows appears as a carbon storage effect
(Table 7).
Thus, the influence of the soil repartition on the environ-
mental impacts of the production of cetearyl alcohol and APG
is discussed in Section 5.2 in order to temper the results about
GW. Regarding the cultivation mode, the sensitivity of the FFB
yield is also assessed in Section 5.3.
The extraction, refining, transesterification and hydrogen-
ation processes also have significant impacts: 20% OD, 30%
GW, 36% MR, 51% PR, 59% EC, 49% AC/EU and 73% WC.
They are mainly linked to the energy supplied (heating, distil-
lation, etc.), the need for water (steam, washing steps, etc.), the
POME treatments, the biogases emitted by POME (methane),
and the use of methanol (even if it is recycled). However, it is
important to underline that the energetic needs are limited
thanks to the use of shells and fibres as waste fuel and
several international projects (Clean Development Mechanism
Table 6 Impact assessment results associated with the production of 1 t of
APG
Impact categories Unit Value
Ozone depletion (OD) kg CFC-11 eq. 3.4 × 10
−4
Global warming (GW) t CO
2
eq. 12.3
Mineral resources (MR) MJ 55.9
Petrochemical resources (PR) MJ 3335.5
Eco-toxicity (EC) PAF m
−2
year
−1
826.3
Acidification/eutrophication (AC/EU) PDF m
−2
year
−1
78.3
Water consumption (WC) m
3
190.2
Fig. 12 Relative contributions per input and output to selected impact cat-
egories for the production of 1 t of APG.
Table 7 GW impact according the nature of soil
Soil
Primary
forest
Intact
meadow
Non-degraded
peat land
CO
2
emission by land use
change (t eq. ha
−1
year
−1
)
25.1 1.7 100.0
Biogenic CO
2
(t eq. ha
−1
year
−1
)
7.7 7.7 7.7
CO
2
emissions by land
use change
(t eq. ha
−1
year
−1
)
17.4 −6.0 92.3
Fig. 13 Relative contributions per input and output to selected impact cat-
egories for the production of cetearyl alcohol.
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projects within the framework of the Kyoto protocol) have
been initiated in order to capture biogases from POME to
produce electricity.
36
According to the United Nations Frame-
work Convention on Climate Change,
63
about 92% of biogases
from POME can be captured allowing the production of 205
MJ of electricity per t of POME. The influence of the non-use
of methanol during the hydrogenation process is assessed in
Section 5.4.
Obviously, the transport also has significant impacts due to
the geographical localization of the different plants: palm cul-
tivation, oil extraction and refining in Malaysia or Indonesia
and oil transesterification and hydrogenation in Germany.
4.3.2 Impact details of the glucosylation process (phase B
without raw materials). According to Fig. 14, the glucosylation
process inputs (chemicals, catalyst, nitrogen, packaging, etc.)
have no significant impacts (between 0 and 2.0%) except for
WC (24%). The volume of water per t of APG is equal to 7.3 m
3
(without raw materials). It ensures the suitable operating of
liquid ring pumps and the flue gas scrubber of the decantation
device and allows efficient washing operations. Its reduction
can be considered, for instance, by recycling the water of the
liquid ring pumps with closed loop systems or by optimizing
the number and the efficiency of the washing steps.
The contribution of energy (mainly gas and electricity) has
the following profile: 4% OD, 9% GW, 24% MR, 5% PR, 20%
EC, 6% AC/EU and 44% WC. It is not so high but it can always
be optimized.
Whatever the impact category, the most contributing para-
meter is the transport due to the transport mode (lorry) and
the distances: wheat cultivation in the North of France, manu-
facture of cetearyl alcohol in Germany and the glucosylation
process in the South of France. Finally, there are the wastes
produced during the glucosylation reactions (glucose mud and
wastewater with COD). As a reminder, their quantities are not
very high (76 kg of mud and 14 l of wastewater per t of APG)
and their toxicities to the environment are not problematic.
Nevertheless, in comparison with the other parameters,
wastes appear to be significant and the reduction of their
quantity or a better valorization can be interesting ways of
improvement.
5 Discussion
The results of FU 1 showed that the packaging of the cream
and its purchasing are the most contributing parameters. As
the influence of the purchasing is quite easy to anticipate (the
lower the distance is, the greener the transport mode is and
the lower the impacts are), the sensitivity of the packaging
only is discussed hereafter.
Even if the APG impacts do not predominate regarding
FU 1, FU 2 allowed us to conclude that the environmental
profile of APG directly depends on the manufacturing con-
ditions of the cetearyl alcohol. So, the influences of the
land use change, the FFB yield and the transesterification/
hydrogenation process on the APG impacts are analyzed in the
following section.
5.1 Sensitivity assessment of the cream packaging (FU 1)
Up to now, the modeling was performed with a 30 g jar made
of 7 g of PET and equipped with a tight fitting lid made of 5 g
of aluminium. This kind of packaging corresponds to an entry
level packaging.
For the jar only, two other types of packaging have been
assessed: a mid-range packaging characterized by the same
material as the reference but with higher thickness (9 g of
PET) and a high range packaging made of 20 g of glass.
According to the sensitivity results shown in Fig. 15, as was
expected, the shifting to a mid-range packaging with more PET
does not give better results whatever the impact category. By
contrast, there are environmental improvements when shifting
to a glass packaging. Compared to the reference, this material
induces a decrease of 60% OD, 7% GW, 16% MR, 23% PR,
29% EC, 13% WC and an increase of 81% AC/EC. This trend is
explained by the processes to prepare PET and glass and,
according to the databases, the glass manufacture is less
impacting than the PET one.
Consequently, a first way to reduce the environmental
profile of the moisturizing cream lies in using suitable pack-
aging giving priority to non-petrochemical and/or renewable
raw materials.
Fig. 14 Relative contributions to selected impact categories for the production
of APG (without raw materials).
Fig. 15 Comparative environmental impacts of different kinds of packaging of
the cosmetic cream.
Paper Green Chemistry
3350 |Green Chem., 2013, 15, 3337–3354 This journal is © The Royal Society of Chemistry 2013
5.2 Sensitivity assessment of the land use change (FU 2)
As described before, the GW impact of APG is equal to 12.3 t
CO
2
eq. t
−1
and is predominantly driven by the nature of soils
for the cultivation of palms.
61,62
The land use change presents
a contribution of about 64% of the total carbon footprint of
APG (7.8 t CO
2
eq. t
−1
). However, Fig. 16 shows that this
carbon footprint may vary significantly depending on the
initial assumptions (from 1.9 to 49.8 t CO
2
eq. t
−1
).
For this study (reference), un-degraded soils were supposed
with a repartition corresponding to an average in Malaysia:
61% of forest, 31% of meadow and 8% of peat land. If this
repartition shifts to 100% of intact meadow, the carbon foot-
print of APG would decrease from 12.3 to 1.9 t CO
2
eq. t
−1
.By
contrast, if the palms are grown on 100% of intact peat land,
the carbon footprint would increase drastically to 49.8 t CO
2
eq. t
−1
. Of course, if the LCA was done from already used soils
for other crops and the land use change was not taken into
account, the final carbon footprint of APG would be very low
but not representative of reality. Consequently, a way of
improving the environmental profile of APG is the limitation
and the control of the land use change. This orientation is
actually very present in media due to the unfortunately well
known problems caused by the intensive cultivation of palm
trees such as primary forest degradation and disappearance,
reduction of biodiversity, etc. In 2004, the Roundtable on Sus-
tainable Palm Oil (RSPO; http://www.rspo.org) was created and
one of the goals of this organization was to promote palm oils
coming from already existing plantations with no more degra-
dation of soils. So, even if the part of palm oils used for APG
production is low, the purchasing specifications of the cetearyl
alcohol can contribute to the reduction of their environmental
impacts.
5.3 Sensitivity assessment of the FFB yield (FU 2)
The FFB yield optimization is also a scope of improvement in
order to prevent the land use change.
In this work, mean cultivation conditions representative of
Malaysia or Indonesia were chosen: 19.9 t of FFB ha
−1
year
−1
and 142 palm trees ha
−1
. The density is quite difficult to opti-
mize because of the physiological needs of the trees and their
size but the FFB yield can be supposed to be higher. On the
one hand, if the climatic conditions are very favourable, the
FFB yield can reach 23.7 t of FFB ha
−1
year
−1
and, on the other
hand, prospective yields of about 32.0 t of FFB ha
−1
year
−1
are
described in the literature
64
with optimized seeds developed
by the Centre de coopération Internationale en Recherches
Agronomiques pour le Développement (CIRAD). Even if these
two levels of yields are not based on recurrent conditions (opti-
mistic climatic conditions or non-commercial seeds), their
influence on the environmental profile of APG is compared in
Fig. 17. Decreases between 3% and 11% for an FFB yield of
24 t ha
−1
year
−1
and between 6 and 25% for a yield of 32 t ha
−1
year
−1
are observed depending on the impact categories. In
conclusion, the productivity of the already cultivated soils is a
crucial parameter. It can be further optimized but beware, the
potential improvements do not have to lead to intensive con-
ditions with high levels of fertilizers or pesticides and mechan-
ization. The balance between the benefits and the drawbacks
to the environment must always be taken into consideration.
5.4 Sensitivity assessment of the transesterification process
(FU 2)
The transesterification and hydrogenation processes to achieve
the cetearyl alcohol from RPKO are also sources of impacts
during the life cycle of APG. As it is the most widespread on
the industrial scale, the “methyl ester route”process was
selected for the LCA of APG (Fig. 18).
It consists of converting the oil into the corresponding
esters by reaction with methanol and recycling this methanol
after the hydrogenation step (Fig. 17). By contrast, the “wax
ester route”process is based on a direct splitting of the oil
into fatty acids which are esterified with fatty alcohol before
hydrogenating them. The fatty alcohol is also recycled and the
main advantage is the non-use of an organic solvent. The
corresponding inputs of these two processes and their com-
pared impacts are illustrated in Table 8 and in Fig. 19.
The “wax ester route”process leads to environmental
benefits: 25% OD, 29% GW, 8% MR, 26% PR, 1% EC, 22%
AC/EU and 19% WC. These results tend to encourage us to
shift to the wax ester route but this improvement requires
important industrial investments. So, this perspective is only a
realistic long term solution.
Fig. 16 Carbon footprint of 1 t of APG according to the nature of the culti-
vated soil.
Fig. 17 Influence of the FFB yield on the impact of APG.
Green Chemistry Paper
This journal is © The Royal Society of Chemistry 2013 Green Chem., 2013, 15, 3337–3354 | 3351
6 Conclusions
This work examined the environmental impacts of APG used
as an emulsifying surfactant in a cosmetic cream and
identified the parameters during APG production which are
responsible for the most important impacts.
The results showed that APG has relatively low impacts
when it is incorporated at 5% into a cosmetic cream. The
impacts are between 4 and 24% depending on the impact cat-
egory. Over the whole life cycle of the cream, the main key
issues are the formulation step and the end use. Their respec-
tive environmental contributions are 15 to 51% and 30 to 77%.
Regarding the formulation step, the two most contributing
parameters are the oil of the emulsion and the packaging of
the cream. The oil’s impacts are directly linked to the quantity
involved (20% in the cream) and also to the cultivation con-
ditions of the plant from which the oil is extracted. For this
study, the oil considered was RPKO, the same oil used for the
manufacture of the cetearyl alcohol. A sensitivity study on the
nature of the packaging highlights that glass is much better
than PET. As far as the end use of the cream is concerned, the
main impacting parameter is the purchasing by the consumer
(between 33 and 77%).
Despite the limited contribution of APG to the cream’s
impacts, their environmental profile was examined and indi-
cated the high impacts of the cetearyl alcohol (more than 80%
by weight in APG). The carbon footprint of APG depends
directly on the cultivation mode of the palm trees and, accord-
ing to the land use change, it can vary between 1.9 and 49.8 t
CO
2
eq. per t of APG. The impacts directly due to the glucosyla-
tion process (without raw materials) are between 2 and 12%,
mainly coming from the transport of raw materials and waste
management.
The LCA of this study consequently gave a precise picture of
the role that APG plays in the sustainability of a cosmetic
emulsion. The next step may be to compare its impacts with
those of other surfactants that also respond to the first func-
tional unit in order to confirm the green status of this kind of
biosurfactant.
19
Finally, improvements in APG processing and use can also
be brought about and all levels of the production chain are
relevant: raw material suppliers (fatty alcohol quality and
transport), APG manufacturers (utilities consumption follow-
up, waste management and transport), finished cosmetic
product formulators (packaging) and final consumers (trans-
port mode).
Acknowledgements
The authors are very grateful for the valuable advice given by
every participant of the workshop. They also acknowledge all
the employees of the plant at Castres who were involved in the
data collection.
Finally, they would like to sincerely thank the ADEME for its
financial support.
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