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\begin{document}

\title{Cocoa butter equivalent from Kpangnan butter and Pequi oil}



\author[1]{Saeed Mirzaee Ghazani}%
\author[2]{Andrea Madalena Guedes}%
\author[2]{Rosemar Antoniassi}%
\author[1]{Alejandro Marangoni}%
\affil[1]{University of Guelph}%
\affil[2]{Embrapa Food Agroindustry}%


\vspace{-1em}



  
  \date{May 26, 2024}


\begingroup
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\selectlanguage{english}
\begin{abstract}
Novel cocoa butter equivalents were designed using dry fractionated
Pequi oil and solvent fractionated Kpangnan butter. Static
crystallization of binary mixtures of these two fractions into the
triclinic form (\selectlanguage{greek}β\selectlanguage{english}2) was achieved after 12 days for all mixtures and
after 4 days for the 80:20 w/w and 90:10 w/w fractionated Kpangnan:Pequi
oil mixtures. Moreover, after 60 days of storage at 22oC, all binary
blends (except 100\% fractionated pequi oil and 100\% fractionated
Kpangnan butter) were crystallized in the most stable triclinic crystal
form (\selectlanguage{greek}β\selectlanguage{english}1). Here we also discovered an unusual melting behavior for the
fractionaled 30:70 w/w and 20:80 w/w fractionated Kpangnan:Pequi oil
mixtures, where after 4 days of static crystallization at room 22oC,
these mixtures displayed higher than predicted melting points, 41.89 oC
and 33.32 oC, respectively. This suggested a faster kinetics of
transformation to the triclinic \selectlanguage{greek}β\selectlanguage{english}2 form for those mixtures. Our results
suggest that the 30:70 w/w fractionated Kpangnan:Pequi oil mixture with
a melting point of 34oC after 60 days storage at 22oC, a stable
triclinic \selectlanguage{greek}β\selectlanguage{english}2 form, and a triglyceride composition of 28\% POP, 4.6\% POS
and 33\% SOS displayed solid state characteristics, melting point and
crystal structure, of a commercial cocoa butter equivalent.%
\end{abstract}%



\sloppy


\textbf{INTRODUCTION}

Exotic fats are defined as a group of fats obtained from wild,
uncultivated crops. Common exotic butters such as illipe (\emph{Shorea
stenoptera} ), sal (\emph{Shorea robusta} ), shea (\emph{Butyrospermum
parkii} ), kokum (\emph{Garcinia indica} ), and mango kernel
(\emph{Magnifera indica} ) have been used to manufacture CBE on an
industrial scale. However, their supply on a large scale is limited
since they are extracted from the seeds or kernels of wild fruit trees
growing in tropical forests (Salas, Bootello, Mart\selectlanguage{ngerman}ínez-Force, \& Garcés,
2009). The main triacylglycerols in these fats are either
1,3-stearoyl-2-oleoyl-glycerol (SOS) or a combination of
1-palmitoyl-2-oleoyl-3-stearoyl-glycerol (POS) and SOS, and these
natural butters lack one of the main structural triacylglycerols (TAGs)
of cocoa butter, 1,3-dipalmitoyl-2-oleoyl-glycerol (POP). The main
source of POP for the formulation of commercial CBEs is palm-mid
fraction (PMF) that is obtained by the multi-step dry fractionation of
palm oil. Currently, the main concern about using palm oil and its
derivatives in food is the lack of sustainability of these products as a
result of rainforest destruction (Austin, Mosnier, Pirker, McCallum,
Fritz, \& Kasibhatla, 2017). Although sustainable palm oil production
has been started in some countries, these attempts are limited compared
to total world palm oil production (Carlson, Heilmayr, Gibbs, Noojipady,
Burns, Morton, Walker, Paoli, \& Kremen, 2018).

Pequi is a yellow to orange, strong-flavored oleaginous fruit of pequi
tree (\emph{Caryocar brasiliense} ), mainly native of the Amazon,
Caatinga, Cerrado, and the rainforest regions of Brazil. However, pequi
trees can also be found in Central and South America (Guedes, Antoniassi
\& Faria-Machado, 2017; Vieira \& Martins, 2000). Pequi fruit has a
green spherical shape containing four internal yellowish mesocarps rich
in oil (35-66\% dry base) covering four pequi kernels containing pequi
kernel oil. Pequi kernel oil has non-edible applications in the
oleochemical industry (Faria-Machado, Tres, van Ruth, Antoniassi,
Junqueira, Lopes, \& Bizzo, 2015). Previous studies showed the primary
fatty acids in pulp pequi oil were palmitic acid (36\%), palmitoleic
acid (1\%), stearic acid (2\%), oleic acid (57\%), linoleic acid (2\%),
and linolenic acid (\textless{}0.5\%). In comparison, the main TAGs in
pequi oil were 1-palmitoyl-2 3-dioleoyl-glycerol (POO) (39\%) and POP
(34\%) (Guedes, Antoniassi, Galdeano, Grimaldi, de Carvalho, Wilhelm \&
Marangoni, 2017).

Kpangnan (\emph{Pentadesma butyracea} ) butter is also known as Kanga,
Kanya, Painya, and Akpoto is obtained from the kernels of the berries
that grow on the Kpangnan tree is known as tallow tree, predominantly in
Ghana and some parts of West Africa such as Democratic Republic of Congo
(Ayegnon, Kayodé, Tchobo, Azokpota, Soumanou \& Hounhouigan, 2015).
Kpangnan butter has non-edible applications in African societies, and it
is mainly used as a massage oil for skin and hair care and in the
manufacturing of soap (Dencausse, Ntsourankoua, Artaud \& CLAMOU, 1995).
The fatty acid composition of Kpangnan butter is quite similar to shea
butter and mainly contains palmitic acid (3-4\%), stearic acid
(43-47\%), oleic acid (49-53\%), and linoleic acid (\textless{}1\%). The
main identified TAGs in Kpangnan butter are POS (1-2\%), triolein (OOO)
(1.5-3\%), 1-stearoyl-2, 3-dioleoyl-glycerol (SOO) (35-49\%) and SOS
(37-61\%). (Adomako, 1977; Tchobo, Natta, Barea, Barouh, Piombo, Pina,
et al. \& Sohounhloue, 2007).

The main objective of this study was to evaluate the physicochemical
properties of various mixtures of dry fractionated pequi oil as a source
of POP and solvent fractionated Kpangnan butter as a source of SOS to
produce more sustainable CBEs.

\textbf{Material and Methods}

Unrefined artisanal pequi pulp oil was provided by Fazenda Lagoa (Minas
Gerais, Brazil), and Kpangnan butter was bought from ALAFFIA Co.
(Olympia, WA, USA). Acetone (ACS reagent, \textgreater{} 99.5\%) for
solvent crystallization was supplied from Fisher Scientific (Ottawa, ON,
Canada).

\textbf{Pequi oil dry fractionation}

The pequi oil was dry fractionated in a 2L jacketed glass reactor (HEL
D-95 126 Shwabach) with a paddle-type mechanical stirrer connected to a
high torque RZR 2102 motor (Heidolph Instruments, Schwabach, Germany)
and a thermostatic bath (Julabo F25) with a temperature controller and
thermocouples. First, 1000 to 1500 g of filtered oil was heated to 50°C
for 20 minutes while mixing at 7 rpm, then it was cooled down at the
rate of 3°C/h to the crystallization temperature (20°C), and while
mixing was continued it was kept at 20°C for seven hours. The olein
fraction was gravimetric transferred to a jacketed stainless steel
filtration system (Zeitz Enzinger NOLL Maschinenbau Maschinenbau AG
EF1412, Mannheim, Germany) coupled to a vacuum pump (Prismatec, São
Paulo, Brazil). The oleic fraction separation was repeated several times
using filter paper (Unifil Qualitativo, C41) to obtain the stearin
fraction.

\textbf{Kpangnan butter solvent fractionation}

Acetone fractionation was used to remove high melting and low melting
TAGs from the Kpangnan oil to obtain a higher proportion of SOS in the
final fractions. The ratio of Kpangnan oil: acetone was 1:4 w/w to
fractionate at three different temperatures of 16, 22, and 25 °C. In the
first acetone crystallization step, most of the SOS was fractionated,
while the second and the third fractionations were used to remove low
melting TAGs (SOO and OOO) and increasing SOS concentration.

\textbf{Preparing binary mixtures}

Binary mixtures were prepared by mixing melted pequi stearin (FPO)
(obtained by dry fractionation at 20C°) with fractionated Kpagnan butter
(FKB) in the ratios of 0:100, 10:90, 20:80, 30:70, 40:60, 50:50, 60:40,
70:30, 80:20, 90:10, and 100:0 (w/w). The mixtures were heated to 80°C
for 30 minutes to clear the memory of crystallization then solidified at
room temperature (22°C) for 4, 12, and 60 days under static
crystallization, followed by XRD and DSC analysis.

\textbf{Determination of Triacylglycerol Composition}

The Triacylglycerol (TAG) composition of the fractionated pequi oil,
fractionated Kpangnan butter, and their binary mixtures were determined
using a Waters Alliance model 2690 high-performance liquid
chromatography (HPLC) with a refractive index detector (Waters model
2410, Waters, Milford, MA, USA). Chromatographic separation of the TAGs
in the samples was obtained with a Waters Xbridge C18 (Waters Limited,
Mississauga, ON, Canada) column (4.6 mm × 250 mm internal diameter with
5 \selectlanguage{greek}μ\selectlanguage{english}m particle size). Isocratic elution with a flow rate of 1 mLmin-1 of
degassed acetone/acetonitrile 60/40 (v/v) was applied. Column and
detector temperatures were set at 40 \textsuperscript{o}C. The separated
peaks were analyzed using Millenium 32 software (K\&K Testing, LLC,
Decatur, GA, USA). The TAG composition was determined using internal
standards and their corresponding retention times.

\textbf{Crystal structure and polymorphism}

Static crystallization at room temperature 22-23 \textsuperscript{o}C at
different crystallization times (4, 12, and 60 days) was applied to
crystallize blends before X-ray analysis. The crystal structure and
polymorphic form of solidified samples were analyzed by X-ray
diffraction (Multiflex Powder X-ray spectrometer, Rigaku, Tokyo, Japan).
The copper X-ray tube (wavelength of 1.54 \selectlanguage{ngerman}Å) was operated at 40 kV and
44 mA. The measurement scan rate was set at 0.3 per minute in the range
2\selectlanguage{greek}θ\selectlanguage{english}=1-30 at 20 \textsuperscript{o}C. The diffracted peak positions were
determined using MDI Jade 9 (MDI, Livermore, CA, USA) software.

\textbf{Melting point and enthalpy of fusion}

Melting points and enthalpies of fusion of samples were obtained using a
differential scanning calorimeter (DSC) model Q2000 (TA Instruments,
Mississauga, ON, Canada). Nitrogen was used as the purge gas with a flow
of 18 mL/minute. In this experiment, melting points (endothermic peak)
of samples (2-5 mg) were determined by heating samples from 5 \selectlanguage{ngerman}°C to 60
°C at the heating rate of 5 °C/minute.

\textbf{RESULTS AND DISCUSSION}

Crystal structure and polymorphism

Binary mixtures of dry fractionated pequi oil (source of POP) and
solvent fractionated Kpangnan butter (source of SOS) were prepared at
different proportions and kept at room temperature to statically
crystallize them for 4, 12, and 60 days. In a previous study, we showed
that a CBE's compatibility with CB depends on the main triacylglycerols
present in the CBE and their crystal polymorphic structure. This is
mostly influenced by interactions between the main TAGs in CBE and CB,
namely POP, POS, and SOS (Ghazani \& Marangoni, 2018). Small and
wide-angle powder X-ray diffraction peaks after 4, 12, and 60 days of
storage at room temperature are shown in Tables 1 to 3, respectively. As
shown in Table 1 and Fig.1, the most prominent reflections in the WAXS
region for 100\% solvent fractionated Kpangnan butter were observed at
4.74 Å (s), 4.50 Å (m), 3.9 Å (S), and 3.63 Å (w), suggesting the \selectlanguage{greek}γ
\selectlanguage{english}crystal structure of SOS (Sato, Arishima, Wang, Ojima, Sagi \& Mori,
1989). In this field, vs, s, m, and w, represent ''very strong'',
''strong'', ''medium'' and ''weak'' peak intensities. The long-spacing
observed for 100\% fractionated Kpangnan butter was at 73.7 \selectlanguage{ngerman}Å,
corresponding to the reflection from the (001) crystalline plane.

Similar short-spacing has been reported by Sato, Arishima, Wang, Ojima,
Sagi \& Mori (1989) for SOS in \selectlanguage{greek}γ \selectlanguage{english}crystal form at 4.72 \selectlanguage{ngerman}Å (s), 4.50 Å (m),
3.88 Å (s), and 3.63 Å (w), while Wang, Sato, Sagi, Izumi \& Mori (1987)
reported an identical long-spacing pattern at 73.7 Å for SOS in \selectlanguage{greek}γ
\selectlanguage{english}crystal form. Similar diffraction patterns in both SAXS and WAXS regions
were observed for 10\% to 40\% mixtures containing fractionated pequi
oil. With increasing amounts of fractionated pequi oil, from 50\% to
70\%, a mixture of \selectlanguage{greek}γ \selectlanguage{english}and pseudo-\selectlanguage{greek}β\selectlanguage{english}'\textsubscript{2} polymorphic forms
was obtained. This can be deduced from the presence of a reflection at
\textasciitilde{}42 \selectlanguage{ngerman}Å in the SAXS region and WAXS reflections at 4.23 Å
and 3.96 Å that indicates the presence of the
pseudo-\selectlanguage{greek}β\selectlanguage{english}'\textsubscript{2}form of POP (Sato, Arishima, Wang, Ojima, Sagi
\& Mori, 1989). Moreover, the long-spacing value at 42 \selectlanguage{ngerman}Å corresponds to
the double chain length structure of the POP molecule in the
pseudo-\selectlanguage{greek}β\selectlanguage{english}'\textsubscript{2} crystal structure (Sato, Arishima, Wang,
Ojima, Sagi \& Mori, (1989). The binary mixtures containing 80\% and
90\% fractionated pequi oil showed a mixture of mainly triclinic crystal
structures in the \selectlanguage{greek}β\selectlanguage{english}\textsubscript{2}crystal form plus
pseudo-\selectlanguage{greek}β\selectlanguage{english}'\textsubscript{2} form. After static crystallization at room
temperature for four days, 100\% fractionated pequi oil showed a
pseudo-\selectlanguage{greek}β\selectlanguage{english}'\textsubscript{2} crystal structure.

After 12 days of storage at 22 \textsuperscript{o}C, in all mixtures,
the pseudo-\selectlanguage{greek}β\selectlanguage{english}'\textsubscript{2} form had transformed to the stable
triclinic \selectlanguage{greek}β\selectlanguage{english}\textsubscript{2} form, except for 100\% fractioned pequi oil
and 100\% fractionated Kpangnan butter, which displayed the
pseudo-\selectlanguage{greek}β\selectlanguage{english}'\textsubscript{2} form, and mixtures of
pseudo-\selectlanguage{greek}β\selectlanguage{english}'\textsubscript{2} and \selectlanguage{greek}β\selectlanguage{english}\textsubscript{2}crystal forms,
respectively. A double chain length structure characteristic of the
pseudo-\selectlanguage{greek}β\selectlanguage{english}'\textsubscript{2} form was observed in both samples (Table 2
and Fig.1).

After 60 days of storage at 22 \textsuperscript{o}C, all mixtures had
transformed to the triclinic \selectlanguage{greek}β\selectlanguage{english}\textsubscript{2} form, except for 100\%
fractionated pequi oil. Two strong reflections in the WAXS region at
4.30 \selectlanguage{ngerman}Å and 3.97 Å, and a long spacing of 41.9 Å were observed (Table 3).
This suggested the presence of a pseudo-\selectlanguage{greek}β\selectlanguage{english}'\textsubscript{1} polymorphic
form, similar to the crystal polymorphic form of pure POP in the
pseudo-\selectlanguage{greek}β\selectlanguage{english}'\textsubscript{1} crystal form (Sato, Ueno \& Yano1999). Wang,
Sato, Sagi, Izumi \& Mori (1987) showed that the polymorphic transition
rate for the POP molecule was very slow, and the transition from
pseudo-\selectlanguage{greek}β\selectlanguage{english}' to \selectlanguage{greek}β\selectlanguage{english}\textsubscript{2} took about 15 days after storing at
30\textsuperscript{o}C. While for SOS molecule, the transition rate from
pseudo-\selectlanguage{greek}β\selectlanguage{english}' to \selectlanguage{greek}β\selectlanguage{english}\textsubscript{2} was fast (16 hours at
35\textsuperscript{o}C).

The addition of fractionated Kpangnan butter to fractionated pequi oil
accelerated the crystal polymorphic transition to the triclinic form.
The very strong peak at 4.6 \selectlanguage{ngerman}Å indicated the \selectlanguage{greek}β \selectlanguage{english}crystal structure for all
blends. It is important to notice that after 60-days of storage, the
high SOS content in fractionated Kpangnan butter induced a
transformation to the \selectlanguage{greek}β\selectlanguage{english}\textsubscript{1} polymorphic form for all
mixtures. The presence of two strong peaks at 3.73 \selectlanguage{ngerman}Å and 3.69 Å
indicated the completion of the polymorphic transition to the most
stable triclinic form (\selectlanguage{greek}β\selectlanguage{english}\textsubscript{1}) (Fig. 2). Sato, Arishima,
Wang, Ojima, Sagi \& Mori (1989) reported a similar diffraction pattern
for pure SOS in the \selectlanguage{greek}β\selectlanguage{english}\textsubscript{1} crystal form.

Table 1- Small and wide-angle powder X-ray diffraction data for the
different crystal polymorphic forms of fractionated pequi oil and
fractionated Kpangnan butter binary mixtures after 4 days of storage\selectlanguage{english}
\begin{longtable}[]{@{}llllllll@{}}
\toprule
\begin{minipage}[b]{0.10\columnwidth}\raggedright\strut
Fractionated Pequi oil (\%)\strut
\end{minipage} & \begin{minipage}[b]{0.10\columnwidth}\raggedright\strut
Long-spacing (\selectlanguage{ngerman}Å)\strut
\end{minipage} & \begin{minipage}[b]{0.10\columnwidth}\raggedright\strut
Short-spacing (\selectlanguage{ngerman}Å)*\strut
\end{minipage} & \begin{minipage}[b]{0.10\columnwidth}\raggedright\strut
Short-spacing (\selectlanguage{ngerman}Å)*\strut
\end{minipage} & \begin{minipage}[b]{0.10\columnwidth}\raggedright\strut
Short-spacing (\selectlanguage{ngerman}Å)*\strut
\end{minipage} & \begin{minipage}[b]{0.10\columnwidth}\raggedright\strut
Short-spacing (\selectlanguage{ngerman}Å)*\strut
\end{minipage} & \begin{minipage}[b]{0.10\columnwidth}\raggedright\strut
Short-spacing (\selectlanguage{ngerman}Å)*\strut
\end{minipage} & \begin{minipage}[b]{0.10\columnwidth}\raggedright\strut
Short-spacing (\selectlanguage{ngerman}Å)*\strut
\end{minipage}\tabularnewline
\midrule
\endhead
\begin{minipage}[t]{0.12\columnwidth}\raggedright\strut
0 (\selectlanguage{greek}γ\selectlanguage{english})\strut
\end{minipage} & \begin{minipage}[t]{0.12\columnwidth}\raggedright\strut
73.7\strut
\end{minipage} & \begin{minipage}[t]{0.12\columnwidth}\raggedright\strut
4.74 (s)\strut
\end{minipage} & \begin{minipage}[t]{0.12\columnwidth}\raggedright\strut
4.50 (m)\strut
\end{minipage} & \begin{minipage}[t]{0.12\columnwidth}\raggedright\strut
3.90 (s)\strut
\end{minipage} & \begin{minipage}[t]{0.12\columnwidth}\raggedright\strut
3.63 (w)\strut
\end{minipage} & \begin{minipage}[t]{0.12\columnwidth}\raggedright\strut
-\strut
\end{minipage} & \begin{minipage}[t]{0.12\columnwidth}\raggedright\strut
-\strut
\end{minipage}\tabularnewline
\begin{minipage}[t]{0.12\columnwidth}\raggedright\strut
10 (\selectlanguage{greek}γ\selectlanguage{english})\strut
\end{minipage} & \begin{minipage}[t]{0.12\columnwidth}\raggedright\strut
70.1\strut
\end{minipage} & \begin{minipage}[t]{0.12\columnwidth}\raggedright\strut
4.74 (s)\strut
\end{minipage} & \begin{minipage}[t]{0.12\columnwidth}\raggedright\strut
4.55 (m)\strut
\end{minipage} & \begin{minipage}[t]{0.12\columnwidth}\raggedright\strut
4.46 (m)\strut
\end{minipage} & \begin{minipage}[t]{0.12\columnwidth}\raggedright\strut
4.21 (w)\strut
\end{minipage} & \begin{minipage}[t]{0.12\columnwidth}\raggedright\strut
3.90 (s)\strut
\end{minipage} & \begin{minipage}[t]{0.12\columnwidth}\raggedright\strut
3.60 (w)\strut
\end{minipage}\tabularnewline
\begin{minipage}[t]{0.12\columnwidth}\raggedright\strut
20 (\selectlanguage{greek}γ\selectlanguage{english})\strut
\end{minipage} & \begin{minipage}[t]{0.12\columnwidth}\raggedright\strut
70.1\strut
\end{minipage} & \begin{minipage}[t]{0.12\columnwidth}\raggedright\strut
4.74 (s)\strut
\end{minipage} & \begin{minipage}[t]{0.12\columnwidth}\raggedright\strut
4.57 (m)\strut
\end{minipage} & \begin{minipage}[t]{0.12\columnwidth}\raggedright\strut
4.43 (m)\strut
\end{minipage} & \begin{minipage}[t]{0.12\columnwidth}\raggedright\strut
4.21 (w)\strut
\end{minipage} & \begin{minipage}[t]{0.12\columnwidth}\raggedright\strut
3.90 (s)\strut
\end{minipage} & \begin{minipage}[t]{0.12\columnwidth}\raggedright\strut
3.62 (w)\strut
\end{minipage}\tabularnewline
\begin{minipage}[t]{0.12\columnwidth}\raggedright\strut
30 (\selectlanguage{greek}γ \selectlanguage{english}+ pseudo-\selectlanguage{greek}β\selectlanguage{english}'\textsubscript{2})\strut
\end{minipage} & \begin{minipage}[t]{0.12\columnwidth}\raggedright\strut
71.8\strut
\end{minipage} & \begin{minipage}[t]{0.12\columnwidth}\raggedright\strut
4.77 (s)\strut
\end{minipage} & \begin{minipage}[t]{0.12\columnwidth}\raggedright\strut
4.58 (m)\strut
\end{minipage} & \begin{minipage}[t]{0.12\columnwidth}\raggedright\strut
4.46 (m)\strut
\end{minipage} & \begin{minipage}[t]{0.12\columnwidth}\raggedright\strut
4.23 (w)\strut
\end{minipage} & \begin{minipage}[t]{0.12\columnwidth}\raggedright\strut
3.92 (s)\strut
\end{minipage} & \begin{minipage}[t]{0.12\columnwidth}\raggedright\strut
3.60 (w)\strut
\end{minipage}\tabularnewline
\begin{minipage}[t]{0.12\columnwidth}\raggedright\strut
40 (\selectlanguage{greek}γ \selectlanguage{english}+ pseudo-\selectlanguage{greek}β\selectlanguage{english}'\textsubscript{2})\strut
\end{minipage} & \begin{minipage}[t]{0.12\columnwidth}\raggedright\strut
71.3\strut
\end{minipage} & \begin{minipage}[t]{0.12\columnwidth}\raggedright\strut
4.77 (s)\strut
\end{minipage} & \begin{minipage}[t]{0.12\columnwidth}\raggedright\strut
4.57 (m)\strut
\end{minipage} & \begin{minipage}[t]{0.12\columnwidth}\raggedright\strut
4.48 (m)\strut
\end{minipage} & \begin{minipage}[t]{0.12\columnwidth}\raggedright\strut
4.23 (w)\strut
\end{minipage} & \begin{minipage}[t]{0.12\columnwidth}\raggedright\strut
3.91 (s)\strut
\end{minipage} & \begin{minipage}[t]{0.12\columnwidth}\raggedright\strut
3.60 (w)\strut
\end{minipage}\tabularnewline
\begin{minipage}[t]{0.12\columnwidth}\raggedright\strut
50 (\selectlanguage{greek}γ \selectlanguage{english}+ pseudo-\selectlanguage{greek}β\selectlanguage{english}'\textsubscript{2})\strut
\end{minipage} & \begin{minipage}[t]{0.12\columnwidth}\raggedright\strut
42.2 and 70.1\strut
\end{minipage} & \begin{minipage}[t]{0.12\columnwidth}\raggedright\strut
4.74 (m)\strut
\end{minipage} & \begin{minipage}[t]{0.12\columnwidth}\raggedright\strut
4.57 (m)\strut
\end{minipage} & \begin{minipage}[t]{0.12\columnwidth}\raggedright\strut
4.43 (m)\strut
\end{minipage} & \begin{minipage}[t]{0.12\columnwidth}\raggedright\strut
4.21 (m)\strut
\end{minipage} & \begin{minipage}[t]{0.12\columnwidth}\raggedright\strut
3.98 (m)\strut
\end{minipage} & \begin{minipage}[t]{0.12\columnwidth}\raggedright\strut
3.90 (s)\strut
\end{minipage}\tabularnewline
\begin{minipage}[t]{0.12\columnwidth}\raggedright\strut
60 (\selectlanguage{greek}γ \selectlanguage{english}+ pseudo-\selectlanguage{greek}β\selectlanguage{english}'\textsubscript{2})\strut
\end{minipage} & \begin{minipage}[t]{0.12\columnwidth}\raggedright\strut
42.6 and 70.1\strut
\end{minipage} & \begin{minipage}[t]{0.12\columnwidth}\raggedright\strut
4.76 (m)\strut
\end{minipage} & \begin{minipage}[t]{0.12\columnwidth}\raggedright\strut
4.59 (m)\strut
\end{minipage} & \begin{minipage}[t]{0.12\columnwidth}\raggedright\strut
4.43 (m)\strut
\end{minipage} & \begin{minipage}[t]{0.12\columnwidth}\raggedright\strut
4.21 (m)\strut
\end{minipage} & \begin{minipage}[t]{0.12\columnwidth}\raggedright\strut
3.98 (s)\strut
\end{minipage} & \begin{minipage}[t]{0.12\columnwidth}\raggedright\strut
3.90 (m)\strut
\end{minipage}\tabularnewline
\begin{minipage}[t]{0.12\columnwidth}\raggedright\strut
70 (\selectlanguage{greek}γ \selectlanguage{english}+ pseudo-\selectlanguage{greek}β\selectlanguage{english}'\textsubscript{2})\strut
\end{minipage} & \begin{minipage}[t]{0.12\columnwidth}\raggedright\strut
41.4 and 69.8\strut
\end{minipage} & \begin{minipage}[t]{0.12\columnwidth}\raggedright\strut
4.75 (m)\strut
\end{minipage} & \begin{minipage}[t]{0.12\columnwidth}\raggedright\strut
4.58 (m)\strut
\end{minipage} & \begin{minipage}[t]{0.12\columnwidth}\raggedright\strut
4.42 (m)\strut
\end{minipage} & \begin{minipage}[t]{0.12\columnwidth}\raggedright\strut
4.21 (m)\strut
\end{minipage} & \begin{minipage}[t]{0.12\columnwidth}\raggedright\strut
3.97 (vs)\strut
\end{minipage} & \begin{minipage}[t]{0.12\columnwidth}\raggedright\strut
3.90 (m)\strut
\end{minipage}\tabularnewline
\begin{minipage}[t]{0.12\columnwidth}\raggedright\strut
80 (\selectlanguage{greek}β\selectlanguage{english}\textsubscript{2})\strut
\end{minipage} & \begin{minipage}[t]{0.12\columnwidth}\raggedright\strut
41.8 and 61.0\strut
\end{minipage} & \begin{minipage}[t]{0.12\columnwidth}\raggedright\strut
4.57 (vs)\strut
\end{minipage} & \begin{minipage}[t]{0.12\columnwidth}\raggedright\strut
4.04 (m)\strut
\end{minipage} & \begin{minipage}[t]{0.12\columnwidth}\raggedright\strut
3.97 (m)\strut
\end{minipage} & \begin{minipage}[t]{0.12\columnwidth}\raggedright\strut
3.87 (m)\strut
\end{minipage} & \begin{minipage}[t]{0.12\columnwidth}\raggedright\strut
3.71 (m)\strut
\end{minipage} & \begin{minipage}[t]{0.12\columnwidth}\raggedright\strut
-\strut
\end{minipage}\tabularnewline
\begin{minipage}[t]{0.12\columnwidth}\raggedright\strut
90 (\selectlanguage{greek}β\selectlanguage{english}\textsubscript{2})\strut
\end{minipage} & \begin{minipage}[t]{0.12\columnwidth}\raggedright\strut
40.9 and 61.8\strut
\end{minipage} & \begin{minipage}[t]{0.12\columnwidth}\raggedright\strut
4.58 (vs)\strut
\end{minipage} & \begin{minipage}[t]{0.12\columnwidth}\raggedright\strut
4.06 (m)\strut
\end{minipage} & \begin{minipage}[t]{0.12\columnwidth}\raggedright\strut
3.97 (m)\strut
\end{minipage} & \begin{minipage}[t]{0.12\columnwidth}\raggedright\strut
3.88 (m)\strut
\end{minipage} & \begin{minipage}[t]{0.12\columnwidth}\raggedright\strut
3.73 (m)\strut
\end{minipage} & \begin{minipage}[t]{0.12\columnwidth}\raggedright\strut
-\strut
\end{minipage}\tabularnewline
\begin{minipage}[t]{0.12\columnwidth}\raggedright\strut
100 (pseudo-\selectlanguage{greek}β\selectlanguage{english}'\textsubscript{2})\strut
\end{minipage} & \begin{minipage}[t]{0.12\columnwidth}\raggedright\strut
41.6\strut
\end{minipage} & \begin{minipage}[t]{0.12\columnwidth}\raggedright\strut
4.59 (m)\strut
\end{minipage} & \begin{minipage}[t]{0.12\columnwidth}\raggedright\strut
4.27 (s)\strut
\end{minipage} & \begin{minipage}[t]{0.12\columnwidth}\raggedright\strut
3.97 (s)\strut
\end{minipage} & \begin{minipage}[t]{0.12\columnwidth}\raggedright\strut
-\strut
\end{minipage} & \begin{minipage}[t]{0.12\columnwidth}\raggedright\strut
-\strut
\end{minipage} & \begin{minipage}[t]{0.12\columnwidth}\raggedright\strut
-\strut
\end{minipage}\tabularnewline
\bottomrule
\end{longtable}

*vs, s, m, and w represent ''very strong'', ''strong'', ''medium'' and
''weak'' peak intensities.

Table 2- Small and wide-angle powder X-ray diffraction data for the
different crystal polymorphic forms of fractionated pequi oil and
Kpangnan butter binary mixtures after 12 days of storage\selectlanguage{english}
\begin{longtable}[]{@{}llllllll@{}}
\toprule
\begin{minipage}[b]{0.10\columnwidth}\raggedright\strut
Fractionated Pequi oil (\%)\strut
\end{minipage} & \begin{minipage}[b]{0.10\columnwidth}\raggedright\strut
Long-spacing (\selectlanguage{ngerman}Å)\strut
\end{minipage} & \begin{minipage}[b]{0.10\columnwidth}\raggedright\strut
Short-spacing (\selectlanguage{ngerman}Å)*\strut
\end{minipage} & \begin{minipage}[b]{0.10\columnwidth}\raggedright\strut
Short-spacing (\selectlanguage{ngerman}Å)*\strut
\end{minipage} & \begin{minipage}[b]{0.10\columnwidth}\raggedright\strut
Short-spacing (\selectlanguage{ngerman}Å)*\strut
\end{minipage} & \begin{minipage}[b]{0.10\columnwidth}\raggedright\strut
Short-spacing (\selectlanguage{ngerman}Å)*\strut
\end{minipage} & \begin{minipage}[b]{0.10\columnwidth}\raggedright\strut
Short-spacing (\selectlanguage{ngerman}Å)*\strut
\end{minipage} & \begin{minipage}[b]{0.10\columnwidth}\raggedright\strut
Short-spacing (\selectlanguage{ngerman}Å)*\strut
\end{minipage}\tabularnewline
\midrule
\endhead
\begin{minipage}[t]{0.12\columnwidth}\raggedright\strut
0 (pseudo-\selectlanguage{greek}β\selectlanguage{english}'\textsubscript{2})\strut
\end{minipage} & \begin{minipage}[t]{0.12\columnwidth}\raggedright\strut
65.1 and 74.0\strut
\end{minipage} & \begin{minipage}[t]{0.12\columnwidth}\raggedright\strut
4.74 (vs)\strut
\end{minipage} & \begin{minipage}[t]{0.12\columnwidth}\raggedright\strut
4.59 (s)\strut
\end{minipage} & \begin{minipage}[t]{0.12\columnwidth}\raggedright\strut
4.49 (m)\strut
\end{minipage} & \begin{minipage}[t]{0.12\columnwidth}\raggedright\strut
3.9 (vs)\strut
\end{minipage} & \begin{minipage}[t]{0.12\columnwidth}\raggedright\strut
3.67 (m)\strut
\end{minipage} & \begin{minipage}[t]{0.12\columnwidth}\raggedright\strut
3.61 (m)\strut
\end{minipage}\tabularnewline
\begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
10 (\selectlanguage{greek}β\selectlanguage{english}\textsubscript{2})\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
64.3\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
4.59 (vs)\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
4.29 (m)\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
4.04 (m)\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
3.88 (m)\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
3.70 (m)\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
-\strut
\end{minipage}\tabularnewline
\begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
20 (\selectlanguage{greek}β\selectlanguage{english}\textsubscript{2})\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
64.5\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
4.61 (vs)\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
4.30 (m)\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
4.04 (m)\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
3.88 (m)\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
3.70 (m)\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
-\strut
\end{minipage}\tabularnewline
\begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
30 (\selectlanguage{greek}β\selectlanguage{english}\textsubscript{2})\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
65.3\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
4.62 (vs)\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
4.29 (m)\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
4.06 (m)\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
3.91 (m)\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
3.71 (m)\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
-\strut
\end{minipage}\tabularnewline
\begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
40 (\selectlanguage{greek}β\selectlanguage{english}\textsubscript{2})\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
64.8\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
4.60 (vs)\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
4.27 (w)\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
4.04 (m)\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
3.90 (m)\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
3.71 (m)\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
-\strut
\end{minipage}\tabularnewline
\begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
50 (\selectlanguage{greek}β\selectlanguage{english}\textsubscript{2})\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
63.6\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
4.58 (vs)\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
4.25 (w)\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
4.03 (m)\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
3.88 (m)\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
3.69 (m)\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
-\strut
\end{minipage}\tabularnewline
\begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
60 (\selectlanguage{greek}β\selectlanguage{english}\textsubscript{2})\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
63.7\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
4.59 (vs)\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
4.29 (w)\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
4.04 (m)\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
3.88 (m)\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
3.71 (m)\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
-\strut
\end{minipage}\tabularnewline
\begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
70 (\selectlanguage{greek}β\selectlanguage{english}\textsubscript{2})\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
62.9\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
4.57 (vs)\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
4.27 (w)\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
4.02 (m)\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
3.86 (m)\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
3.69 (m)\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
-\strut
\end{minipage}\tabularnewline
\begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
80 (\selectlanguage{greek}β\selectlanguage{english}\textsubscript{2})\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
62.4\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
4.57 (vs)\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
4.26 (w)\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
4.04 (m)\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
3.84 (m)\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
3.70 (m)\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
-\strut
\end{minipage}\tabularnewline
\begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
90 (\selectlanguage{greek}β\selectlanguage{english}\textsubscript{2})\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
62.3\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
4.58 (vs)\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
4.26 (w)\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
4.05 (m)\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
3.88 (m)\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
3.70 (m)\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
-\strut
\end{minipage}\tabularnewline
\begin{minipage}[t]{0.12\columnwidth}\raggedright\strut
100 (pseudo-\selectlanguage{greek}β\selectlanguage{english}'\textsubscript{1} + \selectlanguage{greek}β\selectlanguage{english}\textsubscript{2})\strut
\end{minipage} & \begin{minipage}[t]{0.12\columnwidth}\raggedright\strut
40.0\strut
\end{minipage} & \begin{minipage}[t]{0.12\columnwidth}\raggedright\strut
4.57 (s)\strut
\end{minipage} & \begin{minipage}[t]{0.12\columnwidth}\raggedright\strut
4.27 (s)\strut
\end{minipage} & \begin{minipage}[t]{0.12\columnwidth}\raggedright\strut
4.16 (w)\strut
\end{minipage} & \begin{minipage}[t]{0.12\columnwidth}\raggedright\strut
3.95 (s)\strut
\end{minipage} & \begin{minipage}[t]{0.12\columnwidth}\raggedright\strut
3.73 (m)\strut
\end{minipage} & \begin{minipage}[t]{0.12\columnwidth}\raggedright\strut
-\strut
\end{minipage}\tabularnewline
\bottomrule
\end{longtable}

*vs, s, m, and w represent ''very strong'', ''strong'', ''medium'' and
''weak'' peak intensities.

Table 3- Small and wide-angle powder X-ray diffraction data for the
different crystal polymorphic forms of fractionated pequi oil and
Kpangnan butter binary mixtures after 60 days of storage\selectlanguage{english}
\begin{longtable}[]{@{}llllllll@{}}
\toprule
\begin{minipage}[b]{0.10\columnwidth}\raggedright\strut
Fractionated Pequi oil (\%)\strut
\end{minipage} & \begin{minipage}[b]{0.10\columnwidth}\raggedright\strut
Long-spacing (\selectlanguage{ngerman}Å)\strut
\end{minipage} & \begin{minipage}[b]{0.10\columnwidth}\raggedright\strut
Short-spacing (\selectlanguage{ngerman}Å)*\strut
\end{minipage} & \begin{minipage}[b]{0.10\columnwidth}\raggedright\strut
Short-spacing (\selectlanguage{ngerman}Å)*\strut
\end{minipage} & \begin{minipage}[b]{0.10\columnwidth}\raggedright\strut
Short-spacing (\selectlanguage{ngerman}Å)*\strut
\end{minipage} & \begin{minipage}[b]{0.10\columnwidth}\raggedright\strut
Short-spacing (\selectlanguage{ngerman}Å)*\strut
\end{minipage} & \begin{minipage}[b]{0.10\columnwidth}\raggedright\strut
Short-spacing (\selectlanguage{ngerman}Å)*\strut
\end{minipage} & \begin{minipage}[b]{0.10\columnwidth}\raggedright\strut
Short-spacing (\selectlanguage{ngerman}Å)*\strut
\end{minipage}\tabularnewline
\midrule
\endhead
\begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
0 (\selectlanguage{greek}β\selectlanguage{english}\textsubscript{2})\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
65.1\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
4.60 (vs)\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
4.01 (m)\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
3.89 (m)\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
3.78 (m)\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
3.69 (m)\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
3.58 (w)\strut
\end{minipage}\tabularnewline
\begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
10 (\selectlanguage{greek}β\selectlanguage{english}\textsubscript{1})\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
64.9\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
4.58 (vs)\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
4.01 (m)\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
3.89 (m)\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
3.73 (s)\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
3.69 (s)\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
3.59 (w)\strut
\end{minipage}\tabularnewline
\begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
20 (\selectlanguage{greek}β\selectlanguage{english}\textsubscript{1})\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
64.7\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
4.59 (vs)\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
4.06 (m)\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
3.90 (m)\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
3.72 (s)\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
3.69 (s)\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
3.59 (w)\strut
\end{minipage}\tabularnewline
\begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
30 (\selectlanguage{greek}β\selectlanguage{english}\textsubscript{1})\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
64.1\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
4.57 (vs)\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
4.03 (m)\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
3.89 (m)\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
3.72 (s)\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
3.68 (s)\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
3.58 (m)\strut
\end{minipage}\tabularnewline
\begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
40 (\selectlanguage{greek}β\selectlanguage{english}\textsubscript{1})\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
64.6\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
4.59 (vs)\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
4.05 (m)\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
3.90 (m)\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
3.74 (s)\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
3.69 (s)\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
3.58 (m)\strut
\end{minipage}\tabularnewline
\begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
50 (\selectlanguage{greek}β\selectlanguage{english}\textsubscript{1})\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
63.8\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
4.58 (vs)\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
4.04 (m)\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
3.88 (m)\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
3.73 (s)\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
3.68 (s)\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
3.56 (m)\strut
\end{minipage}\tabularnewline
\begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
60 (\selectlanguage{greek}β\selectlanguage{english}\textsubscript{1})\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
63.7\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
4.59 (vs)\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
4.03 (m)\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
3.87 (m)\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
3.74 (s)\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
3.69 (s)\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
3.56 (m)\strut
\end{minipage}\tabularnewline
\begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
70 (\selectlanguage{greek}β\selectlanguage{english}\textsubscript{1})\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
63.3\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
4.60 (vs)\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
4.04 (m)\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
3.86 (m)\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
3.75 (s)\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
3.70 (s)\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
3.56 (m)\strut
\end{minipage}\tabularnewline
\begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
80 (\selectlanguage{greek}β\selectlanguage{english}\textsubscript{1})\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
62.9\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
4.59 (vs)\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
4.05 (m)\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
3.86 (m)\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
3.74 (s)\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
3.69 (s)\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
3.56 (m)\strut
\end{minipage}\tabularnewline
\begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
90 (\selectlanguage{greek}β\selectlanguage{english}\textsubscript{1})\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
61.4\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
4.57 (vs)\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
4.07 (m)\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
3.85 (m)\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
3.73 (s)\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
3.69 (s)\strut
\end{minipage} & \begin{minipage}[t]{0.10\columnwidth}\raggedright\strut
3.56 (m)\strut
\end{minipage}\tabularnewline
\begin{minipage}[t]{0.12\columnwidth}\raggedright\strut
100 (pseudo-\selectlanguage{greek}β\selectlanguage{english}'\textsubscript{1})\strut
\end{minipage} & \begin{minipage}[t]{0.12\columnwidth}\raggedright\strut
41.9\strut
\end{minipage} & \begin{minipage}[t]{0.12\columnwidth}\raggedright\strut
4.30 (s)\strut
\end{minipage} & \begin{minipage}[t]{0.12\columnwidth}\raggedright\strut
4.21 (m)\strut
\end{minipage} & \begin{minipage}[t]{0.12\columnwidth}\raggedright\strut
4.15 (m)\strut
\end{minipage} & \begin{minipage}[t]{0.12\columnwidth}\raggedright\strut
3.97 (vs)\strut
\end{minipage} & \begin{minipage}[t]{0.12\columnwidth}\raggedright\strut
3.51 (w)\strut
\end{minipage} & \begin{minipage}[t]{0.12\columnwidth}\raggedright\strut
-\strut
\end{minipage}\tabularnewline
\bottomrule
\end{longtable}

*vs, s, m, and w represent ''very strong'', ''strong'', ''medium'' and
''weak'' peak intensities.\selectlanguage{english}
\begin{figure}[H]
\begin{center}
\includegraphics[width=0.70\columnwidth]{figures/image1/image1}

\end{center}
\end{figure}

Figure 1- Small- and wide-angle powder X-ray diffraction spectra of (A)
100\% FKB after 4 days, (B) 50:50 blend of FKB:FPO after 4 days, (C)
100\% FPO after 4 days, (D) 100\% FKB after 12 days, (E) 50:50 blend of
FKB:FPO after 12 days, and (F) 100\% FPO after 12 days storage at room
temperature.\selectlanguage{english}
\begin{figure}[H]
\begin{center}
\includegraphics[width=0.70\columnwidth]{figures/image2/image2}

\end{center}
\end{figure}

Figure 2- Small- and wide-angle powder X-ray diffraction spectra of (A)
100\% FKB after 60 days, (B) 50:50 blend of FKB:FPO after 60 days, and
(C) 100\% FPO after 60 days storage at room temperature.

Melting profile

The thermal properties of fractionated pequi oil mixed with fractionated
Kpangnan butter at different ratios and storage times at room
temperature are shown in Table 4 and Fig.3. The X-ray diffraction
analysis showed that after four days of static crystallization at room
temperature, the crystal polymorphic transition was not complete except
for fractionated 80:20 and 90:10 (\%w/w) pequi oil: fractionated
Kpangnan butter, which had significantly higher melting points (Fig. 1).
Since crystallization of the blends after four days of storage was not
complete, different mixtures of metastable crystal forms were observed,
making the interpretation of melting profiles difficult. However, after
12 days of storage, all blends were in the \selectlanguage{greek}β\selectlanguage{english}\textsubscript{2}polymorphic
form, with melting peaks between 32.6 \textsuperscript{o}C to 42.1
\textsuperscript{o}C, which potentially made them a promising CBE for
addition to CB to make chocolate. Moreover, blends containing 70\% to
90\% fractionated pequi oil could be directly used as a 100\% cocoa
butter alternative in compound chocolate formulations.

Table 4- Melting points (\selectlanguage{ngerman}°C) and enthalpies of fusion (J/g) for
fractionated pequi oil (FPO) and fractionated Kpangnan butter (FKB) and
their mixtures (w/w) after 4, 12, and 60 days of storage at
22\textsuperscript{o}C. Values represent the means and standard
deviations of n=2 replicates.\selectlanguage{english}
\begin{longtable}[]{@{}llllllll@{}}
\toprule
FPO (\%) & FKB (\%) & Melting point (\selectlanguage{ngerman}°C) & Enthalpy (J/g) & Melting
point (\selectlanguage{ngerman}°C) & Enthalpy (J/g) & Melting point (\selectlanguage{ngerman}°C) & Enthalpy
(J/g)\tabularnewline
\midrule
\endhead
& & 4 days & 4 days & 12 days & 12 days & 60 days & 60
days\tabularnewline
0 & 100 & 38.20\selectlanguage{ngerman}±0.91 & 127.45\selectlanguage{ngerman}±8.13 & 38.40\selectlanguage{ngerman}±0.42 & 138.90\selectlanguage{ngerman}±3.54 &
42.82\selectlanguage{ngerman}±0.08 & 194.7\selectlanguage{ngerman}±4.67\tabularnewline
10 & 90 & 39.90\selectlanguage{ngerman}±1.47 & 116.20\selectlanguage{ngerman}±10.89 & 43.14\selectlanguage{ngerman}±0.20 & 182.40\selectlanguage{ngerman}±2.69 &
43.01\selectlanguage{ngerman}±0.17 & 169.4\selectlanguage{ngerman}±2.69\tabularnewline
20 & 80 & 37.14\selectlanguage{ngerman}±0.14 & 104.92\selectlanguage{ngerman}±15.96 & 41.98\selectlanguage{ngerman}±0.38 & 160.65\selectlanguage{ngerman}±3.32 &
42.00\selectlanguage{ngerman}±0.11 & 157.35\selectlanguage{ngerman}±7.85\tabularnewline
30 & 70 & 41.89\selectlanguage{ngerman}±0.04 & 126.40\selectlanguage{ngerman}±9.33 & 41.76\selectlanguage{ngerman}±0.28 & 140.85\selectlanguage{ngerman}±3.61 &
41.02\selectlanguage{ngerman}±0.41 & 140.50\selectlanguage{ngerman}±0.57\tabularnewline
40 & 60 & 34.84\selectlanguage{ngerman}±0.05 & 71.38\selectlanguage{ngerman}±0.54 & 40.05\selectlanguage{ngerman}±0.13 & 130.80\selectlanguage{ngerman}±3.82 &
40.03\selectlanguage{ngerman}±0.28 & 105.35\selectlanguage{ngerman}±3.46\tabularnewline
50 & 50 & 33.52\selectlanguage{ngerman}±0.50 & 59.48\selectlanguage{ngerman}±7.69 & 38.35\selectlanguage{ngerman}±0.18 & 126.75\selectlanguage{ngerman}±0.35 &
37.92\selectlanguage{ngerman}±0.18 & 122.9\selectlanguage{ngerman}±8.34\tabularnewline
60 & 40 & 32.19\selectlanguage{ngerman}±0.49 & 49.74\selectlanguage{ngerman}±3.21 & 36.50\selectlanguage{ngerman}±0.47 & 115.20\selectlanguage{ngerman}±0.57 &
35.88\selectlanguage{ngerman}±0.12 & 109.45\selectlanguage{ngerman}±2.47\tabularnewline
70 & 30 & 30.89\selectlanguage{ngerman}±0.62 & 28.47\selectlanguage{ngerman}±4.14 & 33.44\selectlanguage{ngerman}±0.36 & 90.43\selectlanguage{ngerman}±1.37 & 34.27\selectlanguage{ngerman}±0.32
& 94.68\selectlanguage{ngerman}±3.98\tabularnewline
80 & 20 & 33.32\selectlanguage{ngerman}±0.11 & 14.72\selectlanguage{ngerman}±3.27 & 32.91\selectlanguage{ngerman}±0.28 & 77.10\selectlanguage{ngerman}±4.25 & 32.67\selectlanguage{ngerman}±0.22
& 76.12\selectlanguage{ngerman}±5.48\tabularnewline
90 & 10 & 31.59\selectlanguage{ngerman}±0.42 & 11.41\selectlanguage{ngerman}±1.29 & 32.61\selectlanguage{ngerman}±0.18 & 70.68\selectlanguage{ngerman}±1.22 & 31.99\selectlanguage{ngerman}±1.15
& 64.65\selectlanguage{ngerman}±8.08\tabularnewline
100 & 0 & 29.59\selectlanguage{ngerman}±0.27 & 20.73\selectlanguage{ngerman}±1.13 & 29.52\selectlanguage{ngerman}±0.66 & 69.62\selectlanguage{ngerman}±11.60 &
28.93\selectlanguage{ngerman}±0.58 & 30.60\selectlanguage{ngerman}±5.76\tabularnewline
\bottomrule
\end{longtable}\selectlanguage{ngerman}\selectlanguage{english}
\begin{figure}[H]
\begin{center}
\includegraphics[width=0.70\columnwidth]{figures/image3/image3}

\end{center}
\end{figure}

Figure 3- Peak melting temperature (\textsuperscript{o}C) of mixtures of
fractionated pequi oil and fractionated Kpangnan butter at different
proportions (w/w) after static crystallization in 4, 12, and 60 days of
storage at room temperature (22\textsuperscript{o}C)

Molecular composition and phase behavior

The TAG composition of fractionated pequi oil mixed with fractionated
Kpangnan butter (w/w) is shown in Table 5. The main TAGs in 100\% dry
fractionated pequi oil were POP (37\%) and POO (21\%), while SOS (90\%)
was the major TAG in 100\% solvent fractionated Kpangnan butter.
Multi-step solvent fractionation was more efficient for increasing the
amount of symmetrical TAG (SOS) in fractionated Kpangnan butter
(increasing from 52\% before fractionation to 90\% after fractionation).
In contrast, the single-step dry fractionation of pequi oil at
20\textsuperscript{o}C only resulted in an increase in the amount of POP
from 33.7\% to 36.7\% but did significantly decrease POO content from
38.7\% to 21.9\%.

The amount of POS (the main TAG in cocoa butter) in all fractionated
pequi oil-fractionated Kpangnan butter mixtures remained constant
(\textasciitilde{} 5\%). While SOS was the main TAG in mixtures
containing 10\% to 70\% fractionated pequi oil, POP was the major
symmetrical TAG for the rest of the mixtures (80\% and 90\%). van
Malssen, Peschar, Brito \& Schenk (1996) showed that symmetrical
mono-unsaturated triacylglycerols (POP, POS, and SOS) comprised 70\% to
88\% of total TAGs present in cocoa butter. In our study, we found the
total amount of symmetrical TAGs only in fractionated blends containing
10\% to 60\% (w/w) fractionated pequi oil was in the range of total
symmetrical TAGs of cocoa butter. The high melting point of binary
blends containing 10\% to 60\% (w/w) fractionated pequi oilcan be
explained by the high amount of SOS in these mixtures (84\% to 43\%,
respectively). These mixtures have a great potential to be categorized
as cocoa butter improvers (CBIs). Cocoa butter mixed with CBIs had
better heat resistance and bloom development properties at temperatures
higher than ambient temperature (Lipp and Anklam,1998); Timms, 2003).
For the binary mixtures containing 70\% to 100\% fractionated pequi oil,
the high amount of low melting TAGs (OOO, POO, and SOO) resulted in a
lower melting point at all storage times (4, 12, and 60 days).

Timms (2003) reported a blend of solvent fractionated palm oil and
illipe butter was successfully used to produce cocoa butter equivalent
(CBE). For the past 75 years, commercial CBEs in the market continue to
be made in the same way, namely by blending palm mid-fraction (PMF) as a
source of POP, with a high SOS fat such as shea butter, shea stearin,
sal fat, or kokum butter (De Clercq, Kadivar, Van de Walle, De
Pelsmaeker, Ghellynck \& Dewettinck, 2017).

Table 5- The main triacylglycerol composition of fractionated pequi oil
(FPO) and fractionated Kpangnan butter (FKB) and their mixtures (\%)\selectlanguage{english}
\begin{longtable}[]{@{}lllllllll@{}}
\toprule
\begin{minipage}[b]{0.11\columnwidth}\raggedright\strut
FPO (\%)\strut
\end{minipage} & \begin{minipage}[b]{0.11\columnwidth}\raggedright\strut
FKB (\%)\strut
\end{minipage} & \begin{minipage}[b]{0.11\columnwidth}\raggedright\strut
OOO\strut
\end{minipage} & \begin{minipage}[b]{0.11\columnwidth}\raggedright\strut
POO\strut
\end{minipage} & \begin{minipage}[b]{0.11\columnwidth}\raggedright\strut
POP\strut
\end{minipage} & \begin{minipage}[b]{0.11\columnwidth}\raggedright\strut
SOO\strut
\end{minipage} & \begin{minipage}[b]{0.11\columnwidth}\raggedright\strut
POS\strut
\end{minipage} & \begin{minipage}[b]{0.11\columnwidth}\raggedright\strut
SOS\strut
\end{minipage} & \begin{minipage}[b]{0.11\columnwidth}\raggedright\strut
Total POP+POS+SOS\strut
\end{minipage}\tabularnewline
\midrule
\endhead
\begin{minipage}[t]{0.08\columnwidth}\raggedright\strut
0\strut
\end{minipage} & \begin{minipage}[t]{0.08\columnwidth}\raggedright\strut
100\strut
\end{minipage} & \begin{minipage}[t]{0.08\columnwidth}\raggedright\strut
0.33\selectlanguage{ngerman}±0.12\strut
\end{minipage} & \begin{minipage}[t]{0.08\columnwidth}\raggedright\strut
0.30\selectlanguage{ngerman}±0.05\strut
\end{minipage} & \begin{minipage}[t]{0.08\columnwidth}\raggedright\strut
nd\strut
\end{minipage} & \begin{minipage}[t]{0.08\columnwidth}\raggedright\strut
2.63\selectlanguage{ngerman}±0.33\strut
\end{minipage} & \begin{minipage}[t]{0.08\columnwidth}\raggedright\strut
5.41\selectlanguage{ngerman}±0.03\strut
\end{minipage} & \begin{minipage}[t]{0.08\columnwidth}\raggedright\strut
89.65\selectlanguage{ngerman}±0.49\strut
\end{minipage} & \begin{minipage}[t]{0.08\columnwidth}\raggedright\strut
95.06\strut
\end{minipage}\tabularnewline
\begin{minipage}[t]{0.08\columnwidth}\raggedright\strut
10\strut
\end{minipage} & \begin{minipage}[t]{0.08\columnwidth}\raggedright\strut
90\strut
\end{minipage} & \begin{minipage}[t]{0.08\columnwidth}\raggedright\strut
0.38\selectlanguage{ngerman}±0.04\strut
\end{minipage} & \begin{minipage}[t]{0.08\columnwidth}\raggedright\strut
2.52\selectlanguage{ngerman}±0.07\strut
\end{minipage} & \begin{minipage}[t]{0.08\columnwidth}\raggedright\strut
4.29\selectlanguage{ngerman}±0.06\strut
\end{minipage} & \begin{minipage}[t]{0.08\columnwidth}\raggedright\strut
1.17\selectlanguage{ngerman}±0.05\strut
\end{minipage} & \begin{minipage}[t]{0.08\columnwidth}\raggedright\strut
5.16\selectlanguage{ngerman}±0.06\strut
\end{minipage} & \begin{minipage}[t]{0.08\columnwidth}\raggedright\strut
83.96\selectlanguage{ngerman}±2.17\strut
\end{minipage} & \begin{minipage}[t]{0.08\columnwidth}\raggedright\strut
93.43\strut
\end{minipage}\tabularnewline
\begin{minipage}[t]{0.08\columnwidth}\raggedright\strut
20\strut
\end{minipage} & \begin{minipage}[t]{0.08\columnwidth}\raggedright\strut
80\strut
\end{minipage} & \begin{minipage}[t]{0.08\columnwidth}\raggedright\strut
0.81\selectlanguage{ngerman}±0.09\strut
\end{minipage} & \begin{minipage}[t]{0.08\columnwidth}\raggedright\strut
4.13\selectlanguage{ngerman}±0.01\strut
\end{minipage} & \begin{minipage}[t]{0.08\columnwidth}\raggedright\strut
7.97\selectlanguage{ngerman}±0.02\strut
\end{minipage} & \begin{minipage}[t]{0.08\columnwidth}\raggedright\strut
1.20\selectlanguage{ngerman}±0.00\strut
\end{minipage} & \begin{minipage}[t]{0.08\columnwidth}\raggedright\strut
4.86\selectlanguage{ngerman}±0.23\strut
\end{minipage} & \begin{minipage}[t]{0.08\columnwidth}\raggedright\strut
75.48\selectlanguage{ngerman}±0.11\strut
\end{minipage} & \begin{minipage}[t]{0.08\columnwidth}\raggedright\strut
88.30\strut
\end{minipage}\tabularnewline
\begin{minipage}[t]{0.08\columnwidth}\raggedright\strut
30\strut
\end{minipage} & \begin{minipage}[t]{0.08\columnwidth}\raggedright\strut
70\strut
\end{minipage} & \begin{minipage}[t]{0.08\columnwidth}\raggedright\strut
1.04\selectlanguage{ngerman}±0.01\strut
\end{minipage} & \begin{minipage}[t]{0.08\columnwidth}\raggedright\strut
5.35\selectlanguage{ngerman}±0.11\strut
\end{minipage} & \begin{minipage}[t]{0.08\columnwidth}\raggedright\strut
11.52\selectlanguage{ngerman}±0.04\strut
\end{minipage} & \begin{minipage}[t]{0.08\columnwidth}\raggedright\strut
0.97\selectlanguage{ngerman}±0.99\strut
\end{minipage} & \begin{minipage}[t]{0.08\columnwidth}\raggedright\strut
4.97\selectlanguage{ngerman}±0.09\strut
\end{minipage} & \begin{minipage}[t]{0.08\columnwidth}\raggedright\strut
68.17\selectlanguage{ngerman}±0.16\strut
\end{minipage} & \begin{minipage}[t]{0.08\columnwidth}\raggedright\strut
84.65\strut
\end{minipage}\tabularnewline
\begin{minipage}[t]{0.08\columnwidth}\raggedright\strut
40\strut
\end{minipage} & \begin{minipage}[t]{0.08\columnwidth}\raggedright\strut
60\strut
\end{minipage} & \begin{minipage}[t]{0.08\columnwidth}\raggedright\strut
1.41\selectlanguage{ngerman}±0.13\strut
\end{minipage} & \begin{minipage}[t]{0.08\columnwidth}\raggedright\strut
7.57\selectlanguage{ngerman}±0.07\strut
\end{minipage} & \begin{minipage}[t]{0.08\columnwidth}\raggedright\strut
16.46\selectlanguage{ngerman}±0.01\strut
\end{minipage} & \begin{minipage}[t]{0.08\columnwidth}\raggedright\strut
0.85\selectlanguage{ngerman}±0.19\strut
\end{minipage} & \begin{minipage}[t]{0.08\columnwidth}\raggedright\strut
5.08\selectlanguage{ngerman}±0.01\strut
\end{minipage} & \begin{minipage}[t]{0.08\columnwidth}\raggedright\strut
61.55\selectlanguage{ngerman}±0.45\strut
\end{minipage} & \begin{minipage}[t]{0.08\columnwidth}\raggedright\strut
83.09\strut
\end{minipage}\tabularnewline
\begin{minipage}[t]{0.08\columnwidth}\raggedright\strut
50\strut
\end{minipage} & \begin{minipage}[t]{0.08\columnwidth}\raggedright\strut
50\strut
\end{minipage} & \begin{minipage}[t]{0.08\columnwidth}\raggedright\strut
1.79\selectlanguage{ngerman}±0.09\strut
\end{minipage} & \begin{minipage}[t]{0.08\columnwidth}\raggedright\strut
9.11\selectlanguage{ngerman}±0.04\strut
\end{minipage} & \begin{minipage}[t]{0.08\columnwidth}\raggedright\strut
20.23\selectlanguage{ngerman}±0.07\strut
\end{minipage} & \begin{minipage}[t]{0.08\columnwidth}\raggedright\strut
0.93\selectlanguage{ngerman}±0.04\strut
\end{minipage} & \begin{minipage}[t]{0.08\columnwidth}\raggedright\strut
4.88\selectlanguage{ngerman}±0.09\strut
\end{minipage} & \begin{minipage}[t]{0.08\columnwidth}\raggedright\strut
50.64\selectlanguage{ngerman}±0.22\strut
\end{minipage} & \begin{minipage}[t]{0.08\columnwidth}\raggedright\strut
75.74\strut
\end{minipage}\tabularnewline
\begin{minipage}[t]{0.08\columnwidth}\raggedright\strut
60\strut
\end{minipage} & \begin{minipage}[t]{0.08\columnwidth}\raggedright\strut
40\strut
\end{minipage} & \begin{minipage}[t]{0.08\columnwidth}\raggedright\strut
2.21\selectlanguage{ngerman}±0.21\strut
\end{minipage} & \begin{minipage}[t]{0.08\columnwidth}\raggedright\strut
11.02\selectlanguage{ngerman}±0.02\strut
\end{minipage} & \begin{minipage}[t]{0.08\columnwidth}\raggedright\strut
25.26\selectlanguage{ngerman}±0.55\strut
\end{minipage} & \begin{minipage}[t]{0.08\columnwidth}\raggedright\strut
0.94\selectlanguage{ngerman}±0.02\strut
\end{minipage} & \begin{minipage}[t]{0.08\columnwidth}\raggedright\strut
4.94\selectlanguage{ngerman}±0.00\strut
\end{minipage} & \begin{minipage}[t]{0.08\columnwidth}\raggedright\strut
42.75\selectlanguage{ngerman}±0.16\strut
\end{minipage} & \begin{minipage}[t]{0.08\columnwidth}\raggedright\strut
72.95\strut
\end{minipage}\tabularnewline
\begin{minipage}[t]{0.08\columnwidth}\raggedright\strut
70\strut
\end{minipage} & \begin{minipage}[t]{0.08\columnwidth}\raggedright\strut
30\strut
\end{minipage} & \begin{minipage}[t]{0.08\columnwidth}\raggedright\strut
2.77\selectlanguage{ngerman}±0.19\strut
\end{minipage} & \begin{minipage}[t]{0.08\columnwidth}\raggedright\strut
13.09\selectlanguage{ngerman}±0.45\strut
\end{minipage} & \begin{minipage}[t]{0.08\columnwidth}\raggedright\strut
28.02\selectlanguage{ngerman}±0.74\strut
\end{minipage} & \begin{minipage}[t]{0.08\columnwidth}\raggedright\strut
0.99\selectlanguage{ngerman}±0.04\strut
\end{minipage} & \begin{minipage}[t]{0.08\columnwidth}\raggedright\strut
4.62\selectlanguage{ngerman}±0.18\strut
\end{minipage} & \begin{minipage}[t]{0.08\columnwidth}\raggedright\strut
33.61\selectlanguage{ngerman}±1.02\strut
\end{minipage} & \begin{minipage}[t]{0.08\columnwidth}\raggedright\strut
66.24\strut
\end{minipage}\tabularnewline
\begin{minipage}[t]{0.08\columnwidth}\raggedright\strut
80\strut
\end{minipage} & \begin{minipage}[t]{0.08\columnwidth}\raggedright\strut
20\strut
\end{minipage} & \begin{minipage}[t]{0.08\columnwidth}\raggedright\strut
4.35\selectlanguage{ngerman}±0.08\strut
\end{minipage} & \begin{minipage}[t]{0.08\columnwidth}\raggedright\strut
18.51\selectlanguage{ngerman}±0.45\strut
\end{minipage} & \begin{minipage}[t]{0.08\columnwidth}\raggedright\strut
32.92\selectlanguage{ngerman}±0.21\strut
\end{minipage} & \begin{minipage}[t]{0.08\columnwidth}\raggedright\strut
1.19\selectlanguage{ngerman}±0.04\strut
\end{minipage} & \begin{minipage}[t]{0.08\columnwidth}\raggedright\strut
4.63\selectlanguage{ngerman}±0.04\strut
\end{minipage} & \begin{minipage}[t]{0.08\columnwidth}\raggedright\strut
21.05\selectlanguage{ngerman}±0.04\strut
\end{minipage} & \begin{minipage}[t]{0.08\columnwidth}\raggedright\strut
58.59\strut
\end{minipage}\tabularnewline
\begin{minipage}[t]{0.08\columnwidth}\raggedright\strut
90\strut
\end{minipage} & \begin{minipage}[t]{0.08\columnwidth}\raggedright\strut
10\strut
\end{minipage} & \begin{minipage}[t]{0.08\columnwidth}\raggedright\strut
4.33\selectlanguage{ngerman}±0.13\strut
\end{minipage} & \begin{minipage}[t]{0.08\columnwidth}\raggedright\strut
19.69\selectlanguage{ngerman}±0.77\strut
\end{minipage} & \begin{minipage}[t]{0.08\columnwidth}\raggedright\strut
36.13\selectlanguage{ngerman}±1.09\strut
\end{minipage} & \begin{minipage}[t]{0.08\columnwidth}\raggedright\strut
1.24\selectlanguage{ngerman}±0.06\strut
\end{minipage} & \begin{minipage}[t]{0.08\columnwidth}\raggedright\strut
4.17\selectlanguage{ngerman}±0.14\strut
\end{minipage} & \begin{minipage}[t]{0.08\columnwidth}\raggedright\strut
9.19\selectlanguage{ngerman}±0.16\strut
\end{minipage} & \begin{minipage}[t]{0.08\columnwidth}\raggedright\strut
49.49\strut
\end{minipage}\tabularnewline
\begin{minipage}[t]{0.08\columnwidth}\raggedright\strut
100\strut
\end{minipage} & \begin{minipage}[t]{0.08\columnwidth}\raggedright\strut
0\strut
\end{minipage} & \begin{minipage}[t]{0.08\columnwidth}\raggedright\strut
4.49\selectlanguage{ngerman}±0.45\strut
\end{minipage} & \begin{minipage}[t]{0.08\columnwidth}\raggedright\strut
21.91\selectlanguage{ngerman}±0.93\strut
\end{minipage} & \begin{minipage}[t]{0.08\columnwidth}\raggedright\strut
36.72\selectlanguage{ngerman}±0.72\strut
\end{minipage} & \begin{minipage}[t]{0.08\columnwidth}\raggedright\strut
1.37\selectlanguage{ngerman}±0.08\strut
\end{minipage} & \begin{minipage}[t]{0.08\columnwidth}\raggedright\strut
3.82\selectlanguage{ngerman}±0.09\strut
\end{minipage} & \begin{minipage}[t]{0.08\columnwidth}\raggedright\strut
0.70\selectlanguage{ngerman}±0.02\strut
\end{minipage} & \begin{minipage}[t]{0.08\columnwidth}\raggedright\strut
41.23\strut
\end{minipage}\tabularnewline
\bottomrule
\end{longtable}

nd: not detected

Based on Fig. 3, the melting point of binary mixtures containing 30\%
and 80\% fractionated pequi oil showed an disproportionate increase in
their melting point after four days of storage at room temperature. To
better understand this phenomenon, the ternary phase diagram of
POP+POS+SOS mixtures in meta-stable polymorphic form (pseudo-\selectlanguage{greek}β\selectlanguage{english}')
(Ghazani \& Marangoni, 2021) was used to pinpoint the location of these
mixtures in the ternary plot (Fig. 4). The area with the symbols of *
and + show the location of mixtures containing 30\% and 80\%
fractionated pequi oil, respectively.\selectlanguage{english}
\begin{figure}[H]
\begin{center}
\includegraphics[width=0.70\columnwidth]{figures/image4/image4}

\end{center}
\end{figure}

Figure 4- Ternary melting phase diagram of static crystallized
POP+POS+SOS in pseudo-\selectlanguage{greek}β\selectlanguage{english}' crystal polymorphic form (adapted from Ghazani
\& Marangoni, 2021). The symbols * and + represents the amount of POP,
POS and SOS in 30\% and 80\% FPO after normalizing, respectively.

Lipp, Simoneau, Ulberth, Anklam, Crews, Brereton, \ldots{} \& Wiedmaier,
(2001) showed that commercial CBEs generally contain a lower amount of
POS, the same amount of SOS, and a higher amount of POP than CB. In our
previous study (Ghazani \& Marangoni, 2018), we reported the main TAG
profile of CB as POP 15\%, POS 39\%, and SOS 28\%. Binary mixtures
containing 70\% fractionated pequi oil, and 30\% fractionated Kpangnan
butter had a TAG composition of 28\% POP (higher than POP amount in CB),
4.6\% POS (lower than POS amount in CB), and 33\% SOS (equal amount than
CB). This mixture displayed melting points of 33 and
34\textsuperscript{o}C after 12 and 60 day storage, respectively, and
crystallized into a stable triclinic \selectlanguage{greek}β\selectlanguage{english}\textsubscript{2} form after 12
days at 22\textsuperscript{o}C. This particular binary mixture displayed
the most desirable solid-state characteristics and had potential for
being used as a commercial CBE.

\textbf{CONCLUSION}

A limited and shrinking supply for CB, combined with an increased
demand, has forced the food industry to look for alternatives to CB to
manufacture chocolate and confectionery products. Even though palm
kernel oil and hydrogenated palm oil fractions can be used a cocoa
butter equivalents and replacers, the current concerns about
sustainability have made these ingredients less desirable. In this
study, we have shown that it is possible to produce functional CBEs
containing no palm oil products from fractionated Kpangnan butter and
fractionated Pequi oil. The melting point and crystal structure of the
selected binary mixture containing 70\% fractionated Pequi and 30\%
Kpangnan butter suggest potential for this mixture as a commercial CBE.

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\begin{figure}[H]
\begin{center}
\includegraphics[width=0.70\columnwidth]{figures/Figure-1/Figure-1}

\end{center}
\end{figure}\selectlanguage{english}
\begin{figure}[H]
\begin{center}
\includegraphics[width=0.70\columnwidth]{figures/Figure-2/Figure-2}

\end{center}
\end{figure}\selectlanguage{english}
\begin{figure}[H]
\begin{center}
\includegraphics[width=0.70\columnwidth]{figures/Fig/Fig}

\end{center}
\end{figure}\selectlanguage{english}
\begin{figure}[H]
\begin{center}
\includegraphics[width=0.70\columnwidth]{figures/Fih/Fih}

\end{center}
\end{figure}

\selectlanguage{english}
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\end{document}

