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Article

Terminalia catappa Kernel Flour Characterization as a Functional


and Bioactive Ingredient for Cookies Formulation
Audrey Vingadassalon 1 , Ewa Pejcz 2 , Agata Wojciechowicz-Budzisz 2 , Remigiusz Ol˛edzki 2,3 ,
Kristy Groton 1,3 , Guylene Aurore 1,† and Joanna Harasym 2,3, *,†

1 Campus de Fouillole, Université des Antilles, COVACHIM M2E (EA 3592), UFR SEN, F-97110 Pointe-à-Pitre,
France; audrey.vingadassalon@univ-antilles.fr (A.V.); kristygroton@gmail.com (K.G.);
guylene.aurore@univ-antilles.fr (G.A.)
2 Department of Biotechnology and Food Analysis, Wroclaw University of Economics and Business,
Komandorska 118/120, 53-345 Wroclaw, Poland; ewa.pejcz@ue.wroc.pl (E.P.);
agata.wojciechowicz-budzisz@ue.wroc.pl (A.W.-B.); remigiusz.oledzki@ue.wroc.pl (R.O.)
3 Adaptive Food Systems Accelerator–Science Centre, Wroclaw University of Economics and Business,
Komandorska 118/120, 53-345 Wroclaw, Poland
* Correspondence: joanna.harasym@ue.wroc.pl
† Co-last authors. These authors contributed equally to this work.

Featured Application: This research demonstrates the potential of Terminalia catappa kernel flour
as a novel, sustainable ingredient in gluten-free cookie formulation, offering enhanced nutritional
value through significant antioxidant properties and dietary fiber content. The findings support the
valorization of this underutilized tropical resource in functional food development, particularly
in regions where T. catappa is abundant but currently underexploited.

Abstract: Terminalia catappa (tropical almond) represents an underutilized resource with potential
applications in functional food development. This study investigated the technological properties
and bioactive characteristics of T. catappa kernel flour and its application in cookie formulation.
The research examined the techno-functional properties, pasting behavior, and bioactive profile of
Citation: Vingadassalon, A.; Pejcz, E.; T. catappa flour and its blends with different sweeteners (erythritol and cane sugar at 5% and 15%
Wojciechowicz-Budzisz, A.; Ol˛edzki, concentrations). Cookies were formulated using optimized ingredients, and their quality parameters
R.; Groton, K.; Aurore, G.; Harasym, J. were evaluated through physical, chemical, and sensory analyses. T. catappa flour demonstrated
Terminalia catappa Kernel Flour significant water holding capacity (4.48 g H2 O/g DM) and notable antioxidant activity in both
Characterization as a Functional and aqueous and ethanolic extracts (DPPH: 1.95–3.35 mg TE/g DM). The addition of sweeteners influ-
Bioactive Ingredient for Cookies enced pasting properties, with higher concentrations generally reducing peak viscosity and pasting
Formulation. Appl. Sci. 2024, 14, 11201.
temperature. Developed cookies exhibited stable water activity (0.294–0.320) over one month of
https://doi.org/10.3390/app142311201
storage and contained substantial dietary fiber (5.018 g/100 g). Sensory evaluation revealed superior
Academic Editors: Lígia Pimentel and acceptability for thicker (10 mm) cookies, particularly in texture and appearance attributes. This study
Ana Fontes establishes T. catappa kernel flour as a promising functional ingredient for gluten-free bakery applica-
Received: 3 November 2024
tions, offering both technological functionality and bioactive properties suitable for health-conscious
Revised: 23 November 2024 product development.
Accepted: 27 November 2024
Published: 1 December 2024 Keywords: Terminalia catappa; tropical almond; seaside almond; Indian almond; Singapore almond;
gluten-free cookies; antioxidant activity; techno-functional properties; sustainable food development;
underutilized plant resources

Copyright: © 2024 by the authors.


Licensee MDPI, Basel, Switzerland.
This article is an open access article
1. Introduction
distributed under the terms and
conditions of the Creative Commons Adding value to natural resources and finding new sources of agri-food ingredients
Attribution (CC BY) license (https:// are crucial issues in the current context of sustainable development and diversification of
creativecommons.org/licenses/by/ food products, particularly in developing countries [1]. In the Caribbean islands, using local
4.0/). biodiversity resources as a substitute for imports is becoming increasingly important. Many

Appl. Sci. 2024, 14, 11201. https://doi.org/10.3390/app142311201 https://www.mdpi.com/journal/applsci


Appl. Sci. 2024, 14, 11201 2 of 19

resources have substantial nutritional characteristics but remain little known and, therefore,
little used due to the lack of studies on their use in agri-food processes. Moreover, increased
consumer interest in health issues has impacted the demand for sustainable products. As
a result, the food industry tends to adapt and innovate in product formulation [2,3]. As
a result, under-utilized fruits and vegetables and their waste products are the subjects of
increasing interest in developing flours, extracts, pharmaceutical substances, or flavors. In
addition, secondary plant metabolites, polyphenols, and phytochemicals in most tropical
plants, fruits, or vegetables are responsible for most host health benefits [4–6] and help to
preserve product quality, bringing health benefits [7].
The Terminalia catappa (T. catappa) tree, also known as the tropical almond, seaside
almond, Indian almond, or Singapore almond, belongs to the Combretaceae family. This
large tree species from India, Malaysia, and Australia has spread to many other countries,
tropical and subtropical regions of the world, and is widespread in tropical regions, partic-
ularly coastal areas. T. catappa has a widespread natural distribution in coastal areas near
the Indian Ocean, across tropical Asia to the Pacific Ocean [8,9]. It is difficult to determine
to what extent its distribution has been made, but it is assumed that it is due to human
movement and dispersal. Thus, the tropical almond tree has been introduced and natural-
ized in many tropical regions, including Brazil, the Caribbean, and East Africa [10]. The
tree can reach a height of 30 m, with leaves measuring between 8 and 30 cm long and 5 and
15 cm wide. Almost all the tree parts seem to be attractive for development. The red bark
is an elastic, cross-grained wood widely used to construct buildings, bridges, cardboard
boxes, etc. The trunk is one of the best sources of gum and resin. The kernels, known as
almonds, are eaten raw or roasted and appreciated for their taste, like that of traditional
almonds [11]. T. catappa is very widespread in the coastal regions of the Caribbean islands,
but its use remains very limited. Using its powder in developing areas could replace the
almond powders derived from Prunus dulcis almonds imported from Europe. Previous
studies have already described the characteristics of T. catappa and we propose using its
powder as a substitute in preparing pastries.
According to Chukwuma et al. [12], T. catappa kernels are attracting growing world-
wide interest due to their high nutritional value and phytochemical content, which is
beneficial to health. In Asia, it is considered a medicinal plant [13], and in African countries,
it is used to manufacture medicines due to its antifungal, anti-inflammatory, nephropro-
tective, and antibacterial action [14–16]. Moreover, according to another study conducted
by Le Hong Nguy [17] concerning the physicochemical, antibacterial, and antioxidant
properties of T. catappa seeds, the flavonoids and tannins present in T. catappa play a crucial
role in its anti-diabetic properties by acting as powerful antioxidants, thus reducing cellular
damage caused by free radicals. In addition, these compounds can enhance insulin action
and modulate signaling pathways associated with glucose metabolism. One study also
demonstrated the richness of the seeds in lipids, enabling the production of oil used in
cooking or animal feed [18].
Despite all this, T. catappa is still little used worldwide, as there are many gaps in
knowledge about its bioactive composition and properties [19]. In addition, this plant
is under-utilized in West Indies and South America and remains an ornamental tree. Its
fruits are rarely consumed and end up falling to the ground, generating organic waste and
undesirable environmental impacts [20]. This underutilization of T. catappa seeds motivated
this study to analyze its kernel powder’s techno-functional and rheological properties and
its antioxidative performance. The experiment evaluates the quality of cookie formulations
based on the T. catappa kernel flour, which provides a valuable insight for economical
exploitation directly as a food ingredient. The characterization of T. catappa almond flour
thus supports its use as an alternative in developing sustainable agri-food products that
are also widely consumed, such as shortbread cookies.
Appl. Sci. 2024, 14, 11201 3 of 19

2. Materials and Methods


2.1. Raw Material
Indian almond fruits (Terminalia catappa) were harvested from trees located in Capesterre-
Belle-Eau, Guadeloupe (West Indies), in a coastal area with sandy soil along the Atlantic
Ocean (15◦ 59′ 59.7′′ N 61◦ 36′ 11.2′′ W) (Figure S1). The endocarp and mesocarp were
removed from the T. catappa fruits to reach the kernels. Then the kernels were manually
cleaned and dried at 40 ◦ C for 48 h in a dryer (Biosec Pro 2200 W, Tauro Essiccatori,
Camisano Vincentino, Italy). The dried kernels were ground to a fine powder using an
electric grinder (Taurus Aromatic 150 W, Taurus Group, Oliana, Spain). The powders were
immediately vacuum-packed and stored under optimum conditions between −20 ◦ C and
room temperature until use.
The examined blends consisted of T. catappa kernel powder and two different
sweeteners—cane sugar and erythritol—in two shares of 5% and 10% (calculated per
100 g of T. catappa kernel powder used, e.g., 5 g/15 g of cane sugar/erythritol).

2.2. Techno-Functional Blend Characteristics


Moisture content was determined gravimetrically after drying the sample at 135 ◦ C in
the oven (SML, Zalmed, Łomianki, Poland), according to Official Method AAC44-19.01,
AACC 2000. The water absorption capacity (WAC), oil absorption capacity (OAC), and
hydrophilic/lipophilic index (HLI) of T. catappa powder blends were measured following
the protocol outlined elsewhere [21], with slight modifications. Briefly, the WAC was
determined by mixing 3 g of the sample with 30 mL of distilled water, while the OAC
was assessed by combining the sample with 30 mL of rapeseed oil in centrifuge tubes.
The dispersions were vortexed (Heidolph Reax, Schwabach, Germany) for 30 s, allowed
to rest, then centrifuged at 3000× g (Thermo Fisher Scientific, Waltham, MA, USA). The
supernatants were removed, and tubes were placed in an oven (Vindon Scientific, Rochdale,
UK) at 50 ◦ C to eliminate residual liquid. WAC and OAC values (g of liquid/g of dry
sample) were calculated as described previously [21]. The hydrophilic/lipophilic index
(HLI) was then determined by calculating the WAC/OAC ratio.
The water absorption index (WAI), reflecting sample gelatinization and entrapment
of small molecules within the matrix or their release into the supernatant, as well as the
water solubility index (WSI), which indicates the quantity of compounds released from
the gel, and swelling power (SP), were evaluated based on the method by Harasym et al.
(2020) [2], with minor adjustments. Each 3 g sample was dispersed in 30 mL distilled
water within pre-weighed centrifuge tubes and heated to 90 ◦ C for 10 min in a water bath
(MLL147, AJL Electronics, Kraków, Poland). After cooling to room temperature, samples
were centrifuged at 3000× g for 10 min, after which the sediment was weighed and the
supernatant transferred to pre-weighed Petri dishes for drying at 110 ◦ C for 24 h in an oven
(SML, Zalmed, Łomianki, Poland) to determine solid content. WAI (g water/g dry solid),
WSI (g water/100 g dry solid), and SP (g water/g dry solid) were calculated as described
by Harasym et al. (2020) [22].
Foaming capacity and stability (FC, FS) were evaluated according to Kaushal et al.
(2012) [23] with slight modifications. Briefly, the flour/blend (1 g) was dispersed in distilled
water (50 mL) in a graduated cylinder, tapped, and shaken vertically by hand for 5 min.
The initial and final volumes were noted, and the difference was expressed as FC [mL/g
DM]. Then the sample was left for 1 h, and the suspension volume was recorded. The foam
stability was calculated as [%] according to the following equation:

FS [%] = (V1H/V initial ) × 100 (1)

Emulsifying activity and stability (EA, ES) were measured as described by Kiiru et al.
(2024) [24] by combining the sample with water and oil, homogenizing the mixture, and
assessing the emulsion volume after centrifugation. Stability was further confirmed by
reheating and allowing the emulsion to settle.
Appl. Sci. 2024, 14, 11201 4 of 19

2.3. Pasting Properties


Pasting properties of T. catappa powder blends were evaluated across trials with
varying sweetener compositions. Measurements were conducted using a Rapid Visco
Analyser (RVA 4500, Perten Instruments, Waltham, MA, USA) following the AACC 76-21.01,
AACC 1999 method. Each trial followed a standardized temperature profile, beginning
with a holding phase at 50 ◦ C for 2 min, followed by a heating ramp from 50 ◦ C to 95 ◦ C at
a rate of 5 ◦ C/min. The samples were then held at 95 ◦ C for 5 min, cooled at 10 ◦ C/min
back to 50 ◦ C, and held for another 4 min. The parameters recorded included peak viscosity
(PV), trough viscosity (TV), breakdown viscosity (BV), final viscosity (FV), setback viscosity
(SV), peak time, and pasting temperature.

2.4. Bioactive Properties of Blends


2.4.1. Extraction
The extraction process was conducted according to the methodology outlined by
Ol˛edzki et al. (2022) [25], with some modifications. In brief, 1.5 g of each sample was
homogenized with 5 mL of acidified (1% HCl) water or ethanol for 1 min using a vortex
mixer (MX-S, Chemland, Stargard, Poland). Subsequently, the samples were agitated
at room temperature on a laboratory rotary shaker (MX-RD PRO, Chemland, Stargard,
Poland) for 2 h and then centrifuged at 3500× g and 4 ◦ C for 10 min (MPW-350, MPW MED.
INSTRUMENTS, Warsaw, Poland). The resulting supernatants were stored at 8 ◦ C until
further analysis. All spectrophotometric analyses were carried out using methodologies
previously described by Ol˛edzki et al. (2022) [25], with minor adjustments.

2.4.2. Reducing Sugars


To determine the reducing sugar content of the samples, 0.25 mL of DNS reagent
(3,5-dinitrosalicylic acid) was mixed thoroughly to 0.5 mL of each sample. The mixture was
then incubated in a boiling water bath for 5 min and cooled to 50–60 ◦ C. Following this,
3 mL of distilled water was added to the mixture, and the absorbance was measured at
530 nm. Glucose was the standard for generating the calibration curve, ranging from 100
to 800 µg/mL. The reducing sugar content was expressed as mg of glucose equivalent per
gram of sample dry weight (gDW).

2.4.3. Reduction of the Cationic Radical ABTS


The antiradical capacity of the samples was assessed using the ABTS+ (2,2-azo-bis
(3-ethyl benzothiazoline-6-sulfonic acid)) assay. Specifically, 0.0204 mL of each sample was
combined with 1.0 mL of a diluted ABTS+ solution, which was prepared according to the
method outlined by Ol˛edzki et al. (2022) [25]. The absorbance of the resulting mixture
was measured at 734 nm 10 s after the sample was mixed with the ABTS+ solution. Trolox
was the standard for generating the calibration curve, ranging from 100 to 800 µmol/L.
The antiradical capacity was reported as mg of Trolox equivalent (TE) per gram of sample
dry weight.

2.4.4. DPPH Assay


The antioxidant capacity of the samples was evaluated using the DPPH assay. In this
procedure, 0.0345 mL of each sample was combined with 1 mL of a 0.1 mM methanolic
DPPH (2,2-diphenyl-1-picrylhydrazyl radical) solution. The absorbance of the mixture was
recorded at 517 nm after a 20-min incubation period. Trolox was employed as a standard
to create the calibration curve, which ranged from 100 to 800 µmol/L. The antioxidant
capacity was reported as mg of Trolox equivalent (TE) per gram of sample dry weight.

2.4.5. Ferric Reducing Antioxidant Power (FRAP Assay)


To assess the Ferric Reducing Antioxidant Power (FRAP) of the samples, 0.0345 mL of
each sample was combined with 0.998 mL of a freshly prepared FRAP solution, as described
by Ol˛edzki et al. (2022) [25]. After a 15-min incubation, the absorbance of the mixture
Appl. Sci. 2024, 14, 11201 5 of 19

was measured at 593 nm. Ferrous sulfate (FeSO4 ) served as the standard for creating the
calibration curve, which ranged from 100 to 800 µmol/L. The FRAP values were reported
as mg of FeSO4 equivalent per gram of sample dry weight.

2.5. Fourier Transform Infrared Spectroscopy (FTIR) Analysis


FTIR spectra of the samples were obtained using a Fourier transform infrared (FTIR)
spectrophotometer (Nicolet 6700 FT-IR, Thermo Fisher Scientific, Waltham, MA, USA)
equipped with a diamond crystal cell for attenuated total reflection (ATR) operation. Each
sample was scanned 64 times across a wavelength range of 4000–400 cm−1 at a nominal
resolution of 4 cm−1 . Background correction was performed using the air spectrum to
ensure accurate measurements.

2.6. Cookies Formulation


The cookies were prepared using T. catappa flour as the primary base. Initial trials
using a combination of cane sugar and erythritol produced a salty, cracker-like flavor profile.
Therefore, maintaining the cane sugar within the previously set range, after a series of
preliminary baking trials, the final formulation was set and included 145 g of T. catappa flour,
45 g of water, 15 g of coconut oil, 20 g of honey, and 10 g of cane sugar. Incorporating honey
significantly enhanced the perception of sweetness and overall palatability of the cookies.
The optimal sweetener balance, combining 20 g of honey and 10 g of cane sugar,
was selected after multiple tests and is retained for future developments. The dough
preparation involved thoroughly mixing the T. catappa flour with the other ingredients to
form a cohesive dough.
Adjustments to the cookie thickness were also explored to optimize the sensory
qualities and baking consistency. Thicker cookies (10 mm) offered a rich texture and
mouthfeel, while thinner cookies (5 mm) delivered crispiness and enhanced aroma. Each
variation appeals to different consumer preferences. The dough was shaped into flat rounds
with the desired thickness (5 mm or 10 mm, depending on the test), ensuring uniform size
for even baking. The cookies were baked at 180 ◦ C for approximately 15 min, until the
edges turned lightly golden. After baking, the cookies were allowed to cool completely
before serving.

2.7. Quality Features of Cookies


2.7.1. Physicochemical Quality Features
The water activity (Aw) of the cookies was determined with an AquaLab 3TE analyzer
(Decagon Devices, Inc., Pullman, WA, USA). The hardness of the samples was assessed
using a three-point bending test. Specifically, a Texturemeter FC200STAV50 AXIS (Axis
Ltd., Gdansk, Poland) was employed. Each sample was positioned across two supports
set 8 cm apart, and a downward force was applied at the center by a wedge moving at a
rate of 150 mm/min. The hardness was quantified as the maximum force (N) needed to
fracture the sample.
The fiber content of the samples was analyzed based on AOAC Method 991.43, and
AACC Method 32-07.01, further adapted from the AACC total dietary fiber (TDF) method
32-05.01 and the soluble/insoluble dietary fiber method with additional modifications
made for this study [26].

2.7.2. Sensory Quality Features


Sensory analysis is essential for evaluating organoleptic properties and aligning new
agri-food products with consumer expectations. To resolve an internal preference discrep-
ancy regarding cookie thickness, a comparative assessment was conducted between two
samples: Sample A (thicker) and Sample B (thinner). A panel of 35 participants (57% fe-
male, 43% male) comprising students and teachers evaluated the samples based on sensory
criteria including appearance, smell, flavor, aftertaste, texture, and overall preference, using
a five-point scale from “Strongly Dislikes” to “Adores”.
Appl. Sci. 2024, 14, 11201 6 of 19

2.8. Statistical Analysis


All the analyses were performed in triplicate. The results are reported as means ±
standard deviations. The results’ variance (ANOVA and multifactor ANOVA) analysis
was evaluated with Statgraphics Centurion software (Centurion XVII.I version, StatPoint
Technologies, Inc., Warrenton, VA, USA). Analysis of variance (ANOVA) was conducted
for statistical significance, and Tukey’s HSD (honestly significant difference) test (α = 0.05)
was used to identify the significant difference of each sample type.

3. Results and Discussion


3.1. Functional Characteristics of T. catapa and Its Blends with Erythritol and Cane Sugar
The water and oil absorption characteristics of T. catappa flour and its blends with
erythritol and cane sugar are presented in Table 1.

Table 1. Absorptional characteristics of T. catappa and its erythritol and cane sugar blends.

Sample WHC WAC WAI SP WSI OAC HLI


g H2 O/g DM g H2 O/100 g DM g oil/g DM
4.48 ± 0.13 a b 3.31 ± 0.13 c b 14.69 ± 4.12 a 1.84 ± 0.02 a 1.47 ± 0.02 a
T. catappa 2.61 ± 0.02 3.95 ± 0.06
5-E 4.42 ± 0.25 a 2.65 ± 0.08 b 2.98 ± 0.06 b 3.83 ± 0.33 ab 21.10 ± 4.92 bc 1.85 ± 0.18 a 1.49 ± 0.21 a
15-E 4.39 ± 0.51 a 2.45 ± 0.06 ab 2.86 ± 0.02 ab 3.70 ± 0.05 ab 21.67 ± 0.88 bc 1.73 ± 0.37 a 1.51 ± 0.30 a
5-CS 4.29 ± 0.15 a 2.48 ± 0.18 ab 2.96 ± 0.03 b 3.63 ± 0.13 a 17.27 ± 1.89 ab 1.91 ± 0.13 a 1.35 ± 0.17 a
15-CS 4.20 ± 0.47 a 2.33 ± 0.17 a 2.81 ± 0.02 a 3.69 ± 0.05 ab 23.19 ± 0.86 c 1.61 ± 0.03 a 1.50 ± 0.10 a
E—erythritol, CS—cane sugar, 5 and 15 means 5 g and 15 g added per 100 g of T. catappa flour, WHC—water
holding capacity, WAC—water absorption capacity, OAC—oil absorption capacity, HLI—hydrophilic–lipophilic
index, WAI—water absorption index, WSI—water solubility index, SP—swelling power. Lowercase letters mean
significant differences in columns at p = 0.05.

The water holding capacity (WHC) values ranged from 4.20 ± 0.47 to 4.48 ± 0.13 g
H2 O/g DM, with the highest value observed for pure T. catappa powder. Adding erythritol
and cane sugar resulted in slight, though statistically insignificant (p > 0.05), decreases in
WHC values, probably caused by solubilizing of the sweeteners without capturing water
in the matrix.
Water absorption capacity (WAC) exhibited values between 2.33 ± 0.17 and 2.65 ± 0.08 g
H2 O/g DM. The 5% erythritol blend showed the highest WAC (2.65 ± 0.08), while the 15%
cane sugar blend demonstrated the lowest value (2.33 ± 0.17). The oil absorption capacity
(OAC) values were relatively consistent across all samples, ranging from 1.61 ± 0.03 to
1.91 ± 0.13 g oil/g DM, with no statistically significant differences.
The hydrophilic/lipophilic index (HLI) values remained stable across all samples,
ranging from 1.35 ± 0.17 to 1.51 ± 0.30, indicating that the addition of sweeteners did not
significantly affect the hydrophilic–lipophilic balance of the blends.
The water absorption index (WAI) showed a decreasing trend with increasing sweet-
ener content, with values ranging from 2.81 ± 0.02 to 3.31 ± 0.13 g H2 O/g DM. The highest
WAI was observed in pure T. catappa (3.31 ± 0.13), while the 15% cane sugar blend showed
the lowest value (2.81 ± 0.02).
Water solubility index (WSI) values varied from 14.69 ± 4.12 to 23.19 ± 0.86 g H2 O/100 g
DM, with the highest value observed in the 15% cane sugar blend. Swelling power (SP)
showed minimal variation across samples, ranging from 3.63 ± 0.13 to 3.95 ± 0.06 g H2 O/g
DM, with pure T. catappa exhibiting the highest value.
These results suggest that while adding sweeteners impacted the absorptional charac-
teristics of T. catappa powder, most changes were relatively modest, except the WSI, which
showed more pronounced variations with sweetener addition.
The water holding capacity (WHC) values (4.20–4.48) for T. catappa powder and its
blends demonstrate good water retention properties comparable to other nut flours. The
Appl. Sci. 2024, 14, 11201 7 of 19

Water absorption capacity (WAC) values ranging from 2.33 to 2.65 g/g are similar to
those reported by Pambou-Tobi et al. (2021) [27] for T. catappa seed flour. In the study by
Stefan et al. (2019) [28], adding sweeteners such as erythritol and stevia reduced the water
absorption of dough. The authors suggest the behavior occurs because sweeteners reduce
the content of protein and complex carbohydrates, which are responsible for binding water
in the dough; however, a more reasonable explanation suggests that the reduction in water
absorption is due to the sweeteners’ competition for water with proteins and complex
carbohydrates, rather than a direct reduction in their content within the dough.
The oil absorption capacity (OAC) values (1.61–1.91 g/g) suggest moderate lipid-
binding capabilities, which are essential for food applications. These values are comparable
to those in other tropical nut flours [29]. The high oil binding capacity of T. catappa is
confirmed by the results of Adedola et al. (2019) [30], where the oil absorption capacity
increased with increasing levels of T. catappa flour in blends.
The OAC in food is due to oil retention in the polar chains of proteins. The higher pro-
tein and fat content in T. catappa samples compared to 100% starch samples promoted more
lipid–lipid, lipid–protein interactions, resulting in a higher OAC. According to Otegbayo
et al. (2013) [31], the ability of proteins in a food sample to retain fat is an important quality
feature because fat acts as a flavor carrier and thus increases palatability.
The hydrophilic–lipophilic index (HLI) values (1.35–1.51) indicate balanced water and
oil binding properties, making the flour suitable for various food applications. The water
solubility index (WSI) values (14.69–23.19%) suggest good solubility characteristics, while
the swelling power (SP) values (3.63–3.95) indicate moderate swelling capacity, which is
advantageous for baked products.
The foaming and emulsification characteristics of T. catappa powder and its blends with
erythritol and cane sugar are presented in Table 2. Foaming capacity (FC) values slightly
decreased with increasing sweetener content, ranging from 51.73 ± 0.02 to 53.21 ± 0.73%.
The highest FC was observed in pure T. catappa (53.21 ± 0.73%), while the 15% cane sugar
blend showed the lowest value (51.73 ± 0.02%). The 5% erythritol and 5% cane sugar
blends exhibited intermediate values of 52.64 ± 0.01% and 52.39 ± 0.73%, respectively.

Table 2. Foaming and emulsification characteristics of T. catappa and its blends with erythritol and
cane sugar.

Samples FC [mL] FS [%] EA [%] ES [%]


a c 103.2 ± 3.1 a
T. catappa 53.21 ± 0.73 b 103.2 ± 3.1 7.89 ± 0.10
5-E 52.64 ± 0.01 a 104.4 ± 1.5 a 9.01 ± 0.03 d 104.4 ± 1.5 a
15-E 51.91 ± 0.01 ab 105.2 ± 0.0 a 7.09 ± 0.01 b 105.2 ± 0.0 a
5-CS 52.39 ± 0.73 a 103.8 ± 0.0 a 7.01 ± 0.02 b 103.8 ± 0.0 a
15-CS 51.73 ± 0.02 ab 104.8 ± 1.5 a 6.03 ± 0.02 a 104.8 ± 1.5 a
E—erythritol, CS—cane sugar, 5 and 15 means 5 g and 15 g added per 100 g of T. catappa flour, FC-foaming
capacity, FS—foaming stability, EA—Emulsification activity, ES—Emulsification stability. Lowercase letters mean
significant differences in columns at p = 0.05.

Foam stability (FS) values remained relatively consistent across all samples, ranging
from 103.2 ± 3.1 to 105.2 ± 0.0%, with no statistically significant differences. Interestingly,
all blends showed slightly higher FS values compared to pure T. catappa, suggesting that
the addition of sweeteners might contribute to foam stabilization, which is confirmed by
the results of the research by Nastaj et al. (2020) [32], where the addition of erythritol to
foam created from whey protein isolate improved the stability of the foam, but reduced
its volume. Erythritol increases the viscosity of the solution, which slows down the liquid
drainage from the foam and prevents it from collapsing, slightly increases the surface
tension of solutions, and in combination with protein, creates a more stable structure at the
water–air interface.
Appl. Sci. 2024, 14, 11201 8 of 19

Emulsifying activity (EA) demonstrated more pronounced variations among samples,


ranging from 6.03 ± 0.02 to 9.01 ± 0.03. The 5% erythritol blend showed the highest EA
(9.01 ± 0.03), while the 15% cane sugar blend exhibited the lowest value (6.03 ± 0.02). A
general trend of decreasing EA was observed with increasing sweetener content, particu-
larly with cane sugar additions. Emulsion stability (ES) values were consistent across all
samples, ranging from 103.2 ± 3.1 to 105.2 ± 0.0, with no statistically significant differences
between treatments. This suggests that sweetener addition did not significantly impact the
stability of formed emulsions.
These results indicate that while sweetener addition had minimal impact on foaming
and emulsion stability, it did influence foaming capacity and particularly emulsifying
activity, with higher sweetener concentrations generally resulting in reduced functional
properties. The foaming capacity (FC) values (51.73–53.21%) and foaming stability (FS)
values (103.2–105.2%) are comparable to those reported by Maboh et al. (2023) [29]. These
properties suggest good potential for applications requiring aeration and foam stability.
The emulsifying activity (EA) ranging from 6.03 to 9.01 and emulsion stability (ES)
values of 103.2–105.2% demonstrate the flour’s ability to stabilize oil-in-water emulsions.
This is particularly important for food applications where emulsion stability is crucial, such
as baked goods and processed foods.
The viscometric characteristics of T. catappa powder and its blends with erythritol and
cane sugar are presented in Table 3.

Table 3. Viscometric characteristics of T. catappa and its erythritol and cane sugar blends.

Peak Trough Breakdown Final Setback Pasting


Peak Time
Sample Viscosity Viscosity Viscosity Viscosity Viscosity Temperature
[mPa·s] [s] [◦ C]
T. catappa 172.0 ± 23.0 c 166.0 ± 13.0 b 6.0 ± 2.0 b 277.0 ± 23.0 c 111.0 ± 7.0 c 6.0 ± 0.5 a 87.0 ± 6.0 c
5-E 104.0 ± 34.0 ab 100.5 ± 10.0 a 3.5 ± 1.5 a 162.0 ± 14.0 ab 61.5 ± 2.0 b 6.5 ± 0.0 a 87.0 ± 5.0 c
15-E 103.0 ± 28.0 ab 97.5 ± 7.0 a 10.5 ± 2.0 bc 139.0 ± 11.0 a 46.5 ± 1.0 a 6.5 ± 0.0 a 56.5 ± 2.0 a
5-CS 193.0 ± 21.0 c 181.0 ± 21.0 b 12.0 ± 1.0 c 307.0 ± 32.0 c 126.0 ± 4.0 c 6.0 ± 0.5 a 70.0 ± 4.0 b
15-CS 98.0 ± 13.0 a 92.5 ± 6.0 a 5.5 ± 1.5 ab 134.0 ± 10.0 a 41.5 ± 2.0 a 6.0 ± 1.0 a 53.5 ± 1.0 a
E—erythritol, CS—cane sugar, 5 and 15 means 5 g and 15 g added per 100 g of T. catappa flour, and lowercase
letters mean significant column differences at p = 0.05.

Peak viscosity (PV) varied considerably among samples, ranging from 98 ± 13 to


193 ± 21 mPa·s. Pure T. catappa and the 5% cane sugar blend exhibited the highest peak
viscosities (172 ± 23 and 193 ± 21 mPa·s, respectively), while blends with 15% sweetener
content showed significantly lower values (103 ± 28 and 98 ± 13 mPa·s for erythritol and
cane sugar, respectively).
Trough viscosity (TV) values followed a similar pattern to peak viscosity, ranging from
92.5 ± 6 to 181 ± 21 mPa·s. Pure T. catappa and the 5% cane sugar blend maintained higher
trough viscosities (166 ± 13 and 181 ± 21 mPa·s, respectively), while higher sweetener
concentrations resulted in lower TV values.
Breakdown viscosity (BV) varied from 3.5 ± 1.5 to 12 ± 1 mPa·s, with the 5% cane
sugar blend showing the highest value (12 ± 1 mPa·s) and the 5% erythritol blend showing
the lowest (3.5 ± 1.5 mPa·s). Final viscosity (FV) ranged from 134 ± 10 to 307 ± 32 mPa·s,
with higher values observed in pure T. catappa and the 5% cane sugar blend.
Setback viscosity (SV) showed significant variations, ranging from 41.5 ± 2 to
126 ± 4 mPa·s. The highest setback values were observed in pure T. catappa and the
5% cane sugar blend (111 ± 7 and 126 ± 4 mPa·s, respectively), while both 15% sweetener
blends showed lower values.
Peak time remained relatively constant across all samples at approximately 6–6.5 min,
showing no significant differences between treatments. Pasting temperature varied sig-
blend (111 ± 7 and 126 ± 4 mPa·s, respectively), while both 15% sweetener blends showed
Appl. Sci. 2024, 14, 11201 lower values. 9 of 19
Peak time remained relatively constant across all samples at approximately 6–6.5
min, showing no significant differences between treatments. Pasting temperature varied
significantly
nificantly fromfrom53.5
53.5±±11toto87
87± ± 66 °C.
◦ C.Pure
PureT. T.catappa
catappaand andthe the5%5%erythritol
erythritolblend
blendshowed
showed
the highest pasting temperatures (87 ± 6 and 87 ± 5 °C, respectively),
the highest pasting temperatures (87 ± 6 and 87 ± 5 C, respectively), while ◦ while both 15% sweet-
both 15%
ener blends exhibited significantly lower pasting temperatures.
sweetener blends exhibited significantly lower pasting temperatures.
These
Theseresults
resultsindicate
indicatethat
thatsweetener
sweeteneraddition,
addition,particularly
particularlyatathigher higherconcentrations,
concentrations,
substantially
substantially affected the pasting properties of T. catappa powder, generallyresulting
affected the pasting properties of T. catappa powder, generally resultinginin
reduced
reducedviscosity
viscosityparameters
parametersand andlower
lowerpasting
pastingtemperatures.
temperatures.According AccordingtotoLiu Liuetetal.al.
(2024) [33], erythritol, acting as a plasticizer, reduced the viscosity of
(2024) [33], erythritol, acting as a plasticizer, reduced the viscosity of corn starch solution corn starch solution
during
duringgelatinization.
gelatinization.
Erythritol,
Erythritol,penetrating
penetratingthe thestarch
starchstructure,
structure,can candisrupt
disrupthydrogen
hydrogenbonds bondsbetween
between
starch
starch molecules, which leads to a decrease in viscosity, and can bind watermolecules,
molecules, which leads to a decrease in viscosity, and can bind water molecules,
reducing
reducingtheir
their availability to starch
availability to starchmolecules
moleculesand andthusthuslimiting
limiting starch
starch swelling,
swelling, whichwhich
also
also contributes
contributes to ato a decrease
decrease in viscosity.
in viscosity.
The
Thetype
typeofofsweetener
sweeteneralso alsoinfluenced
influencedthese thesecharacteristics,
characteristics,with withcane
canesugar
sugarand and
erythritol showing different effects at similar concentration levels. In
erythritol showing different effects at similar concentration levels. In the studies by Boruk the studies by Boruk
and
andWinkler
Winkler(2023)
(2023)[34]
[34]and
andPongsawatmanit
Pongsawatmanitetetal. al.(2002)
(2002)[35],[35],the
theaddition
additionofofsucrose
sucrosetoto
wheat
wheatdough
doughand andcassava
cassavastarch
starchincreased
increasedits itsviscosity.
viscosity.
The
Thepasting
pastingproperties
properties show
show significant variations
variations with withpeak
peakviscosity
viscosityranging
rangingfrom
from98
98toto 193
193 mPas.
mPas. These
These values
values align
align withwith those
those HaliluHalilu
et al.et (2021)
al. (2021) reported
reported for similar
for similar nut-
nut-based
floursflours
based [36]. The
[36].breakdown
The breakdown viscosity (3.5–12(3.5–12
viscosity mPas)mPas)indicates good paste
indicates good stability during
paste stability
cooking,
during while the
cooking, whilesetback viscosity
the setback (41.5–126
viscosity mPas) suggests
(41.5–126 a moderate
mPas) suggests retrogradation
a moderate retro-
tendency. The pasting temperature range (53.5–87 ◦ C) is typical for nut flours and indicates
gradation tendency. The pasting temperature range (53.5–87 °C) is typical for nut flours
good
and gelatinization
indicates properties suitable
good gelatinization for various
properties suitablefood applications.
for various food applications.
Figure1 illustrates
Figure 1 illustratesthethe pasting
pasting profiles
profiles of T.of T. catappa
catappa powder powder
and itsand its blends
blends with
with eryth-
erythritol
ritol and caneand sugar
cane sugar
over over
timetimeunder under controlled
controlled temperature
temperature conditions.The
conditions. Theviscosity
viscosity
curvesdemonstrate
curves demonstrate distinct
distinct patterns among the the different
differentformulations
formulationsduring duringthe heating–
the heat-
cooling cycle.
ing–cooling cycle.

350 100
90
300
80

Temperature [°C]
250 70
Viscosity [mPa·s]

200 60
50
150 40
100 30
20
50
10
0 0
1
9
17
25
33
41
49
57
65
73
81
89
97
105
113
121
129
137
145
153
161
169
177
185
193

Time [s]
T. catappa 5-E 15-E 5-CS 15-CS Temp(°C)

Figure1.1.Pasting
Figure profilesofofT.T.catappa
Pastingprofiles catappaand
andits
itsblends
blendswith
witherythritol
erythritoland
andcane
canesugar.
sugar.

PureT.T.catappa
Pure catappaand
andthe
the5%5%cane
canesugar
sugarblend
blendexhibited
exhibitedthe
thehighest
highestviscosity
viscosityalong
alongthe
the
profiles, reaching approximately 170–190 mPa · s during the heating phase. These
profiles, reaching approximately 170–190 mPa·s during the heating phase. These samples samples
donot
do notshow
showthethecharacteristic
characteristicpasting
pastingbehavior
behaviorwithwithprecise
precisepeak
peakformation,
formation,followed
followedbyby
a breakdown phase and subsequent increase during cooling. Oppositely,
a breakdown phase and subsequent increase during cooling. Oppositely, they resemblethey resemble
more high protein sample pasting profiles with a prolonged phase of building viscosity.
These samples’ relatively high (compared to initial) final viscosities (around 270–300 mPa·s)
suggest some retrogradation tendencies.
Appl. Sci. 2024, 14, 11201 10 of 19

Adding higher concentrations of sweeteners (15% of erythritol and cane sugar) resulted
in even lower viscosity profiles throughout the entire pasting cycle. These blends do not
show isolated peaks with a viscosity of approximately 100 mPa·s during the heating and
maintaining phase, resembling the profile of pure T. catappa.
The final viscosities of these blends were also notably lower (130–140 mPa·s), suggest-
ing a dilution effect to the control and lower concentration blends. The 5% erythritol blend
showed an intermediate pasting profile, with a peak viscosity of around 104 mPa·s and a
relatively stable viscosity throughout the heating-holding phase.
All samples showed relatively stable viscosity during the holding phase at 95 ◦ C,
indicating good thermal stability of the formed pastes. The cooling phase demonstrated
varying degrees of setback, with pure T. catappa and the 5% cane sugar blend showing
the most pronounced increases in viscosity, indicating a stronger tendency for viscosity
formation. These pasting profiles align with the numerical data presented in Table 3,
confirming that both the type and concentration of sweeteners significantly influence the
pasting behavior of T. catappa powder blends.
The pasting profiles demonstrate characteristic behavior for high fat high protein nut-
like flours, showing slowed transitions through gelatinization, peak viscosity, and setback
phases [37]. The addition of different sweeteners notably affects the viscosity development,
with erythritol and cane sugar showing distinct impacts on the pasting behavior. This
aligns with Misra et al.’s (2023) [38] findings regarding the influence of additives on flour
pasting properties.

3.2. Bioactive Characteristics of T. catappa and Its Blends with Erythritol and Cane Sugar
Table 4 presents the bioactive profile of T. catappa powder and its blends with erythritol
and cane sugar, evaluated through multiple antioxidant assays using both ethanolic and
water extracts.

Table 4. Bioactive profile of T. catappa and its erythritol and cane sugar blends.

Reducing DPPH DPPH


Samples ABTS ETOH ABTS H2 O FRAP ETOH FRAP H2 O
Sugars ETOH H2 O
[GEmg/1 gDM] [TE mg/1 gDM] (FeSO4 mg/1 gDM)
a a a 1.96 ± 0.05 a
T. catappa 6.04 ± 0.13 b 1.95 ± 0.05 3.35 ± 0.04 b 3.17 ± 0.13 1.96 ± 0.42 2.15 ± 0.30 ab
5-E 4.07 ± 0.04 a 2.06 ± 0.62 a 1.85 ± 0.13 a 3.30 ± 0.17 a 1.97 ± 0.05 a 1.97 ± 0.42 a 2.11 ± 0.13 ab
15-E 4.38 ± 0.26 a 2.73 ± 0.75 a 2.63 ± 0.80 ab 3.46 ± 0.33 a 1.75 ± 0.14 a 1.75 ± 0.14 a 2.28 ± 0.19 ab
5-CS 4.19 ± 0.07 a 2.40 ± 0.49 a 1.96 ± 0.06 a 3.97 ± 0.17 a 1.87 ± 0.00 a 1.87 ± 0.00 a 1.97 ± 0.05 a
15-CS 4.32 ± 0.01 a 2.11 ± 0.29 a 2.15 ± 0.50 a 4.21 ± 1.24 a 1.57 ± 0.03 a 1.57 ± 0.03 a 2.63 ± 0.25 b
sample ns ns ns
solvent ns ns **
sample × solvent ns *** *
E—erythritol, CS—cane sugar, mean values with different lowercase letters imply significant differences between
means in rows at p < 0.05. Second order interaction analysis *—p < 0.05; **—p < 0.01; ***—p < 0.001, ns—non
significant (p > 0.05).

The reducing sugar content showed significant variations among samples, with pure
T. catappa exhibiting the highest value (6.04 ± 0.13 mg GE/g DM), and sweetener-containing
blends showing lower values ranging from 4.07 ± 0.04 to 4.38 ± 0.26 mg GE/g DM.
DPPH radical scavenging activity varied depending on the extraction solvent used.
Ethanolic extracts showed values ranging from 1.95 ± 0.05 to 2.73 ± 0.75 mg TE/g DM,
with the 15% erythritol blend exhibiting the highest antioxidant activity. Water extracts
demonstrated higher DPPH values for pure T. catappa (3.35 ± 0.04 TE mg/1 gDM) than
in ethanol extract (1.95 ± 0.05 TE mg/1 gDM). ABTS radical scavenging capacity showed
higher values in ethanolic extracts compared to water extracts. Ethanolic extract values
Appl. Sci. 2024, 14, 11201 11 of 19

ranged from 3.17 ± 0.13 to 4.21 ± 1.24 mg TE/g DM, with the 15% cane sugar blend
showing the highest activity. Water extracts showed lower values ranging from 1.57 ± 0.03
to 1.97 ± 0.42 mg TE/g DM, with minimal variation among samples. FRAP assay results
showed similar trends across both extraction methods. Ethanolic extracts ranged from
1.57 ± 0.03 to 1.97 ± 0.42 mM FeSO4 , while water extracts showed slightly higher values
ranging from 1.97 ± 0.05 to 2.63 ± 0.25 mM FeSO4 . The 15% cane sugar blend exhibited
the highest FRAP value in water extracts.
Statistical analysis revealed significant interaction between sample results and the
extraction solvent used on the ABTS results (p < 0.001) while DPPH showed no significant
interaction effects. FRAP values (p < 0.05) were dependent on the extraction solvent, which
modulated by interaction the FRAP values on different samples. Sample type alone showed
no significant effect on DPPH, ABTS, and FRAP values.
Two-way ANOVA showed that the antioxidant activity expressed by the ABTS method
significantly depends on the type of extractant used. In EtOH extracts, all variants of the
tested samples showed significantly higher antioxidant activity than water extracts. Using
a sweetener did not affect the antioxidant activity change (for the ABTS method) compared
to the control, both in the case of ethanol and water extract. Similar results were obtained
in the studies by Bouagnon et al. (2024) [39] in which the ethanol extract of T. catappa
showed higher antioxidant activity (measured by the ABTS method) than the same raw
material extracted by water [39]. Antioxidant activity of the control sample (measured
using the DPPH method, which involves measuring the reaction of quenching the stable
free radical 2,2-diphenyl-1-picrylhydrazyl) depended significantly on the type of extractant
used and was higher for the water extract. The analysis of variance also showed that
adding a sweetener to the tested raw material did not affect (compared to the control)
the antioxidant activity in the ethanol extract. This may be due to the lower extraction
of highly polar antioxidants (such as ascorbic acid) in EtOH than to the water, which
was the reason why no differences were observed in the antioxidant activity (by DPPH
method) of the tested raw materials compared to the control (in the case of the ethanol
extract). Similar results were obtained in studies on tropical plants of the genera Struchium
sparganophora, Amaranthus cruentus, Telfairia occidentalis, Ocimum gratissimum, Cnidoscolous
aconitifolius, and Vernonia amigdalina, where polar extracts showed significantly higher
capacity to scavenge 1,1-diphenyl-2-picrylhydrazyl radicals than extracts of lower polarity
and non-polar extracts [40].
In the case of water extracts, two-way ANOVA showed that 5% addition of erythritol
and 5% and 15% addition of cane sugar have a statistically significant effect (cause a
significant decrease) on antioxidant activity (measured by the DPPH method) compared
to the control. Perhaps the bioactive compounds in cane sugar have too low polarity to
be extracted into ethanol. Cane sugar is a raw material that contains large amounts of
such bioactive components as flavonoids (such as apigenin, luteolin, tricine), alkaloids
(such as piperidine and trigonelline), phytosterols (such as β-sitosterol, campesterol, and
stigmasterol), terpenoids (such as arundoin and isoarborinol), and policosanols (such as
docosanol, hexacosanol, and tetracosanol). Most of these antioxidants are non-polar or
low-polar antioxidants that will not be extracted in water and alcoholic solution [41]. At
the same time, the saccharides present in cane sugar (mainly sucrose) that were extracted
into the water extract could have a pro-oxidant effect. In the water environment, with
access to oxygen, oxidized sucrose free radicals (OSFRs) are formed. The released oxidized
sucrose free radicals (OSFRs) can react with bioactive substances present in T. catappa
seeds, creating more stable non-radical compounds or regaining their reduced form [42].
Hence, the decrease in antioxidant activity (measured by the DPPH method) in an aqueous
solution was observed after adding a sweetener in the form of cane sugar to the almond
raw material. Moreover, the cane sugar concentrations used may have been too low to
effectively extract the antioxidant compounds contained in cane sugar.
Variance analysis showed that the type of extractant used did not affect the value
of reducing activity (FRAP) of the tested control raw material. Furthermore, variance
Variance analysis showed that the type of extractant used did not affect the value
reducing activity (FRAP) of the tested control raw material. Furthermore, variance ana
Appl. Sci. 2024, 14, 11201 12 of 19
sis showed that adding a sweetener did not affect the value of reducing activity of t
tested raw material (relative to the control) in the case of extraction with an ethanol so
tion. It is indicated that potent reducing agents include alkali metals, such as sodiu
analysis showed that adding
magnesium, a sweetener
zinc, calcium, and did not affect
potassium, the value
which of reducing
are present activityamounts
in significant of in
the tested raw material (relative
catappa seeds [43]. to the control) in the case of extraction with an ethanol
solution. It is indicated that potent
The analysis reducing
of reducing agents include
properties alkali
(measured bymetals,
FRAP)such as sodium,
shows that the extracti
magnesium, of these substances into water and ethanol can occur at a similar level andinintensity.
zinc, calcium, and potassium, which are present in significant amounts T. P
catappa seeds [43].
yphenols present in plants, especially phenolic acids and flavonoids, can also act as
The analysis of reducing properties (measured by FRAP) shows that the extraction
ducing agents (electron donors) [44]. Analysis of variance showed that 15% addition
of these substances into water and ethanol can occur at a similar level and intensity.
cane sugar to the tested raw material caused a statistically significant increase in reduci
Polyphenols present in plants, especially phenolic acids and flavonoids, can also act as
activity compared to the control in the case of an aqueous solution. It was confirmed th
reducing agents (electron donors) [44]. Analysis of variance showed that 15% addition of
cane sugar contains such phenolic acids as hydroxycinnamic acid, caffeic acid, and sinap
cane sugar to the tested raw material caused a statistically significant increase in reducing
acid and flavonoids as apigenin, luteolin, and catechin [41]. The higher solubility of the
activity compared to the control in the case of an aqueous solution. It was confirmed that
substances in water was probably the reason for the high reducing activity (compared
cane sugar contains such phenolic acids as hydroxycinnamic acid, caffeic acid, and sinapic
the control) in the case of the aqueous extract containing T. catappa seeds with 15% add
acid and flavonoids as apigenin, luteolin, and catechin [41]. The higher solubility of these
tion of sugar cane.
substances in water was probably the reason for the high reducing activity (compared to
These results indicate that both sweetener addition and extraction solvent choice
the control) in the case of the aqueous extract containing T. catappa seeds with 15% addition
fluence the bioactive properties of T. catappa powder, with different antioxidant assa
of sugar cane.
These showing varyingthat
results indicate sensitivities to these addition
both sweetener factors. The
anddata suggestsolvent
extraction that water and ethano
choice
influence the bioactive properties of T. catappa powder, with different antioxidant assays antio
extracts may access different profiles of bioactive compounds, leading to varying
dant capacities
showing varying across
sensitivities different
to these assay
factors. Themethods.
data suggest that water and ethanolic ex-
tracts may access different profiles of bioactive powder
The FTIR spectra of T. catappa compounds,and leading
its blendsto with erythritol
varying and cane sug
antioxidant
revealdifferent
capacities across characteristic absorption bands indicating the presence of various function
assay methods.
groups and their interactions.
The FTIR spectra of T. catappa powder The
andspectra show
its blends several
with distinct
erythritol andabsorption
cane sugar regions th
characterise the samplesʹ molecular composition (Figure 2).
reveal characteristic absorption bands indicating the presence of various functional groups
and their interactions. The spectra show several distinct absorption regions that characterise
the samples’ molecular composition (Figure 2).

0.6

T.catappa
0.5
5-E
15-E
5-CS
0.4 15-CS
Absorbance

0.3

0.2

0.1

0.0

-0.1
400 800 1200 1600 2000 2400 2800 3200 3600 4000

Wavenumber (cm-1)
Figure 2. FTIR spectra of T. catappa and its erythritol and cane sugar blends.
Figure 2. FTIR spectra of T. catappa and its erythritol and cane sugar blends.
The broad absorption band observed in the 3200–3400 cm−1 region corresponds to
O-H stretching The broad absorption
vibrations, band observed
primarily representing in the 3200–3400
hydroxyl cm−1carbohydrates
groups from region corresponds to
and moisture content in the samples. Changes in the intensity and slight shiftsfrom
H stretching vibrations, primarily representing hydroxyl groups carbohydrates
in this band a
among different blends indicate varying degrees of hydrogen bonding interactions between
the sweeteners and T. catappa components. The region between 2800 and 3000 cm−1 shows
characteristic C-H stretching vibrations, typically associated with CH2 and CH3 groups
Appl. Sci. 2024, 14, 11201 13 of 19

present in the samples’ organic compounds. The intensity of these peaks varies with sweet-
ener addition, reflecting changes in the relative concentration of these molecular groups.
A prominent band around 1630–1650 cm−1 can be attributed to C=O stretching vibra-
tions, likely from proteins and other carbonyl-containing compounds. The amide bands in
this region also indicate the presence of protein structures in the samples.
The fingerprint region (1200–900 cm−1 ) shows overlapping peaks characteristic of
C-O and C-C stretching vibrations, typically associated with carbohydrates and glycosidic
linkages. The addition of sweeteners notably affects the intensity and pattern of peaks in
this region, indicating modifications in the carbohydrate structure and interactions. Sharp
peaks observed in the 1000–1100 cm−1 range are characteristic of C-O-C linkages and ring
vibrations of carbohydrates. The varying intensities of these peaks among different blends
reflect the changing carbohydrate composition with sweetener addition.
These spectral patterns confirm the successful incorporation of sweeteners into the
T. catappa matrix and provide evidence of molecular interactions between the components,
supporting the observed changes in functional properties described in previous tables.
The FTIR spectra reveal characteristic molecular fingerprints of T. catappa flour and its
blends. The peaks indicate the presence of key functional groups associated with proteins,
carbohydrates, and lipids, confirming the complex composition of the flour. These findings
are consistent with those reported by Ng et al. (2014), providing valuable information
about the material’s molecular structure and potential functionality [45].

3.3. Quality Features of Cookies Made with T. catappa


The initial water activity (Aw) of the cookies at production was recorded at
0.294 ± 0.024, indicating a moderate moisture level that supports freshness and shelf
stability (Figure 3a). Following open-air storage, Aw was re-measured at critical intervals
to assess changes in moisture distribution. After seven days, Aw increased slightly to
0.303, suggesting minimal but detectable moisture absorption, likely due to environmental
exposure. After one month, Aw rose further to 0.320, reflecting a gradual moisture up-
take over time. This progressive increase may indicate internal moisture redistribution,
impacting texture and product stability. The gradual rise in Aw highlights a tendency for
the products to absorb moisture over time, potentially influencing texture and shelf life
Appl. Sci. 2024, 14, x FOR PEER REVIEW
and indicating a need for regular Aw monitoring to maintain target quality and14safetyof 19
standards during storage.

0.34 15.60
15.20
0.33 0.32 15.40
15.00
0.32 15.20
Water activity

Hardness [N]

0.30
0.31 0.29 15.00 14.70
0.30 14.80
0.29 14.60
0.28 14.40
0.27 14.20
0.26 14.00
fresh stored 7 stored 30 fresh stored 7 stored 30
days days days days

(a) (b)
Figure
Figure 3. Quality
Quality features
features of
of cookies
cookies during storage (a) Water activity; (b) Hardness.

In the
The results
cookies of Santos
exhibited anetaverage
al. (2020) [46], the
hardness water
of 15.2 activity
N (or of tropical
1.55 KGF) almonds
at production,
was studied and
characterizing themfound to be relatively
as moderately high,a balanced
hard with which can facilitate
texture microbial
(Figure 3b). Togrowth if
evaluate
not effect
the adequately controlled.
of moisture Despite
changes this, the microbial
on structural integrity, count remained
hardness within safe under
was re-measured limits,
identical conditions after extended exposure. After seven days, no significant change in
hardness was observed, indicating short-term stability in texture despite minor increases
in Aw. After one month, a slight decrease in hardness to 14.7 N (or 1.49 KGF) was rec-
orded. This minor softening effect is consistent with gradual moisture absorption, which
may subtly alter their matrix over prolonged storage. The reduction in hardness over time
0.28 14.40
0.27 14.20
0.26 14.00
Appl. Sci. 2024, 14, 11201 fresh stored 7 stored 30 fresh stored 7 stored 30
14 of 19
days days days days

(a) (b)
suggesting that tropical almonds could be a viable raw material for products like cookies,
Figure 3. Quality features of cookies during storage (a) Water activity; (b) Hardness.
where lower water activity levels during baking would help inhibit microbial growth and
improve shelf life.
The cookies exhibited an average hardness of 15.2 N (or 1.55 KGF) at production,
The cookies exhibited an average hardness of 15.2 N (or 1.55 KGF) at production,
characterizing them as moderately hard with a balanced texture (Figure 3b). To evaluate
characterizing them as moderately hard with a balanced texture (Figure 3b). To evaluate the
the effect of moisture changes on structural integrity, hardness was re-measured under
effect of moisture changes on structural integrity, hardness was re-measured under identical
identical conditions after extended exposure. After seven days, no significant change in
conditions after extended exposure. After seven days, no significant change in hardness
hardness was observed, indicating short-term stability in texture despite minor increases
was observed, indicating short-term stability in texture despite minor increases in Aw. After
in Aw. After one month, a slight decrease in hardness to 14.7 N (or 1.49 KGF) was rec-
one month, a slight decrease in hardness to 14.7 N (or 1.49 KGF) was recorded. This minor
orded. This minor softening effect is consistent with gradual moisture absorption, which
softening effect is consistent with gradual moisture absorption, which may subtly alter
may subtly alter their matrix over prolonged storage. The reduction in hardness over time
their matrix over prolonged storage. The reduction in hardness over time suggests that
suggests that moisture gain contributes to gradual softening, which could affect the sensory
moisture gain contributes to gradual softening, which could affect the sensory experience.
experience. This softening effect aligns with existing research, where components such as
This softening effect aligns with existing research, where components such as amylose
amylose and amylopectin
and amylopectin play aplay a critical
critical role inrole in determining
determining cookiecookie hardness.
hardness. For example,
For example, cookies
cookies
with higher amylose content tend to be harder and more compact, while amylopec-
with higher amylose content tend to be harder and more compact, while amylopectin
tin contributes
contributes to
to aa lighter
lighter and
andcrispier
crispiertexture.
texture.The Thetexture
textureofof
cookies
cookies cancan
also be be
also affected
affected
by by
thethe
proportions of carbohydrates, proteins, and structural elements like
proportions of carbohydrates, proteins, and structural elements like cellulose cellulose andand
pectin [47]. Monitoring these changes will help refine packaging and storage
pectin [47]. Monitoring these changes will help refine packaging and storage practices practices to to
preserve the desired texture and consumer satisfaction throughout the product’s
preserve the desired texture and consumer satisfaction throughout the product’s shelf life. shelf life.
TheThe
antioxidant
antioxidant profile of cookies
profile of cookiesis presented
is presentedon on
Figure 4. 4.
Figure

5 4.65 4.58
3.95 3.92
10^-6 mg FeSO4/1 g DM

4
mg TE/1 g DM

2
1.20 1.21
1

Ethanolic extract Aqueous extract

Figure 4. Antioxidative activity of cookies.


Figure 4. Antioxidative activity of cookies.
The DPPH antioxidant capacity analysis reflects the presence of compounds capable
ofThe DPPH antioxidant
neutralizing capacity
free radicals, with a analysis reflects the
slight advantage presence ofactivity
in antioxidant compounds capable
observed for the
of neutralizing free The
aqueous extract. radicals,
ABTSwith
assaya shows
slight advantage in antioxidant
relatively high activity
values in both observed
extracts, for a
indicating
high antioxidant potential against ABTS radicals, essential for counteracting oxidative stress.
The FRAP assay results display substantial ferric-reducing abilities, with the ethanolic
extract slightly outperforming the aqueous one. These antioxidant analyses collectively
highlight the cookies’ significant capacity to counteract oxidative damage from free radicals,
with varying potencies depending on the assay and extract type. Mwangi et al. (2024) [48]
demonstrated that T. catappa L. leaves have significant antioxidant capabilities, with a
DPPH scavenging activity of 70.4% and an IC50 of 5.6 µg/mL, indicating a solid ability to
neutralize free radicals and mitigate oxidative stress. Santos et al. (2020) [46] reported that
defatted seed flour contains a total phenolic content of 649.51 mg/100 g, contributing to an
antioxidant activity of 46.05 µg TE/mg, playing a crucial role in enhancing the antioxidant
potential of the cookies. The results suggest that the cookies may offer beneficial protective
effects against oxidative damage in the body.
The dietary fiber analysis of the cookies reveals a total dietary fiber content of 5.018 g
per 100 g. This includes water-soluble (1.258 g) and water-insoluble (3.760 g) fibers, with a
[46] reported that defatted seed flour contains a total phenolic content of 649.51 mg/100 g,
contributing to an antioxidant activity of 46.05 µg TE/mg, playing a crucial role in enhanc-
ing the antioxidant potential of the cookies. The results suggest that the cookies may offer
beneficial protective effects against oxidative damage in the body.
Appl. Sci. 2024, 14, 11201 The dietary fiber analysis of the cookies reveals a total dietary fiber content of 5.018 15 of 19
g per 100 g. This includes water-soluble (1.258 g) and water-insoluble (3.760 g) fibers, with
a notably higher proportion of the latter. The significant presence of water-insoluble fiber
suggests thatnotably higher
the cookies proportion
contribute of the latter.
to digestive healthThe
bysignificant presence
aiding in bowel of water-insoluble
regularity and fiber
adding bulk suggests thatMeanwhile,
to the diet. the cookies contribute to digestive
the water-soluble health
fiber, thoughby aiding
presentinin bowel
lower regularity and
amounts, offersadding bulk tohealth
additional the diet. Meanwhile,
benefits, such as the water-soluble
potential cholesterol fiber, though present
regulation and in lower
amounts, offers additional health benefits, such as potential
support for blood sugar stability. The combined fiber profile indicates that these cookies cholesterol regulation and
support for blood sugar stability. The combined fiber profile
can serve as a valuable source of dietary fiber, promoting digestive health while poten- indicates that these cookies
tially offeringcan serve
other as a valuable
benefits associatedsource of dietary
with fiber intake.fiber, promoting
Terminalia catappadigestive
can serve health
as an while poten-
tially for
excellent material offering other the
enhancing benefits associated
dietary with fiber
fiber content of foodintake. Terminalia
products, which catappa
is re- can serve as
an excellent material for enhancing the dietary fiber content
lated to various health benefits such as improved digestive health and a reduced risk of of food products, which is
related to various health benefits such as improved digestive
chronic diseases [46]. The presence of both water-soluble and water-insoluble fibers in health and a reduced risk
of chronic diseases [46]. The presence of both water-soluble
Terminalia catappa makes it particularly valuable, as these fibers contribute to bowel regu-and water-insoluble fibers
in Terminalia
larity, cholesterol catappa
regulation, and makes
overallitgut
particularly valuable,
health, making it aas these fibers
beneficial contribute
addition to to bowel
regularity, cholesterol regulation, and
cookie formulations aimed at promoting health and well-being.overall gut health, making it a beneficial addition to
cookie formulations aimed at promoting health and well-being.
The sensory evaluation highlights distinct consumer preferences for the thicker (10
The sensory evaluation highlights distinct consumer preferences for the thicker (10 mm)
mm) and thinner (5 mm) cookies, each offering unique qualities that appeal to different
and thinner (5 mm) cookies, each offering unique qualities that appeal to different aspects
aspects of the tasting experience (Figure 5).
of the tasting experience (Figure 5).

10 mm 5 mm

Appearance
5
4
Texture 3 Flavor
2
1
0

Aftertaste Taste

Crispiness

Figure
Figure 5. Sensory 5. Sensory
assessment assessment
of cookies of cookies
depending on depending on their thickness.
their thickness.
The thicker cookie is favoured for its overall appearance and mouthfeel, providing
The thicker cookie is favoured for its overall appearance and mouthfeel, providing a
a satisfying texture that enhances enjoyment. Meanwhile, the thinner cookie is preferred
satisfying texture that enhances enjoyment. Meanwhile, the thinner cookie is preferred for
for its crispiness, delivering a desirable crunch, and also scores slightly higher in aroma,
its crispiness, delivering a desirable crunch, and also scores slightly higher in aroma, add-
adding to its sensory appeal.
ing to its sensory appeal.
The thicker cookie is generally preferred for its visual appeal and the pleasant, rich
texture it offers in the mouth, making it ideal for those seeking a more substantial eating
experience. With its enhanced crispiness and subtle aromatic advantage, the thinner cookie
appeals to those who favor a light and crunchy texture. These results highlight that the
thicker cookies excel in appearance and texture, while the thinner stands out in crispiness
and aroma.
Figure 6 presents the visual comparison of cookies based on their thickness: (a) thicker
cookies (10 mm), and (b) thinner cookies (5 mm), illustrating the differences in appearance
that correlate with the sensory qualities and baking outcomes of each thickness.
The study of Ekumankama and Onoyima (2021) [49] demonstrated that blending
almond seed flour with wheat flour significantly enhances the sensory qualities of cookies,
resulting in higher acceptability regarding taste, aroma, and mouthfeel. Cookies produced
with T. catappa kernel flour were particularly well received, highlighting the potential of
almond flour to enrich the overall sensory experience.
cookie appeals to those who favor a light and crunchy texture. These results highlight that
the thicker cookies excel in appearance and texture, while the thinner stands out in crisp-
iness and aroma.
Figure 6 presents the visual comparison of cookies based on their thickness: (a)
Appl. Sci. 2024, 14, 11201 thicker cookies (10 mm), and (b) thinner cookies (5 mm), illustrating the differences in
16 of 19
appearance that correlate with the sensory qualities and baking outcomes of each thick-
ness.

(a) (b)
Figure
Figure6.6.Appearance
Appearanceofofcookies
cookiesdepending
dependingonon
their thickness:
their (a)(a)
thickness: thicker (10(10
thicker mm); (b) (b)
mm); thinner (5
thinner
mm).
(5 mm).

4. Conclusions
The study of Ekumankama and Onoyima (2021) [49] demonstrated that blending al-
mondThis
seedcomprehensive
flour with wheat flour significantly
investigation enhances
of Terminalia the sensory
catappa qualities
kernel flour of cookies,
has revealed its
resulting in higher acceptability regarding taste, aroma, and mouthfeel.
significant potential as a functional food ingredient, particularly in gluten-free Cookies produced
cookie
with T. catappaThe
formulation. kernel
flourflour were particularly
demonstrates welltechno-functional
remarkable received, highlighting the potential
properties, of
with water
almond
holdingflour to enrich
capacity and oiltheabsorption
overall sensory experience.
characteristics comparable to conventional nut flours.
Substantial bioactive compounds, evidenced by significant antioxidant activity across
4.multiple
Conclusions
assay methods, position T. catappa flour as a valuable ingredient for developing
functional food products.investigation of Terminalia catappa kernel flour has revealed its
This comprehensive
The interaction
significant potential asbetween T. catappa
a functional flour and different
food ingredient, sweeteners
particularly provides
in gluten-free cookiecrucial
for-
insights for
mulation. Theproduct formulation, with
flour demonstrates optimaltechno-functional
remarkable results achieved using a combination
properties, with water of
natural sweeteners. The successful development of cookies with stable physicochemical
holding capacity and oil absorption characteristics comparable to conventional nut flours.
properties and
Substantial appreciable
bioactive dietary fiber
compounds, contentby
evidenced (5.018 g/100 g)
significant demonstrates
antioxidant the practical
activity across
applicability of this ingredient in food manufacturing. The favourable sensory
multiple assay methods, position T. catappa flour as a valuable ingredient for developing evaluation
results indicate
functional good consumer acceptance potential, particularly for thicker cookies.
food products.
These findings contribute
The interaction between T.significantly
catappa flourtoand
the different
valorization of T. catappa
sweeteners as a sustain-
provides crucial
able food resource and open new avenues for commercial exploitation
insights for product formulation, with optimal results achieved using a combination of in the functional
food sector.
natural Future research
sweeteners. shoulddevelopment
The successful focus on scaling production
of cookies with processes and exploring
stable physicochemical
additional applications in various food systems.
properties and appreciable dietary fiber content (5.018 g/100 g) demonstrates the practical
applicability of this ingredient in food manufacturing. The favourable sensory evaluation
Supplementary Materials: The following supporting information can be downloaded at: https:
results indicate good consumer acceptance potential, particularly for thicker cookies.
//www.mdpi.com/article/10.3390/app142311201/s1, Figure S1: Terminalia catappa kernel and flour.
These findings contribute significantly to the valorization of T. catappa as a sustaina-
Author
ble resource and Conceptualization,
foodContributions: open new avenues J.H.,
forG.A., E.P. and A.V.;
commercial methodology,
exploitation in theG.A., J.H. and
functional
R.O.; validation, J.H.; formal analysis, K.G., A.W.-B., E.P. and R.O.; investigation, K.G.; resources,
G.A. and J.H.; data curation, J.H.; writing—original draft preparation, J.H., A.W.-B., E.P., R.O. and
A.V.; writing—review and editing, A.V., G.A., E.P., A.W.-B., R.O. and J.H.; visualization, E.P. and
J.H.; supervision, J.H.; project administration, G.A. and J.H.; funding acquisition, G.A. and J.H. All
authors have read and agreed to the published version of the manuscript.
Funding: This research received no external funding.
Institutional Review Board Statement: Not applicable.
Informed Consent Statement: Not applicable.
Data Availability Statement: The original contributions presented in this study are included in the
article/supplementary material. Further inquiries can be directed to the corresponding author.
Appl. Sci. 2024, 14, 11201 17 of 19

Acknowledgments: We sincerely thank Dr. Henry Joseph (Phytobokaz) for providing T. catappa seeds
powder for experiments. Kristy Groton thanks to the Erasmus+ Training program offering research
training opportunities.
Conflicts of Interest: The authors declare no conflicts of interest.

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