Potential Application of Used Coffee Grounds in Le

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Journal of Ecological Engineering

Journal of Ecological Engineering 2023, 24(3), 10–19 Received: 2022.11.14


https://doi.org/10.12911/22998993/157388 Accepted: 2023.01.05
ISSN 2299–8993, License CC-BY 4.0 Published: 2023.01.15

Potential Application of Used Coffee Grounds in Leather Tanning

Ahmed I. Nasr1*, Mohammed A. El Shaer2, Mohamed A. Abd-Elraheem2


1
Wool Production and Technology Department, Animal and Poultry Production Division, Desert Research
Center, Cairo, Egypt
2
Department of Agricultural Biochemistry, Faculty of Agriculture, Al-Azhar University, Cairo, Egypt
* Corresponding author’s e-mail: [email protected]

ABSTRACT
Safety of environment and human health is an essential requirement of modern industrial techniques. Therefore,
using natural agents in tanning industry may emerge as a trusted method to avoid the chemical contamination
caused by using traditional chromium salts in tanning process. This study aimed to evaluate the hot water extract
of used coffee grounds (UCGs) as a vegetable tanning agent. The collected UCGs were dried and extracted with
hot water at 90 °C for 2h. The phytochemical screening properties of UCGs extract were determined. Sufficient
amount of extract was prepared to be used in leather tanning. Three groups were tanned with UCGs extract solely
at concentrations of 20, 30 or 40% of pelts’ weight, while another three groups were tanned with the same con-
centrations and then re-tanned with 10% of a synthetic tanning agent “Phenol sulfonates”. On tanned leathers,
organoleptic, physical and chemical properties were determined; scanning electron micrographs were depicted to
examine the leather surface and collagen fiber bundles. Analysis of UCGs extract revealed that it has good tanning
properties, as it contained tannins (14.92%), tannins/non tannins ratio (2.06), hide powder (39.57) and Stiasny
number (21.16). The results of leather properties showed that using UCGs extract alone at concentration of 40%
achieved the best results for the vegetable tanning where the tanned leather had higher (P<0.05) tensile strength,
tearing strength and shrinking temperature than that treated with the lower level of 20% UCGs extract. However,
40% of UCGs extract is highly recommended to be used to accomplish the required shrinkage temperature that
should be ≥ 70 °C. UCGs extract could be successfully used as tanning agent in vegetable tanning to produce du-
rable leathers with good fullness; it may be used for different manufacturing products, such as footwear and bags.
Moreover, using a combination of UCGs extract at any of the used concentrations with phenol sulfonates 10% led
to significant improvement in all studied traits as compared with using UCGs extract alone.

Keywords: leather properties, tannins, vegetable tanning.

INTRODUCTION wastes of this industry showed many negative ef-


fects on plants, animals and human’s health [Er-
Leather tanning converts animal skins or hides dem & Ozverdi, 2008; Jia, et al., 2016] that pro-
as a material susceptible to biodegradation into moted a return to vegetable tanning again as an
leathers as a non-degradable material, stable ther- eco-friendly tanning method [Alim, et al., 2019].
mally and resistant to abrasion that can be used in
Vegetable tanning is based on the use of nat-
the manufacture of various leather products [Cov-
ural plant extracts with high content of tannin
ington, 2009]. For decades, vegetable tanning was
the only known tanning method. With develop- compounds having small particles enough to pen-
ment of the industry, other tanning methods had etrate, react and crosslink with collagen fibers in
been developed, such as mineral tanning, which is raw skins or hides. Both of condensed and hydro-
currently prevalent in the world. Although chrome lysable tannins with high concentrations in some
tanning has various advantages compared to veg- famous plants (e.g. wattle, mangrove, quebracho
etable tanning [BASF, 2007], solid and liquid and hemlock, myrobalan and chestnut) are being

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Journal of Ecological Engineering 2023, 24(3), 10–19

currently used in leather tanning [BASF, 2007; froth and before it boils, it is taken off the heat.
Dutta, 2008; Covington, 2009]. Sufficient amount of wet UCGs were supplied
As a result of the continuous need for vegeta- from different cafés in Alexandria city, Egypt.
ble tanning extracts, there is a large gap between The collected UCGs were mixed and dried at
the production and consumption of these extracts, room temperature (25 ± 3 °C) and then stored in
causing an increment in tanning cost production. paper bags until being used.
Therefore, the provision of new plant sources is
important to bridge this gap [Falcão & Araújo, Extraction
2018; Guo, et al., 2020].
Extraction of tannins from plant sources is af- Extraction was performed using water with-
fected by different conditions including solvent out any chemical additives. UCGs were soaked in
type, extraction temperature and the solid to sol- water with constant solid/ liquid ratio (1/10, w/w)
vent ratio [Das, et al., 2020]. Using hot water was for a day. The next day, the extraction was carried
found to be the best method for extracting plant out in a 2-L Pyrex glass reactor with mechanical
agents that are used in leather tanning, due to its stirring and automatic temperature control. UCGs
simplicity, high content of tannins and lower cost were heated and once the temperature reached
of extraction process [Galvez, et al., 1997; Li & 90 °C, extraction began to run for 2 hours. After
Maplesden, 1998; Vázquez, et al., 2008; Guo, et extraction, the warm suspension was vacuum fil-
al., 2020]. tered. The liquid extract was dried in an oven at
Coffee is one of the most popular drinks 60 °C till it is dried.
around the world, and it is consumed in large
quantities, amounting to about 11 million tons Phytochemical screening
annually [FAOSTAT, 2020]. Coffee is usually
prepared by extracting it in hot water to leave Extraction yield
the used coffee grounds (UCGs) as a waste. The
Total extraction yield was calculated as
quantity of UCGs produced is estimated about
weight ratio between the dried extract and the ini-
75% of the weight of the original coffee beans, so
tial dry weight of the raw material.
the quantity produced annually reaches 8 million
tons [Choi & Koh, 2017]. Total phenol and tannin contents
Several studies indicated different organic
components that can be exploited from UCGs for Total phenols and tannin contents were de-
multiple purposes, such as making fertilizers, bio- termined by the Folin–Ciocalteu method using
diesel and sorbent for metal removal instead of a spectrophotometer. The total phenols were es-
dumping into general waste and sent to landfill timated as tannic acid equivalent (TAE), while
[Choi & Koh, 2017; Das, et al., 2020; Tran, et al., Polyvinylpolypyrolidone (PVPP) was used to
2020]. Recently, the water extract of UCGs was bind tannin-phenolics for measurement of tan-
chemically evaluated and gave promising results nins, then non-tannins were determined and tan-
as a leather tanning agent [Mutuku, et al., 2022], nins were calculated [Makkar, 2003].
but unfortunately, the application of UCGs extract
in leather tanning has not been performed yet. Lead (II) acetate test
The current investigation aimed to estimate An amount of 0.5 ml of lead acetate solution
the possibility of using hot water extract from (1%) was added to 10 mg of solid extract and the
UCGs to be used in vegetable leather tanning. formation of precipitate indicates the presence
of tannins and phenolic compounds [Ahmed, et
al., 2018].
MATERIALS AND METHODS
Ferric (III) chloride test
Sample collection
Five mg of the extract was taken and 0.5 ml
Wet UCGs are usually produced after prepar- of 5% ferric (III) chloride was added. The de-
ing coffee using the Turkish method, in which velopment of dark bluish black color indicated
ground coffee beans are mixed with water and the presence of tannin compounds [Ahmed, et
then heated. As soon as the mixture begins to al., 2018].

11
Journal of Ecological Engineering 2023, 24(3), 10–19

Flavonoids test common in pre-tanning stage till pickling step.


Few drops of diluted NaOH solution were In tanning step, pelts were divided randomly into
added to 5 ml of 10% extract solution. An intense six groups (three pelts in each group). Table (1)
yellow color was appeared in the test tube as the shows the differences among experimental groups
presence of flavonoids [Hossain, et al., 2013]. in tanning and re-tanning steps.

Hide powder test Tanned leather properties


UCGs extract (400 mg) was dissolved in
Physical and chemical testing was applied on
100 ml of distilled water. Slightly chromated
hide-powder (3 g) was added and the mixture different samples of all finished leathers. Samples
was stirred for one hour. The suspension was were obtained as per ASTM methods [ASTM,
then filtered through a sintered glass filter. The 2014]. The specimens were conditioned at 20 °C
weight gain of the hide powder was expressed ± 2 °C and 65% ± 4% R.H. over a period of 48
as a percentage of weight of the starting material hours. Physical properties, namely; thickness,
[Vázquez, et al., 2008]. density, tensile strength, elongation percentage
at break, split tearing strength, static water ab-
Stiasny number sorption, permeability to water vapor and shrink-
UCGs extract (100 mg) was dissolved in 10 age temperature were measured. Every reported
ml of distilled water. Then, 1 ml of 10M HCl value was an average of three specimens. Chemi-
and 2 ml of formaldehyde (37%) were added and cal properties of pH, moisture % and ash % con-
the mixture was heated under reflux for 30 min- tent were studied. The organoleptic properties of
utes. Later, the hot reaction mixture was filtered tanned leathers were assessed by five experienced
through a sintered glass filter. The precipitate was tanners according to the standard tangible evalu-
washed 5 times with 10 ml hot water and final- ation technique [Kasmudjiastuti & Murti, 2017].
ly dried. The yield of tannin was expressed as a The organoleptic properties included softness,
percentage of the weight of the starting material
grain smoothness, grain tightness, fullness, and
[Vázquez, et al., 2008].
general appearance on a scale of 1–10 points for
Fourier Transform Infrared Spectrometry (FTIR) each functional property (higher points indicate a
superior property).
The spectrophotometer (Bruker Varian 70
transform infrared using Platinum ATR unit) was
used to analyze the chemical structure and the fin- Scanning electron microscopy (SEM)
gerprint extract. Small quantity of the extract in
The leather specimens were cut from official
the solid phase was used and scanned directly on
sampling position according to ASTM- D2813,
the instrument stage.
subjected to sputter coating with gold ions using
a JCF-1100E- JEOL and evaluated using a JEOL
Tanning sheep skins
JSM-IT series electron microscope. Three micro-
Eighteen slaughtered male Egyptian Barki graphs were depicted for each sample; the cross
sheep skins were sent to El-Shafie tannery in El- section at 40x, grain surface at 100x, and collagen
Max region, Alexandria, Egypt. All skins were bundles at 150x.

Table 1. Experimental tanning groups


Experimental group Tanning step Re-tanning step
Group 1 20% UCGs extract Not re-tanned
Group 2 30% UCGs extract Not re-tanned
Group 3 40% UCGs extract Not re-tanned
Group 4 20% UCGs extract 10% Dolatan F*
Group 5 30% UCGs extract 10% Dolatan F*
Group 6 40% UCGs extract 10% Dolatan F*
* Note: Dolatan F is a synthetic re-tanning agent based on phenol sulfonates from Zschimmer & Schwarz company.

12
Journal of Ecological Engineering 2023, 24(3), 10–19

Statistical analysis it was similar to that in a previous investigation


[Low, et al., 2015].
The data were analyzed using GLM of SAS The results of the preliminary phytochemicals
program [SAS, 2008] to evaluate the effect of screening were positive for ferric (III) chloride,
tanning material, UCGs extract concentration lead (II) acetate and sodium hydroxide tests (Ta-
and their interaction on the physical and chemi-
ble 2 and Figure 2). This ensures that the UCGs
cal properties of finished leathers. The following
extract contains tannins and flavonoids com-
model was used:
pounds. In addition, the results of total phenol,
Yijk = µ + Ti + Cj + TCij + eijk (1) tannins, non-tannins and T/NT ratio confirmed
where: Yijk – the observation taken on finished the presence of phenolic compounds and agreed
leather; with the corresponding values obtained in another
µ – overall mean; investigation [Mutuku, et al., 2022].
Ti – a fixed effect of tanning material;
Cj – a fixed effect of UCGs extract con-
Table 2. Properties of used coffee grounds extract
centration;
Property Value
TCij – an interaction effect between tan-
ning material and tanning concentration; Yield 42.43%

eijk – the random error assumed to be Total phenol 24.37 g TAE/100g extract*
normally distributed with mean = 0 Tannins 14.92 g TAE/100g extract*
and variance = σ2e. Non-tannins 7.23 g TAE/100g extract*
Figure 1 summarizes all working steps of T/NT ratio 2.06
this study. Hide powder 39.57
Stiasny no 21.16
Ferric III chloride test for
+
RESULTS AND DISCUSSION tannins
Lead(II) acetate test for
+
tannins
Phytochemical screening of used
Sodium hydroxide test for
coffee grounds extract flavonoids
+

Table 2 shows the properties of UCGs extract. pH 5.21 mmol/l


The extraction yield accounted for 42.43% and * Note: TAE – tannic acid equivalent.

Figure 1. Schematic diagram for working steps

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Journal of Ecological Engineering 2023, 24(3), 10–19

et al., 2008]. In this study, the obtained values of


hide powder (39.57) and Stiasny number (21.16)
illustrated that UCGs extract contains sufficient
amounts of tannins to react with collagen fibers
in the skins [Covington, 2009]. The obtained
pH value of UCGs extract was 5.21 mmol/l.
This value was within the required pH range
for interaction between tannins and skin fibers
which ranges between 2 and 8 mmol/l, where the
change in the isoelectric point of collagen fibers
allows it to bind with tannins compounds [Com-
balia, et al., 2016].
The bands shown in the FTIR spectrum of
Figure 2. Changes in used coffee grounds extract by
UCGs extract indicated the presence of tannins
testing; (1) normal extract 10%, (2) lead (II) acetate test compound (Figure 3). The band at 3343 cm-1 re-
for tannins, (3) sodium hydroxide test for flavonoids, fers to the vibrations of hydroxyl groups and its
and (4) ferric (III) chloride test for tannins broadening indicates strong vibrations. This in-
dicates the presence of many functional groups
of phenolic compounds, such as condensed tan-
As for the UCGs properties related to leather
nins. Additionally, the 1636 cm-1 band indicates
tanning, T/NT ratio that expresses the tanning
the stretching of the C-C bonds of aromatic rings
strength of the extract was 2.06. This value indi-
in the structures of phenolic compounds. More-
cated to superiority of UCGs extract over some
over, the bands at 1051 and 995 cm-1 refer to C-H
commercial vegetable tanning extracts (pine
absorption [Nasr, et al., 2017; Falcão & Araújo,
bark and badan) and its similarity to some other 2018; Marques, et al., 2021].
extracts (tara, chestnut and sumac), while it is
weaker than other extracts (quebracho and mi-
Tanned leathers properties
mosa) [BASF, 2007]. Typically, the hide powder
test informs about the proportion of tannins in the The effects of tanning material, UCGs extract
extract which bind with the skin [Dutta, 2008], concentration and the interaction between them
whereas the Stiasny number indicates the con- on the physical properties of tanned leathers are
densed tannins content in the extract [Vázquez, shown in Table 3.

Figure 3. FTIR spectrum of used coffee grounds extract

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Journal of Ecological Engineering 2023, 24(3), 10–19

Table 3. Physical properties of tanned leathers as affected by tanning material, UCGs extract concentration and
their interaction
Tensile Tearing Shrinkage Water
Property Thickness Density Elongation PWV
strength strength temperature Absorption
Unit mm gm/cm3 Kg/cm2 Kg/cm % o
C mg/cm2/hr %
ASTM D1813 D2346 D2209 D4704 D2211 D6076 D5052 D1815
Effect of tanning material (T)
UCGs extract 1.67 0.80 a
149.89b 47.97 53.49 67.44b 1.68 246.03
UCGs extract +
1.56 0.68 b
233.55 a
49.50 46.90 81.78 a
1.65 249.06
synthetic agent
Significance ns ** * Ns ns ** ns ns
Effect of UCGs extract concentration (C)
20% 1.43b 0.69 123.52b 35.89c 49.81 72.33 1.68 255.47
30% 1.62 ab
0.74 194.52 ab
46.63b 47.65 74.67 1.70 251.51
40% 1.79a 0.79 257.12a 63.70a 53.12 76.83 1.62 235.65
Significance * ns * ** ns ns ns ns
Interaction effect (T × C)
20% 1.38b 0.72bc 100.94c 36.21d 48.85 63.67e 1.71 249.61
UCGs
30% 1.70ab 0.79ab 159.61bc 49.49bc 51.19 68.33d 1.65 256.98
extract
40% 1.93 a
0.88 a
189.11 bc
58.22 b
60.42 70.33 c
1.69 231.50
UCGs 20% 1.47b 0.65c 146.10bc 43.77cd 50.77 81.00a 1.65 261.33
extract
+ 10% 30% 1.54 b
0.69 bc
229.42 b
69.17 a
44.11 81.00 a
1.74 246.05
synthetic
agent 40% 1.66 ab
0.70 bc
325.13 a
35.55 d
45.81 83.33 a
1.56 239.81

Significance * * ** ** ns ** ns ns
Overall of means 1.61 0.74 191.72 48.73 50.19 74.61 1.67 247.55
Standard error of
0.06 0.02 19.59 3.09 1.79 1.82 0.03 3.65
mean

Note: UCGs used coffee grounds. ns – not significant, * significant at p<0.05, ** significant at p<0.01.
Means in the same column with different superscripts letter are significantly different (p<0.05).

Physical properties Regarding the effect of UCGs extract con-


centration, a proportional increment in leather
The effect of tanning material was obvious
thickness (P<0.05), tensile strength (P<0.01)
on the lower density (P<0.01) besides the higher
and tearing strength (P<0.01) was accompanied
tensile strength (P<0.05) and shrinkage tempera-
to the increased concentration of UCGs extract
ture (P<0.01) of UCGs tanned leathers than those
from 20 to 40%. Cross-sectional depictions by
re-tanned by a synthetic tanning agent. The mi- electron microscopy emphasized the UCGs ex-
croscopic images in Figure (4) showed that using tract concentration effects on density and thick-
UCGs extract alone facilitated swelling of col- ness of leather specimens (Figure 4). The varia-
lagen bundles, whereas re-tanning leathers im- tion in density might be attributed to the engage-
proved coherence and reduced swelling in fiber ment between the fiber bundles and tannins that
bundles. These results indicated higher efficiency increase the mass and volume as well, but in
of using the mixture of UCGs extract and the different ratios leading to higher density when
synthetic tanning agent rather than using UCGs higher concentrations were applied. This may
extract solely. In agreement, various studies clari- explain the variation in thickness, as shown in
fied that miscellaneous tanning usually produces Figure 4. The other explanation may be due to
higher quality leathers than those tanned with the presence of other substances in the extract,
only one tanning materials, due to the diversity such as sugars that may cause fermentation and
of active groups in different tanning agents and thus increase the spacing among the fiber bun-
hence more bonds and crosslinks with collagen dles [Covington, 2009]. This gave an indication
fibers in skins that improves strengths and shrink- of a clear fermentation as a result of the tannins
age temperature in tanned leathers [BASF, 2007; present in the UCGs extract, compared with re-
Dutta, 2008; Covington, 2009]. tanning leathers with a synthetic tanning agent.

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Journal of Ecological Engineering 2023, 24(3), 10–19

Figure 4. Scanning electron micrographs for all tanned leathers groups with used coffee grounds (UCGs);
(A) cross section depicted at x40, (B) grain surface depicted at 100x, and (C) collagen bundles depicted at 150x

With respect to leathers durability properties, significant differences. The effect was significant
the tensile and tearing strengths of tanned leathers (P<0.05) with both thickness and density and
were improved by increasing of the UCGs extract highly significant (P<0.01) with tensile strength,
concentration. This improvement might be re- tearing strength and shrinkage temperature. The
ferred to at least one of two explanations or both; results of shrinkage temperature showed that us-
the first explanation might be due to the increased ing UCGs extract alone in tanning with concen-
crosslinks formed among collagen fibers that trations less than 40% produced the leathers with
strengthened adhesion and cohesion (Figure 4), a shrinkage temperature of less than 70 degrees,
and made them more resistant to loads. The other which is the lowest allowed shrinkage temperature
prospected explanation might be due to the in- in vegetable tanning [BASF, 2007; Dutta, 2008;
verse mathematical relationship between leather Covington, 2009]. Additionally, the other results of
thickness and either tensile or tearing strengths interaction effect showed that increasing the con-
[Abdelsalam, et al., 1998]. centration of UCGs extract improved the quality
The interaction between the effects of tanning of tanned leathers, as well as the properties were
material and UCGs extract concentration showed further enhanced when re-tanning with a synthetic

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Journal of Ecological Engineering 2023, 24(3), 10–19

tanning agent. Consequently, a concentration of the corresponding re-tanned leathers, as a result


40% UCGs extract was found to be the minimum of the addition of the synthetic tanning agent.
limit when using UCGs solely or it can be used
with any concentration in miscellaneous tanning Organoleptic properties
to produce leathers suitable for the purposes of Re-tanning leathers in this study with a syn-
manufacturing footwear and bags, according to thetic tanning material improved their organoleptic
the recommended quality requirements of different properties (Table 5). The improvement in leathers
leather types [UNIDO, 1994; BASF, 2007]. fullness and softness related with increasing leather
thickness, as well as enhancing both tensile and tear-
Chemical properties ing strength (Table 3). Additionally, narrow pores
Regarding the chemical properties of tanned and light wrinkles on the surfaces of re-tanned leath-
leathers (Table 4), the ash content of tanned leath- ers (Figure 4) explained the improvement in grain
ers with UCGs extract was higher (P<0.01) than tightness, grain smoothness and general appearance.

Table 4. Chemical properties of tanned leathers as affected by tanning material, UCGs extract concentration and
their interaction
Property Moisture Ash pH
Unit % % mmol/L
ASTM D6403 D2617 D2810
Effect of tanning material (T)
UCGs extract 13.21 1.25b 4.43
UCGs extract + synthetic agent 13.19 2.60 a
4.59
Significance ns ** ns
Effect of UCGs extract concentration (C)
20% 13.26 1.53 4.62
30% 13.14 1.95 4.57
40% 13.21 2.29 4.35
Significance ns ns ns
Interaction effect (T × C)
20% 13.27 0.91d 4.30
UCGs extract 30% 13.14 1.33 cd
4.43
40% 13.22 1.52c 4.57
20% 13.24 2.17 b
4.93
UCGs extract +
30% 13.13 2.57ab 4.70
synthetic agent
40% 13.20 3.07 a
4.13
Significance ns ** ns
Overall of means 13.20 1.93 4.51
Standard error of mean 0.04 0.19 0.12
Note: UCGs used coffee grounds. ns – not significant, ** significant at P<0.01. Means in the same column with
different superscripts letter are significantly different (P<0.05).

Table 5. Organoleptic properties of different tanned leather


Grain Grain General
Group Fullness Softness
tightness smoothness appearance
20% UCGs extract 4.6 5 5.8 5.8 6.4
30% UCGs extract 8 7.2 7.8 7.6 7.6
40% UCGs extract 9 7.4 7.8 7.8 8.2
20% UCGs extract + 10% synthetic agent 5.8 6 7.2 7.4 8.4
30% UCGs extract + 10% synthetic agent 8.4 7.4 8.4 8.2 9.2
40% UCGs extract + 10% synthetic agent 9.6 7.8 8.8 8.4 9.4
Note: UCGs used coffee grounds.

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Journal of Ecological Engineering 2023, 24(3), 10–19

CONCLUSIONS processes, applications and possibilities. South Af-


rican Journal of Botany, 135, 58–70.
UCGs extract contains tannins with good tan- 10. Dutta S.S. 2008. An Introduction to the Principles
ning strength. The concentration 40% of UCGs of Leather Manufacture. 4th edition, Indian Leather
extract is highly recommended for use to ac- Techno Association, India.
complish the required shrinkage temperature that 11. Erdem M., Ozverdi A. 2008. Leaching behavior of
should be ≥ 70 °C. UCGs extract could be suc- chromium in chrome shaving generated in tanning
cessfully used as tanning agent in vegetable tan- process and its stabilization. Journal of Hazardous
ning to produce durable leathers with good full- Materials, 156, 51–55.
ness; it could be used in manufacturing different 12. Lina F., Araújo M.E.M. 2018. Vegetable Tannins
products, such as footwear and bags. Moreover, Used in the Manufacture of Historic Leathers. mol-
ecules, 23(1081), 1–20.
using a combination of UCGs extract at any of the
used concentrations with phenol sulfonates 10% 13. FAOSTAT. 2020. Production-Crops data. World
led to significant improvement in leather proper- Food And Agriculture Organization, Rome.
ties as compared with using UCGs extract solely. 14. Galvez J.M., Riedl B., Conner A.H. 1997. Ana-
lytical studies on Tara tannins. Holzforschung, 51,
235–243.
Acknowledgements
15. Guo L., Qiang T., Ma Y., Wang K., Du K. 2020. Op-
Special thanks to Elshafei’s Sons tannery, timisation of tannin extraction from Coriaria nepal-
ensis bark as a renewable resource for use in tanning.
Alexandria, Egypt for supporting in the practical
Industrial Crops & Products, 149(112360), 1–10.
part of this study.
16. Amzad H.M., AL-Raqmi K.A.S., AL-Mijizy Z.H.,
Weli A.M., Al-Riyami Q. 2013. Study of total phe-
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