ABUAD Journal of Engineering Research and Development (AJERD)

ISSN (online): 2645-2685; ISSN (print): 2756-6811

Volume 7, Issue 2, 152-162

Comparative Modelling, Sensitivity Analysis and Thermodynamics Study of

the Adsorption Characteristics of Dried Nauclea latifolia Medicinal Leaves
Abiola John ADEYI

Department of Forest Products and Utilization, Forestry Research Institute of Nigeria, P.M.B. 5054, Jericho Hills Ibadan,
Nigeria
[email protected]

Corresponding Author:[email protected], +2347036800478

Date Submitted: 29/05/2024
Date Accepted: 02/08/2024
Date Published: 12/08/2024

Abstract: The adsorption characteristics of Nauclea latifolia medicinal leaves were examined across selected temperatures (30–50°C)
and water activity levels (0.044–0.900) to assess its storage stability. Both univariate semi-empirical and multivariate statistical models
were comparatively employed to represent and predict the observed adsorption characteristics. Additionally, sensitivity analysis was
conducted to evaluate the dependence of the adsorption characteristics (that is, equilibrium moisture content (EMC (g/g d.b.)) on
temperature and water activity storage factors. The net isosteric heat and entropy of adsorption were also determined alongside
compensation theory values. The results indicated that EMC decreased with increasing temperature and increased with rising water
activity. The minimum and maximum EMC values of 0.015 and 0.221 g/g d.b. were observed at 50 °C. The safe moisture content for
storing dried Nauclea latifolia medicinal leaves was 12.6 g/g d. at 30 to 40 °C and 9 g/g d.b. at 50°C. Amongst the models tested, the
Peleg model demonstrated best performance, with its R² values ranging from 0.9897 to 0.994 and RMSE values between 0.0039 and
0.0129. Sensitivity analysis revealed that EMC is more sensitive to water activity than to temperature. The net isosteric heat and entropy
of adsorption decreased with increasing EMC, indicating that the process was enthalpy-driven. In conclusion, the findings underscore
the importance of environmental management in maintaining the storage properties of Nauclea latifolia medicinal leaves. The results of
the models are useful in guiding the optimal storage conditions and the design of tailored storage facilities for Nauclea latifolia
medicinal leaves.
Keyword: Nauclea latifolia Medicinal Leave, Adsorption, Modelling, Sensitivity Analysis, Storage.

1. INTRODUCTION
Nauclea latifolia is a medicinal plant that is extensively used in traditional African medicine due to its diverse
pharmacological properties [1]. Its leave has been indicated for effectiveness in treating various ailments such as cough,
jaundice, stomach disorders, malaria fever, and cancer [2]. Other traditional uses included managing fever, pain, dental
caries, septic mouth, dysentery, and as an antipyretic and antinociceptive agent [3 - 4]. In post-harvest handlings, drying of
Nauclea latifolia leaves enhances preservation, concentration of bioactive compounds, ease of transportation, and shelf
stability; making it more suitable for medicinal, culinary, and related applications [5]. Hence, a complementary storage
characteristic of Nauclea latifolia leave after drying is essential for sustainable utilization and conservation. Such
investigation entails its hygroscopic behaviour in storage and it the main focus in this study.

The adsorption characteristics of food, drug and herb focus on examining their interactions with environmental
moisture, which is crucial to resource management and environmental impact such as resource efficiency for optimized
storage conditions, spoilage and waste reduction [6]. Hence, optimized moisture absorption practices would promote low
environmental impact such as microbial growth and enzymatic reactions, thereby reducing the need for chemical
preservatives and additives [7], and also minimize the release of harmful substances into the environment; thus promoting
ecological sustainability. Implementing optimal storage conditions can also lead to energy savings by reducing the need for
excessive refrigeration or re-drying processes [8]. Most importantly, adsorption of moisture under various conditions (that
is, sorption isotherm), provides insights into storage stability, quality preservation, and shelf life prediction [6] [9].

It has been established that the sorption isotherms serve an important quantitative indicator [7]. These isotherms
represent the correlation between equilibrium moisture content and relative humidity and offer insights into the distribution
and intensity of water molecule connections within products and their hygroscopic equilibrium [10]. Amongst the methods
available for sorption isotherms interpretation, mathematical models have been emphasized to enhance the description of
these isotherms, with a little less than a hundred equations comprising two or more parameters proposed [7]. Other

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complimentary mathematical model indices such as isosteric heat integral and differential of sorption, compensation theory,
amongst others have also remained crucial indicators that deepen the understanding of storage and drying processes. These
parameters signify the energy released during adsorption/desorption process, and the energy required to disrupt the
intermolecular forces between water vapour molecules and the adsorbent surface [6]. Mathematical models play a major
role in process control and management.

Presently, varied modelling techniques such as empirical/semi-empirical, physics, statistical, artificial intelligence
amongst others are currently in use; however, empirical models are classical, traditional and simple to implement, and are
therefore widely utilized [11]. Although empirical models do not necessarily consider the underlying physical or chemical
mechanism of a process, however, they offer good predictive power and flexibility [6]. Notably, a potent deficiency of
empirical models is the limitation to one-dimensionality. Going forward, statistical mathematical models describe the
relationship between variables (multi-dimensionality) in a dataset. Statistical models encompass both the structure of the
relationship and the associated uncertainty. Statistical models can range from simple linear regression models to complex
hierarchical models, depending on the nature of the data and the research question [12]. It therefore means that statistical
models have capability for modelling multidimensional data, and capture possible factors interaction and uncertainties,
which is impossible for an empirical model. Despite the advantages and disadvantages, modelling efficiency (coefficient of
determination, root means square error and others) remains topmost in determining the successful utilization of a model.
Therefore, comparing the model efficiencies of adsorption characteristics of Nauclea latifolia medicinal leave between
empirical and statistical models is a co-focus in this study.

Sensitivity analysis is such an important post modelling technique to assess the impact of variations in input parameters
or assumptions on the outputs of a model. It helps to identify which input factors have the most significant influence on the
model's predictions or outcomes [13]. Sensitivity analysis is essential for modelling the adsorption characteristics of
biological material, as it will help to identify key parameters, optimize experimental design, quantify uncertainty, assist
process control, on-line controller design and enhance model interpretation.

Storage study and sorption isotherm modelling of leaves, just like any other biological material, is crucial for
understanding the moisture sorption behaviour, which is essential for various applications such as processing,
pharmaceuticals, and agro-forestry. In relevant literatures, Vasileva et al. [14] examined the moisture sorption
characteristics of white mulberry (Morus alba) as a natural alternative to sugar and modelled the observed experimental
data. Sobowale et al. [15] focused on determining the sorption isotherms and heat of sorption of Moringa oleifera leaves,
providing insights into the moisture sorption behaviour. However, a study on sorption isotherm of Nauclea latifolia
medicinal leave, development of alternative multi-dimensional statistical model and post modelling sensitivity analysis are
scarce in the literature. Therefore, the aim of this study was to fill these notable gaps in study.
2. MATERIALS AND METHODS
2.1 Procedure
Nauclea latifolia leaves were obtained from a farmland in Ogbomoso Township (8.133°N latitude and 4.245°E
longitude), Oyo state, Nigeria during raining season (20 th July, 2023). A digital weighing balance (accuracy of ±0.000 g)
and Stangas (SG-9052G, Stangas Luxury Modern Appliances, Italy) oven and glass jars were used for measurements,
drying purposes and equilibration of samples, respectively. Physically sound leaves were utilized for the experiment. The
leaves (1 kg) were washed in distilled water and air-dried in the laboratory environment (27 – 30°C) for 1 h prior to oven
drying at 70°C for 10 h. The dried leaves were then packed and stored in a glass bottle for one day until the next
experimental phase.
2.2 Investigation of Adsorption Characteristics
The equilibrium moisture content of Nauclea latifolia leaves at 30, 40, and 50°C were determined using a gravimetric
technique in accordance with the method of Heras et al., (2014) [16]. This method relies on saturated salt solutions to
maintain a constant relative humidity in the surrounding air. Six saturated salt solutions (KOH, MgCl 2, K2CO3, NaNO3,
KCl, and BaCl2) were prepared by dissolution in distilled water at a higher temperature (50°C) to ensure saturation upon
cooling (29°C). Glass jars (1 litre each) with insulated lids were utilized for the experiment. Each jar was filled one-quarter
full with a prepared saturated salt solution, maintaining a layer of solid salts throughout the equilibration period. A tripod
was placed in each jar to hold Nauclea latifolia leaves samples. These solutions provided a range of water activity from
0.07 to 0.89. Leaf samples (0.005 g ±0.001 g) were weighed and placed in the jars with the saturated salt solutions. The
jars were tightly sealed and placed in the oven at specified temperatures (30, 40, 50°C) for equilibration. Samples were
weighed daily until no further mass change occurred (7 days). The equilibrated samples were then brought out of the jar
and oven dried at 105°C for 24 h. The difference in mass before (𝑚𝑏 ) and after (𝑚𝑎 ) oven drying allowed calculation of
the moisture content (𝑚𝑒 ) at hygroscopic equilibrium with Equation 1.
𝑚𝑏 −𝑚𝑎
𝑚𝑒 = (1)
𝑚𝑎

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2.3 Univariate Empirical Modelling of Sorption Kinetic

Univariate modelling refers to the analysis and modelling of data that consists of observations on a single characteristic
or attribute [17]. Empirical models are univariate and are generally less computationally demanding. This allows for faster
model development and analysis, particularly when dealing with datasets of limited size [18]. In this study, four semi-
empirical models with independent characteristic of time (t) and parameters/constants were utilized to understand,
represent and explain the adsorption characteristics of Nauclea latifolia leave. The model names and their respective
mathematical composition are represented in Table 1. The univariate empirical modelling was implemented in Matlab
R2014a software.

Table 1: Model utilized for experimental data fitting

Model Model Equation Reference

Name Representation Number
GAB 𝑎𝑏𝑐𝛼 (2) [19]
𝑚𝑒 = (1−𝛼𝑐)(1−𝛼𝑐+𝛼𝑐𝑏)
Henderson – Thompson 𝑚𝑒 = [
𝐿𝑛(1−𝛼) 1/𝑏
] (3) [16]
−𝑎(𝑑+𝑐)
White and Eiring 1 (4) 16]
𝑚𝑒 =
(𝑎+𝑏𝛼)
Smith 𝑚𝑒 = 𝑎 − 𝑏(𝐿𝑛(1 − 𝛼)) (5) [19]
𝑏 𝑑
Peleg 𝑚𝑒 = 𝑎(𝛼) + 𝑐(𝛼) (6) [19]
Caurie 𝑚𝑒 = exp (𝑎 + 𝑏𝛼) (7) [9]
a, b, c and d are the model parameters of the empirical models, while 𝛼 is the water activity

2.4 Multivariate Modelling of Sorption Kinetics

Multivariate modelling is an indispensable tool in various academic disciplines due to its ability to analyze complex
datasets with multiple interacting variables [20][21]. Compared to univariate approaches that focus on single variables,
multivariate models offer understanding of factors interaction that deepens relationship understanding and identification of
latent variables [22]. In this study, multi-linear regression modelling was implemented in Design Expert 6 software. Multi-
linear regression is a powerful tool used to model the relationship between a continuous dependent variable and two or
more independent variables [23].

The multivariate model is represented by Equation (8)

Y = β𝑜 + β1 𝑋1 + β2 𝑋2 + … . + β𝑛 X𝑛 + ε (8)

Where: the dependent variable (Y) is expressed as a linear combination of the independent variables (𝑋1 to X𝑛 ) along with
an error term (ε). The coefficients (β) represent the regression coefficients, which quantify the individual effect of each
independent variable on the dependent variable, holding all other variables constant [20]. The error term (ε) accounts for
unexplained variance in the data, which could be due to random error, measurement inaccuracies, or the influence of other
variables not included in the model [23].
2.5 Modelling Efficiency
The efficiency of the models were determined using statistical indicators, including the sum of squared error (SSE),
coefficient of determination (R2) and, root mean square error (RMSE). A lower SSE and RMSE with a higher R2 (usually
ranged from 0 to 1) indicate a better fit and their respective mathematical representations are depicted in Equation. (9) –
(11) [24][25].

SSE = ∑ni=1(Pred, i − Exp, i)2 (9)

2
(Pred,i–Exp,i)
R2 = 1 – (∑𝑛𝑖=1 2 ) (10)
(Pred,i– AverageExp)

2
∑𝑛
𝑖=1(Exp,i– Pred,i)
RMSE =√ (11)
𝑁

Where: Pred,i is the 𝑖𝑡ℎ predicted value, Exp,i is the ith experimental value and AveragedExp is the average of all the
experimental value. n represents the number of observations.

2.6 Net Isosteric Heat of Sorption and Differential Entropy of Sorption

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The thermodynamics properties are generally evaluated from moisture sorption data with the Clausius-Clapeyron
equation [19] as represented by Equation (12).

∆ℎ𝑑 ∆𝑆𝑑
[−𝐿𝑛(𝛼)]𝑀 = − (12)
𝑅𝑇 𝑅

Where: 𝛼 is the water activity, M is the moisture content, R is the gas constant, T is the temperature, ∆ℎ𝑑 is the net
isosteric heat of sorption and ∆𝑆𝑑 is the differential entropy of sorption.

1 −∆ℎ𝑑
By plotting 𝐿𝑛 (𝛼) versus , for a given moisture content (M), ∆ℎ𝑑 is determined from the slope of Equation (12) i.e. ,
𝑇 𝑅
∆𝑆𝑑
and ∆𝑆𝑑 is determined from the intercept of Equation (12) i.e. .
𝑅

When this is applied at different moisture contents, the dependence of ∆ℎ𝑑 and ∆𝑆𝑑 with moisture content can be
determined.

2.7 Enthalpy – Entropy Compensation Theory

The compensation theory proposes a linear relationship between ∆ℎ𝑑 and ∆𝑆𝑑 as represented in Equation (13) [10].

∆ℎ𝑑 = 𝑇𝛽 𝑋 ∆𝑆𝑑 + ∞ (13)

Where: 𝑇𝛽 is the isokinetic temperature, ∞ is the free energy

In order to validate the applicability of this theory to the thermodynamic properties of Nauclea latifolia medicinal
leaves, Krug’s method was employed to juxtapose the constant rate temperature 𝑇𝛽 with the harmonic average
temperature𝑇ℎ𝑚 . If 𝑇𝛽 equals 𝑇ℎ𝑚 , the theory can effectively elucidate the driving mechanism behind the process. In
instances where 𝑇𝛽 surpasses𝑇ℎ𝑚 , the adsorption process is primarily driven by enthalpy; conversely, when 𝑇𝛽 is less than
𝑇ℎ𝑚 , the adsorption process is pre-dominantly entropy-driven. The equation for the harmonic average temperature, 𝑇ℎ𝑚 , is
delineated in Equation (14) [10].
𝑁
𝑇ℎ𝑚 = 1 (14)
∑𝑁
𝑖=1 𝑇

Where: 𝑁 is the number of isotherms

2.8 Sensitivity Analysis

The sensitivity analysis was implemented in Python 3 using uniform assumption to determine the importance of each
input variable for the observed moisture adsorption properties of Nauclea latifolia leaf at different storage temperatures
and relative humidity. The derived multi-dimensional statistical model assisted in sensitivity analysis.

3. RESULTS AND DISCUSSIONS

3.1 Adsorption Characteristics
The moisture absorption characteristics of Nauclea latifolia leaves in this study are represented in Figure 1.

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Figure: 1: Moisture adsorption characteristics of Nauclea latifolia

The figure showed that the moisture adsorption characteristics of Nauclea latifolia leave conforms to the typical type II
sigmoidal shaped curve in accordance with Brunauer's classification [19], which is common to food materials. The
equilibrium moisture content increased with increment in water activity and reduced with increment in temperature which
is also consistent with the observation of Akoy and von Hörsten, (2013) [26]. The least EMC was 0.015 found at 50°C and
water activity level of 0.044 while the highest EMC was 0.313 found at 30°C and water activity level of 0.9. The observed
increase in equilibrium moisture content as water activity increased is attributed to increased average molecular weight of
the mobile water fraction of the solution. Hence, the elevated water activity enhanced the mass transfer driving force
between the materials and surrounding water molecules. This effect amplifies the potential for water molecule migration
on the material's surface, potentially leading to the phenomenon of multi-molecular layer water adsorption [27].

The decreasing effect of the elevated temperature on the equilibrium moisture content can be attributed to the fact that
elevated temperature induces both physical and chemical alterations within the material matrix. This disrupts the
established equilibrium between the material's hydrophilic and hydrophobic moieties, leading to a decrease in the number
of adsorbed water molecules [15]. Then, the equilibrium moisture content shifted towards a lower water holding capacity.
Similar results were documented with persimmon leaves [16].

In storage, water activity (α) is a critical factor governing the reproduction and proliferation of microorganisms. Its
value directly influences the quality characteristics and storage stability of food products [10]. Studies, such as the work by
Yu et al. (2016) [28], have demonstrated that microbial growth, encompassing bacteria, yeasts, and molds, is significantly
inhibited when α falls below 0.7. Notably, a further decrease in Α to values below 0.6 appears to render most
microorganisms within the food matrix incapable of survival. Based on this established knowledge, the present study
adopted α values of 0.65 as reference indices for safe moisture content in dried Nauclea latifolia. At this value, the safe
moisture content for Nauclea latifolia is 12.6 (g/g d.b.) for 30 and 40°C storage temperatures and 9 (g/g d.b.) for 50°C
storage temperatures. Ruan et al. (2022) [10] reported a safe moisture content of 18.77 - 15.60%, and the relative safe
moisture content of 14.6 – 11.06% for microwave vacuum dried Tilapia, and acknowledged that the finding was critical to
deciding the drying endpoint of tilapia and other biological materials and for choosing storage conditions.
3.2 Univariate Empirical Modelling of the Adsorption Characteristics
Table 2 presented the fitted empirical equations and their respective derived parameters with model performances.

Table 2: Model parameter and performance

Model Model Adsorption Temperature oC

Name Parameter
30 40 50
GAB a 0.0527 1.9470 0.0496
b 77.4700 0.0929 8.2100
c 0.9253 1.0270 0.9123
R2 0.9991 0.9833 0.9878
RMSE 0.0039 0.0175 0.0114
White and Eiring a 19.6000 20.5500 26.1300
b -18.2500 -19.6800 -25.2600
R2 0.9980 0.9933 0.9614
RMSE 0.0050 0.0096 0.0176
Peleg a 0.1044 0.4171 0.2840
b 0.2991 5.6080 5.9040
c 0.3870 0.1072 0.1180
R2 0.9994 0.9997 0.9897
RMSE 0.0039 0.0024 0.0129
Smith a 0.0247 0.0166 0.0098
b 0.1185 0.1291 0.1051
R2 0.9819 0.9828 0.9832
RMSE 0.0156 0.0154 0.0116
Caurie a -3.6850 -3.8090 -4.0000
b 2.7330 2.9250 2.8720
R2 0.9699 0.9797 0.9791
RMSE 0.0201 0.0167 0.0129

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Based on the performance indicators in the table, Peleg model showed the best efficiency in explaining the
experimental data at all studied temperatures due to its highest R2 and lowest RMSE values while Caurie model showed the
least performance. Generally, a model with R2 value greater than 0.7 within the limit of 0 (zero) – 1 (unity) is considered
acceptable [27].

In the study of moisture sorption isotherms and heat of sorption of Algerian Bay leaves (Laurus nobilis), Ouafa et al.,
(2015) [19] also found Peleg model to be the best fitting model for describing the experimentally observed sorption curves.
3.3 Multivariate Statistical Modelling of the Adsorption Characteristics
The developed multivariate model developed for the equilibrium moisture content (EMC (g/g d.b.)) in this study is
presented in Equation (15)

EMC (g/g d.b.) = 0.1660 + 0.0575 * α - 0.0119 * B - 0.4071 * α2 + 1.5878E-004* B2 + 1.4328E-003* α * B (15)

Where: α = Water activity, and B = Temperature (°C)

The model is based on a second-order polynomial regression equation. The intercept of the equation (0.1660),
represents the baseline EMC value when both independent variables α and Bare zero. The linear term represents the effect
of the variable α and B on the EMC in a linear fashion. The 0.0575 coefficient for α indicates the rate of change in EMC
per unit change in α. The -0.0119 coefficient for B suggested that B has a negative effect on EMC, by decreasing EMC
with each unit increase in B. The quadratic term represents the nonlinear effect of α and Bon EMC. The negative nonlinear
coefficient of α indicates that the relationship between α and EMC is concave (relative to x-axis), suggesting diminishing
returns. The positive non linear coefficient of B implied a convex (relative to x-axis) relationship, suggesting accelerating
effects or sensitivity at higher values of B. The interaction term (1.43283E-003 * α * B) captures the combined effect of α
and Bon EMC. The positive coefficient suggests that the presence of one variable enhances the effect of the other on EMC.
On the overall, the Equilibrium Moisture Content (EMC) is a critical property of materials such as agricultural products,
indicating the moisture level at which the material is in equilibrium with its surrounding environment. Understanding and
predicting EMC is crucial for processes like drying, storage, and quality control.

The performance of the multivariate statistical model used in this study is represented in Table 3

Table 3: Analysis of variance of the multivariate statistical model

Source Sum of df Mean F Prob > F Remark Value

Squares Square Value
Model 0.14 5 0.029 55.70 < 0.0001 Significant
α 0.11 1 0.11 217.98 < 0.0001 Significant
B 2.465E-003 1 2.465E-003 4.82 0.0486 Significant
α *B 2.096E-004 1 2.096E-004 0.41 0.5342 Non- significant
α2 0.013 1 0.013 25.30 0.0003 Significant
B2 1.007E-003 1 1.007E-003 1.97 0.1861 Non- significant
Residual 6.141E-003 12 5.118E-004
Cor Total 0.15 17
R-Squared 0.9587
Adj R-Squared 0.9415
Pred R-Squared 0.9096
Adeq Precision 19.898

The Model F-value is a measure of the significance of the overall model. A high Model F-value, such as 55.70 in this
case, means that the model is significant, with extended meaning that the variables (water activity and temperature)
included in the model have a meaningful impact on the equilibrium moisture content. There is a low (only a 0.01%, that is
Prob>F value of 0.0001) chance that a Model F-Value this large could occur due to randomness without any actual
relationship between the variables and the response.

The Prob > F value measures the probability of observing an F-value as extreme as the one obtained under the null
hypothesis (i.e., no significant relationship), the Prob > F value less than 0.05 suggests that the model terms are significant,
while values greater than 0.10 indicate that the model terms are not significant. In this case, the terms α (water activity), B
(equilibrating temperature), and α2 (square of water activity) are deemed as significant model terms, as their associated
Prob > F values are below 0.05. Notably, the insignificance of factor α*B showed that there was no interaction between the
water activity and equilibrating temperature, therefore the two factors affected the equilibrium moisture content differently.

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In addition, the R-squared (R2) value is 0.9587 in this study. Comparatively, the R2 value of this statistical model is
lower than the R2 value of the best performer of the univariate empirical model (that is, Peleg model), however, the model
assisted in gaining more insight into the process such as effect of each contributory factor in the linear and non-linear
region and possible interaction of factors. Such gain and flexibility are useful in automation, monitoring, sensitivity
analysis, and control of the process considering the model’s compactness. The Pred R-Squared (Predicted R-Squared) of
0.9096 indicates the proportion of the variance in the response variable that is explained by the predictors in the model,
while the Adj R-Squared (Adjusted R-Squared) of 0.9415 adjusts the R-squared value for the number of predictors in the
model, providing a more accurate estimate of model fit.

The statement Adeq Precision measures the signal-to-noise ratio, indicating how well the model predicts the response
relative to the inherent variability in the data. A ratio greater than 4 is considered desirable, suggesting that the signal (that
is, the meaningful information) is much stronger than the noise (that is, random variation). In this result with a ratio of
19.898, the signal-to-noise ratio is high, indicating that the model provides an adequate representation of the relationship
between the predictors and the response variable. Therefore, the model is suitable for navigating the design space, implying
that it can be reliably used for making predictions or drawing conclusions about the system under study.

The contribution of each factor (that is, α - water activity, and B - equilibrating temperature) is graphically represented
in Figure 2, based on the implication of the statistical model.

Perturbation
0.313
αA

0.2385
EMC (g/g d.b.)

0.164

B
0.0895

B
Aα

0.015

-1.000 -0.500 0.000 0.500 1.000

Deviation from Reference Point

Figure: 2: Effect of water activity (factor α) and temperature (factor B) on moisture adsorption of Nauclea latifolia

The graph complements the observation seeing in Figure 1 where increment in water activity factor increased the
equilibrium moisture content significantly. The increment was a little reluctant in the beginning, thereafter, the moisture
gain improved drastically. On the contrary, increment in temperature factor had an initial slight increment on the moisture
gain before significant decrease in the moisture gain. Comparatively, the effect of water activity increment looked more
critical to moisture gain than the effect of temperature increment. Ruan et al., (2022) [10] derived R2 value of 0.9559 with
Mod-BET for 30 °C sorption isotherms of microwave vacuum dried Tilapia fillets.
3.4 Model Comparison
Comparing the univariate and multivariate models used in this study, it was observed that both modelling approaches
demonstrated strong performance, as evidenced by their statistical metrics, such as the R 2 and RMSE values shown in
Tables 2 and 3. The univariate models slightly outperformed the multivariate model in these metrics. However, the
multivariate model offers a more compact representation of the process variables by incorporating them simultaneously,
whereas the univariate models consider each variable separately. This compactness allows the multivariate model to
capture not only the individual effects of the process variables but also their interactive (or combined) effects. Such a
compact representation is essential for post-modelling operations, including optimization and effective process controller
design, among other applications.

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3.5 Sensitivity Analysis

Sensitivity analysis of process factors evaluates how changes in independent variables affect a dependent variable
within a given set of assumptions. In the context of processes, it assesses the impact of variations in factors such as input
parameters, operating conditions, or environmental variables on the output or performance of a process. Through the
adjustment of one factor at a time while keeping others constant, sensitivity analysis identifies critical factors influencing
process outcomes. This method enhances decision-making by quantifying the degree of uncertainty and helps in optimizing
process performance and resource allocation. In this study, the sensitivity analysis of the adsorption characteristics of
Nauclea latifolia leaf is represented in Figure 3.

Figure 3: Sensitivity analysis of Nauclea latifolia leaf adsorption

The figure showed that temperature has the highest contribution to the variability of the equilibrium moisture content of
Nauclea latifolia leaf followed by water activity. This is important information for dried Nauclea latifolia leaf storage
facility design and control. In the study of Adeyi et al. [25] on the sensitivity analysis of the effective moisture diffusivity
of fish cracker, it was found out that oven temperature had the highest contribution to effective moisture diffusivity
followed by oven air velocity and sample thickness.
3.6 Thermodynamics Characterization
The net isosteric heat of sorption (∆ℎ𝑑 ) and differential entropy of sorption (∆𝑆𝑑 ) in this study are represented in Figure
4.

25
∆Sd (J/mol.K)

20
∆Sd = 105.9e-0.16 EMC
15 R² = 0.991
∆hd (kJ/mol.K)

10
∆hd = 28.28e-0.13EMC
R² = 0.996
5

0
8 13 18 23 28 33
Equilibrium moisture content (% d.b.)
∆hd ∆Sd

Figure 4: the integral enthalpy and entropy of Nauclea latifolia leaves

The net isosteric heat of sorption is a critical thermodynamic parameter essential for understanding the interaction
between moisture and food materials. It is also instrumental in analyzing the drying process and assessing the stability of
foods under specific storage conditions [29]. As illustrated in Figure 4, the net isosteric heat of sorption (blue line) exhibits
an exponential decline with increasing equilibrium moisture content. At low levels of equilibrium moisture content,
however, the net isosteric heat of sorption remained high. This phenomenon can be attributed to the abundance of active
sites within the Nauclea latifolia leave, which results in a strong adsorption force between the Nauclea latifolia leave and
water molecules. Therefore, at lower moisture content, the material can effectively adsorb water due to the high number of
active sites available for adsorption. This means the material has a strong capacity to attract and hold water molecules

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when it is relatively dry. As the material becomes more saturated with moisture, its ability to adsorb additional water
decreases significantly. The observation is fitted to the exponential model for prediction and the model is represented on
Figure 4 with high prediction efficiency of R2 = 0.996. These results were close to the report of Ouafa et al. [19].
Furthermore, Figure 4 showed the trend of the differential entropy of sorption (red line) obtained in this study. An
increase in the equilibrium moisture content of materials leads to a decrease in the differential entropy. This decrease is
related to the presence of numerous adsorption sites in Nauclea latifolia leaves at low moisture content, which implied a
strong moisture absorption capacity at that state. At higher moisture content levels, few adsorption sites are available and
the adsorption shifts to a multi-molecular layer, leading to a reduced moisture absorption capacity. This result reinforces
the indication that differential entropy can serve as a reference parameter for quantifying the hygroscopicity of materials
during storage. The observation is fitted to the exponential model for prediction and the model is represented on Figure 4.,
with high prediction efficiency of R2 = 0.991. This result conforms to the report of Heras et al. [16].
3.7 Enthalpy – Entropy Compensation
The entropy-enthalpy compensation theory is crucial for analyzing the mechanism of water adsorption in material, and
for understanding the associated physical and chemical changes. Linear regression fitting of differential entropy and net
equivalent adsorption heat in the adsorption test of Nauclea latifolia medicinal leaves as presented in Figure 5 yielded a
high fitting degree with R² = 0.999, indicating the presence of entropy and enthalpy compensation.
The values of 𝑇𝛽 and α were 407.4 K and 0.192 J/mol, respectively. According to Equation (14), the harmonic average
temperature 𝑇ℎ𝑚 was 307.78 K. Since 𝑇𝛽 and 𝑇ℎ𝑚 were not equal, the entropy-enthalpy compensation theory is valid for
this experiment, and thus applicable to the adsorption process of Nauclea latifolia. Furthermore, since 𝑇𝛽 >𝑇ℎ𝑚 , it can be
concluded that the water adsorption process in Nauclea latifolia is enthalpy-driven. In addition, ∞> 0, implying that the
adsorption process is non-spontaneous and requires energy input. Therefore, regulating the environmental energy can
reduce the possibility of deterioration, thereby ensuring the quality of the processed and stored products. This result
conforms to the report of Silva et al. [9], Ruan et al. [10], and Oyelade et al. [13].

7
y = 407.48x + 0.1929
∆Sd (kJ/mol.K)

6 R² = 0.9993

0
0 0.005 0.01 0.015 0.02
∆hd (kJ/mol.K)

Figure 5: Relationship between differential entropy and net isometric heat (enthalpy) of adsorption

4. CONCLUSION
The study focused on the adsorption characteristics of dried Nauclea latifolia leave, examining its behaviour across
different temperatures and water activity levels to assess shelf stability. Various models, including univariate semi-
empirical and multivariate statistical models, were comparatively used to represent and predict the adsorption
characteristics. Post modelling sensitivity analysis highlighted the dependence of equilibrium moisture content to water
activity. The study also analyzed the net isosteric heat and entropy of adsorption. The Peleg model demonstrated superior
performance, with coefficient of determination (R²) values ranging from 0.989 to 0.994. The safe moisture content for
storage was determined to be 12.6 g/g d.b. at 30 - 40°C and 9 g/g d.b. at 50°C. The net isosteric heat and entropy of
adsorption indicated an enthalpy-driven process. In conclusion, the findings emphasized the importance of environmental
management for maintaining proper storage of Nauclea latifolia leaves and provided required knowledge for its stable
storage condition.

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