Impacts of different drying strategies on drying characteristics, the retention of bio-active ingredient and colour changes of dried Roselle Thing Chai Tham, Mei Xiang Ng, Gan Shu Hui, Lee Suan Chua, Ramlan Aziz, Luqman Chuah Abdullah, Sze Pheng Ong, Nyuk Ling Chin, Chung Lim Law PII: DOI: Reference:
S1004-9541(17)30162-3 doi:10.1016/j.cjche.2017.05.011 CJCHE 836
To appear in: Received date: Revised date: Accepted date:
7 February 2017 26 May 2017 27 May 2017
Please cite this article as: Thing Chai Tham, Mei Xiang Ng, Gan Shu Hui, Lee Suan Chua, Ramlan Aziz, Luqman Chuah Abdullah, Sze Pheng Ong, Nyuk Ling Chin, Chung Lim Law, Impacts of different drying strategies on drying characteristics, the retention of bio-active ingredient and colour changes of dried Roselle, (2017), doi:10.1016/j.cjche.2017.05.011
This is a PDF file of an unedited manuscript that has been accepted for publication. As a service to our customers we are providing this early version of the manuscript. The manuscript will undergo copyediting, typesetting, and review of the resulting proof before it is published in its final form. Please note that during the production process errors may be discovered which could affect the content, and all legal disclaimers that apply to the journal pertain.
ACCEPTED MANUSCRIPT Separation Science and Engineering IMPACTS OF DIFFERENT DRYING STRATEGIES ON DRYING CHARACTERISTICS, THE ☆
IP
T
RETENTION OF BIO-ACTIVE INGREDIENT AND COLOUR CHANGES OF DRIED ROSELLE
SC R
Thing Chai Tham1, Mei Xiang Ng2, Gan Shu Hui3, Lee Suan Chua4, Ramlan Aziz5, Luqman Chuah Abdullah6, Sze Pheng Ong7, Nyuk Ling Chin8 and Chung Lim Law9
Department of Chemical Engineering, The University of Nottingham, Malaysia Campus
NU
1,2,3,7,9
Jalan Broga, 43500 Semenyih, Selangor D.E, Malaysia
4,5
MA
Tel.: +6(03)-89248169 Email:
[email protected]
Institute of Bioproduct Development, Universiti Teknologi Malaysia, 81310, UTM, Johor Bahru,Skudai,
Department of Chemical and Environmental Engineering, Universiti Putra Malaysia, 43400 UPM Serdang, Selangor, Malaysia
Department of Process and Food Engineering, Universiti Putra Malaysia, 43400 UPM Serdang, Selangor,
AC
8
CE P
6
TE
D
Malaysia
Malaysia
Abstract: The drying kinetics of Roselle (Hibiscus sabdariffa. L) of variety Terengganu (UMKL-1) and the quality attribution of Roselle were studied. The experiments were conducted using four different drying methods, including solar greenhouse drying (SD), solar greenhouse with intermittent heat pump drying(SIHP), hot air drying (HA) and heat pump drying (HP). Among the four drying methods, HP achieved the highest drying rate at a range from 0.054 g H2O·(g DM)-1·min
-1
-1
to 0.212 g H2O·(g DM)-1·min
while SD had the
-1
lowest drying rate, measured at 0.042 g H2O·(g DM)-1·min . The analysis on colour kinetics revealed that there is no significant colour loss (p >0.05) observed from HP’s dried Roselle. Greater amount of flavonoids compounds i.e. protocatechuic acid was found in SD and SIHP dried finished product whereas HP’s dried Roselle contains
ACCEPTED MANUSCRIPT ☆
Supported by the Ministry of Agriculture (MOA), Malaysia (NER 30001).
higher percentage of catechin as compared to other drying methods.
SC R
IP
T
Keywords: Hibiscus sabdariffa L., drying, heat pump, total colour change, protocatechuic acid, catechin
1.0 Introduction 1.1 Roselle and its medicinal uses
NU
Roselle (Hibiscus sabdariffa L.) is recognized as a tropical shrub which belongs to the family Malvaceae. Roselle can be found in tropic and sub-tropic regions such as India, Indonesia and Malaysia. This herbaceous
MA
subshrub can grow up to 2.4 m tall with cylindrical red stems. The flowers of Roselle are typically red in calyx consisting of five large sepals with a collar (epicalyx) of 8 to 12 pointed bracts around the base[1]. The fleshy
D
base of the flower (the calyx) can be processed into food products[2, 3] to make syrup, refreshing drinks, jellies,
TE
wine, jams and natural food colourants [4-6]. Roselle has been widely used in local medicines and food. The leaves or calyces are traditionally prepared in fusion as they are rich in anthocyanins, which has antioxidant
CE P
property and is useful in diuretic and sedative treatment [7-10]. In fact, the flavonoid compounds of Roselle varies between studies, probably due to genetic, environmental, ecology and harvest conditions of the plant[11]. Studies have reported that the concentration of ascorbic acid of Roselle is 2.5, 3 and 9 times higher compared to
AC
that of blackcurrant, grapes and citrus, respectively[12]. It is also recommended to use Roselle as a folk remedy for abscesses, bilious conditions, cancer, cough, debility, dyspepsia, dysuria, scurvy and strangury [13, 14]. Roselle contains polyphenols of the flavonol and flavanol type in simple or polymerised form. Protocatechuic acid (PCA), a phenolic compound containing a 3,4-dihydroxy substructure, is a compound that naturally occurs in the dried flower of Roselle. It has demonstrated strong healing functions owing to its strong antioxidant and antitumor promotions effects[15, 16] .Besides, the antibacterial effects of PCA against food spoilage bacteria was investigated by Chao et al[17]. Other than PCA, this research paper also considers another type of flavonoid, named as catechin. Catechin is a flavan-3-ol, a type of natural phenol, antioxidant as well as plant secondary metabolite. Cocoas and teas, especially those species derived from the tea plant Camellia sinensis are rich in catechin[18, 19]. Catechin, the naturally occurring flavonoid has been proven in preventing human plasma oxidation [20]and
ACCEPTED MANUSCRIPT inhibiting the oxidation of low density lipoprotein[21].Moreover, other researchers highlighted the potent antioxidant of catechin in cardiovascular and metabolic health[22]. In this paper, the effects of drying techniques on the retention of two bio-active compounds i.e. PCA and catechin in dried Roselle were examined and
T
presented.
an economical and clean method for the preservation of
SC R
Over the years, solar energy is well-known as
IP
1.2 Drying of Roselle
agricultural product [23, 24]. Roselle is dried traditionally using solar greenhouse drying (SD) method in which the calyces are naturally dried by spreading over mats or plastic sheets placed directly on the open floor area[25].
NU
With SD method, the calyces are gathered up and kept securely in store during sundown or rainy day and the similar drying process is repeated on the next day until the weather gets better. A typical SD will take
MA
approximately three to four days to dehydrate the crops as it is dependent on ambient condition such as temperature and relative humidity, RH [2, 26]. Nevertheless, the quality of the dried crop from this drying
D
technique is questionable due to the exposure to contaminations, dirt, pest infestation and other external calamities such as rain, and loss by birds. According to Plotto [27] and EcoCrop [28] , rain or high humidity
TE
during the drying process can lower the quality and yield of the calyces. Thus, a change in weather condition can
CE P
result in poor productivity and inconsistency in drying quality of dried products. Thus far, Roselle’s drying technique still dominant by SD [2] and following by hot air drying (HA) [26, 29]. However, there is a lack of research in advanced drying technique to alleviate the aforementioned issues. In this paper, heat pump system
AC
(HP) is considered as an alternate drying solution for Roselle. Unlike SD, HP able to operate independently and maintain the optimum drying condition for a drying chamber. This will help to mitigate those adversities found in SD. Positive results have been reported from various drying investigations on different products including biomaterials with HP [30-33].Similarly, HP has been utilized for herbs drying such as Jew’s mallow, spearmint and parsley [34]. Although dried Roselle have been used and consumed extensively in pharmaceutical or food industry for a long period, literature review shows a lack of information about raw material processing, especially the drying process. Hence, the present work aims at investigating the drying characteristic of Roselle with SD, SIHP, HA and HP. In this case study, a locally built low temperature heat pump assisted dryer was developed to support the drying of Roselle with and without solar drying system. Besides, this research outlines the influence of both ambient condition and drying location on the drying rate of Roselle which are discussed in the following section. With the applications of four different types of drying techniques, this paper: (a) examine the drying
ACCEPTED MANUSCRIPT kinetics of Roselle calyxes and petals; (b) investigate the colour change of dried Roselle; (c) the retention of bioactive ingredient compounds in Roselle.
T
1.3 Weather condition
IP
A tropical country like Malaysia experiences warm-humid equatorial climate, characterised by both high
SC R
temperature and high humidity throughout the year. Temperature at sea level range from 21°C to 32°C, while the annual rainfall varies from 2,000mm to 2,500mm [35]. Furthermore, Malaysia has RH ranges between 70% and 90% [36]. It is rare to have a full day with complete clear sky although this nation has abundant sunshine. On
NU
average, Malaysia receives about 6 hours of sunshine per day[37].Therefore, the effect of change in weather, especially changes in ambient condition must be taken into account to relate the drying rate of the sample.
MA
Effects of weather change on both temperature and RH were measured and recorded.
2.0 Materials and Methods
D
2.1 Preparation of Material
TE
Fresh Roselle of the variety Terengganu (UMKL-1) with a harvest maturity (approximately 85-100 days after sowing) were purchased from the local farmer located at Senggarang, Johor, Malaysia. The seed’s capsule is
CE P
removed from the fresh calyx with a seed’s capsules removing tool. Then, fresh Roselle’s calyces are preserved in a chest freezer (CFR 400B, Ardo, minimal freezing temperature: -24°C, UK) with a room temperature
AC
controlled below 10°C. For comparison, the Roselle’s calyx is further processed into two forms: one group as whole (remain uncut) and another group is cut into petals with a pair of scissors. The dimension of the Roselle was measured with Vernier callipers (Kern Germany, with an accuracy of ±0.01 mm). The calyx consisting of five large sepals has a dimension of( 5± 1.5) cm long and (2.5 ± 0.5) cm of base width. The petal has a thickness of (3.4 ± 0.3) cm of sepal and (6.0 ± 0.2) cm long. During the experiment, the Roselle calyx and petals were prepared with initial sample mass of (20 ±1.5) g (each sample has three replications) and spread evenly on the stainless steel fine wire mesh tray for drying. 2.2 Drying strategies The experiments are carried out in four different types of operating conditions with various dryers including SD, SIHP, HP and HA. Temperature for each experiment was maintained below 45°C to define the low temperature drying for Roselle calyx and petals. On the other hand, the RH of dryers was recorded below 40% in average during the experiment.
ACCEPTED MANUSCRIPT 2.2.1 First condition: Solar drying (SD) and solar with intermittent heat pump drying (SIHP) SD for Roselle was conducted in a solar greenhouse dryer (SGD) located at Sendayan Commodity Development Centre (SCDC), Seremban, Malaysia. The SGD is designed as natural convection mode with no active air
T
provided to the system. A hemisphere SGD was built with steel structure and covered with transparent thin sheet
IP
made from polyethylene. The transparent sheet captures the incoming solar radiation and acts as a heat collector.
SC R
According to Abdullah and Mursalim [38] ‘Solar radiation is transmitted into the entire drying chamber through the transparent structure and since the resulting long wave radiation created within the chamber is opaque to the transparent wall and roof, the accumulated energy will heat the incoming air from the ambient thereby increasing
NU
the chamber temperature. The accumulated heat that transferred and conducted to the interior of room is used for diffusion activities of water and vapour from the centre to the surface of drying specimen. Meanwhile, the
MA
remaining amount of energy is applied for the water evaporation at the surface or lost to the ambient by radiation or convection. Under ambient condition, this process continues until the dried product reaches equilibrium
D
moisture content. On the other hand, heat pump was introduced in SGD to improve the drying time and efficiency. As shown in Fig.1, the heat pump included an evaporator (refrigerant: R-134a), a condenser unit
TE
(water and air cooled), an expansion valve, compressor and an axial blower. The system takes in moisture laden
CE P
air inside the SGD where the humid air is directed towards the cool surface of the evaporator. Then, the moist air is cooled down to its dew point and liquid water is removed. After the water removal, the process air becomes dry. The temperature of the dry air is increased by hot water flowing through a heat exchanger. An axial blower
AC
is supplying constant dry air to the system. The blower tilt approximately 45° from horizontal position to ensure the dry air is distributed across the drying shelves inside the SGD. In intermittent mode, the HP ceases to operate if room RH falls below 50%. The layout of the SGD and drying shelves was illustrated in Fig.1. Basically, the even span SGD facial facing 266° in west direction and 13 units of drying shelves are arranged in series and parallel inside the SGD. Meanwhile, the sample coding in both SD and SIHP are labelled in RRXYZ, where RR: Roselle sample; X: The shelf’s number (2,7 &11); Y: calyx (1) or petal (2) and Z: sample’s number. 2.2.2 Second conditions: Low temperature heat pump assisted dryer (HP) A locally built vertical two chamber HP was applied to examine the drying process of Roselle. As shown in Fig. 2, the HP has an evaporator (BEM-013, refrigerant: R-134a), a condenser unit (water cooled and air cooled), an expansion valve (TEN 2, Danfoss, Denmark), bi-cylinder compressor for cooling (2hp, TFH 4525Y, coolant: R134a, manufacturer: Tecumseh, France) and a 2 hp axial blower. Similarly, the main objective of HP is to maintain drying chamber’s RH and temperature at optimal conditions by extracting excess humid air from wet
ACCEPTED MANUSCRIPT product inside the drying chamber. The system takes in moisture laden air inside the drying chamber which the moist air was directed to the cool surface of the evaporator. Then, the moist air was cooled down to its dew point and condensate which later turn into dehumidified dry air. Waste heat is recovered from the condenser to
T
increase the dry air temperature. If necessary, temperature of the dry air can be elevated through an auxiliary
IP
heater. This extra heat from dry air creates more vapour pressure that enhance the water diffusion from the
SC R
product. Meanwhile, an embedded blower is blowing constant flow of dry air at high volume to remove the free water from the product. Additionally, the vertical drying chambers are air tight to prevent any potential heat losses to the ambient. The HP is equipped with a user-friendly logic panel and user can pre-set drying parameters
NU
for respective experiment. In this HP experiment, the desired RH was set at minimum of 20%, and room temperature controlled by auxiliary heater.
MA
The arrangement of Roselle calyx, C and petal, P inside the HP was illustrated in Fig.3; T, M and B is referring to top, middle and bottom of the HP, respectively. The air flow circulates inside the dryer is from bottom to top
D
across the drying shelves.
TE
2.2.3 Third conditions: Hot air drying (HA)
HA were performed in a laboratory scale hot air circulation universal oven (UNB 500, Memmert, Germany,
CE P
range: 30-220°C with accuracy of 0.5°C). The drying temperature was controlled at 35°C, 40°C and 45°C respectively and (31±0.5)% for oven humidity. The temperature and RH inside the oven were assumed constant
AC
throughout the drying process.
2.3 Measurement of drying room temperature and humidity The drying parameters including temperature and RH were measured with sets of thermos-hygrometer. Two sets of thermohygrometer (EE220, E+E Elektronik GES.M.B.H,Austria, , measuring range (0…100% RH, accuracy ±1.5%RH)/(-40…80°C, accuracy ±0.1°C) ; HygroFlex3-HF3, Rotronic AG, Switzerland, measuring range (0...100% RH, accuracy ±2.0%RH) (-10…60°C, accuracy ± 0.3°K) were installed at both front and rear of SGD to measure temperature and RH over drying time. For HP, a thermos-hygrometer (Omniport 30, multifunctional hand held meter with logprobe, E+E Elektronik GES.M.B.H,Austria, logprobe 31, for RH(0…100% RH, accuracy ±2%RH); temperature (-40…180°C, accuracy± 0.2°C) , was used to measure the temperature and RH inside the chamber. 2.4 Drying characteristic and kinetic profiling
ACCEPTED MANUSCRIPT Each drying sample has three replications and the moisture content loss is determined in accordance to AOAC standard[39]. An analytical balance (ME204; sensitivity 0.1 mg, Mettler Toledo, USA) was used for consecutive weight measurement of the Roselle’s samples. Later, the water activity of dried sample was measured with water
T
activity meter (Pawkit, AquaLab, USA; accuracy:± 0.2). Meanwhile, dried Roselle sample weighed two grams
IP
each from respective drying test was carry out in a universal laboratory oven (UNB 500, Memmert, Germany) at
SC R
105°C for 24 hours to obtain bone dry weight and determine the moisture content in dry basis (db.) The moisture content, Xd of Roselle was determined with reference to the bone-dry weight, Wd expressed in equation (1) as shown below:
𝑊𝑡 − 𝑊d × 100% 𝑊d
NU
𝑋d (% 𝑑𝑟𝑦 𝑏𝑎𝑠𝑖𝑠) =
(1)
MA
For the purpose of graphical presentation, the moisture ratio was defined based on the moisture content (Eqn. 2)[40]. Consequently, the comparison between various set of drying conditions can be done. The moisture ratio,
∅=
𝑋𝑖 − 𝑋eq 𝑋0 − 𝑋eq (2)
CE P
TE
D
∅ of Roselle during drying experiments was calculated by following equation:
X0, represents the original moisture content, Xi is the moisture content at time t, and Xeq is the equilibrium moisture content. Xeq is determined when three consecutive reading were obtained from the experiment. The
AC
initial and final moisture content were tabulated respectively in Table 1. -1
The drying rate (g H2O·(g DM)-1·min ) was determined by approximation of the derivatives to finite differences as shown in Eqs. (3)-(4)[41, 42]. *Drying rate at 𝑡 = 𝑡0 (first point), d𝑋 d𝑡
=
𝑋1 −𝑋0 𝑡1 −𝑡0
(3)
*Drying rate at 𝑡 = 𝑡𝑛 ; 𝑛 = 1, … , 𝑁 − 1 (intermediate point), d𝑋 𝑋𝑛+1 − 𝑋𝑛−1 = d𝑡 𝑡𝑛+1 − 𝑡𝑛−1
(4)
*Drying rate at 𝑡 = 𝑡f (last point),
(5)
ACCEPTED MANUSCRIPT
T
d𝑋 𝑋𝑓 − 𝑋𝑓−1 = d𝑡 𝑡𝑓 − 𝑡𝑓−1
-1
IP
Where 𝑡 is time (min) and 𝑋𝑜 and 𝑋𝑓 are the moisture content (g H2O·(g DM)-1·min ) at initial and equilibrium
SC R
conditions, respectively.
NU
2.5 Colour determination
Various types of drying techniques will have different effects on the physicochemical properties of a dried
MA
product[43, 44]. In this study, the physical property of Roselle i.e. colour is measured with a handheld colour meter (LC100, The Tintometer Ltd, England). Colour was measured at three different sides of Roselle calyx with three replications each on the sample and averaged to obtain the mean and standard deviation reading.
D
Colour data of Roselle calyces and petals is expressed in 𝐿∗ , 𝑎∗ and 𝑏 ∗ values where 𝐿∗ presented as the lightness
TE
coefficient which range from (0 for black to 100 for white), 𝑎∗ ranged positive value of 60 indicates redness, and negative value of -60 indicates greenness). Meanwhile, 𝑏 ∗ (positive value of 60 indicates yellowness while
CE P
negative value of -60 indicates blueness). Then, 𝑎∗ and 𝑏 ∗ were further derived into hue angle via Eq. (6). Generally, fresh Roselle has positive 𝑎∗ and 𝑏 ∗ indicates redness and yellowness of the calyces. Total colour
AC
change of the sample was calculated by using Eqn. 7 [45, 46]. 𝑏∗
(6)
Hue angle = tan−1 (𝑎∗) 1
∆𝐸 ∗ = [(𝐿∗ − 𝐿∗𝑜 )2 + (𝑎∗ − 𝑎𝑜∗ )2 + (𝑏 ∗ − 𝑏𝑜∗ )2 ]2
(7)
in which high degree of colour degradation of dried product was expressed by a high value of ∆𝐸 ∗ . 2.6 Statistical analysis The data of colour and retention of bio-active ingredients were reported in mean ± standard deviation (SD) of triplicate determination. Statistical calculation by SPSS version 22.0 software (IBM Corp, USA) was carried out. Significant differences (𝑝 < 0.05) between means were evaluated by one way ANOVA and Tukey’s range test. 2.7 Quality analysis for bio-active ingredient of Roselle 2.7.1 Extraction process
ACCEPTED MANUSCRIPT Bio-active ingredients from dried Roselle were extracted by reflux extraction method. Reflux extraction method is the most commonly used method to obtain bio-active ingredient from herbs [47, 48]. Dried Roselle was grinded into powder formed prior to the extraction. Two grams of powder were added into 100 ml methanol
T
in a 250 ml round bottom flask equipped with a cooling condenser followed by boiling for 60 minutes. The
SC R
a tight glass bottle and then stored in fridge for further analysis[49].
IP
supernatant was kept dry and filtered by using a membrane filter to get a clear extract. The extracts were kept in
NU
2.7.2 HPLC-PDA
Dried extract was dissolved in methanol (2.5 ml) and 10μl was taken for injection. All samples extracts
MA
were filtered with 0.45 µm nylon filters prior to injection. Two bio-active ingredients i.e. PCA and catechin were analyzed by a high-performance liquid chromatography (Waters Alliance e2695, Milford, MA) system
D
combined with a photo diode array (Waters 2998, Milford, MA). A C18 reserved phase Xbridge column (5 µm
TE
pore size, 4.6 x 250 mm) was used for the separation process. The elution solvents were classified as mobile phase-A (0.1% acetic acid in distilled water) and mobile phase-B (acetonitrile), respectively. The sample were
CE P
eluted according to the following binary gradient: 0-6.5 min - 20% B, 6.5-10 min –80% B, 10-15 min, 80% B, 15-16 min, 20%B, 16-20 min, 20%B. Each sample extract was analysed at the mobile phase with the flow rate of 0.8 mL/min and detector wavelength at 30 o C. Data were integrated by the software of Empower 3 (Waters
AC
Corporation, USA). All bio-active ingredients were quantified using the external standard method.Quantification was based on the peak area[50]. A serial of standard solution with different concentration ranging from 1 – 500 ppm was prepared for calibration curve. 3.0 Results and discussion 3.1 Drying characteristic of Roselle In this study, the drying profile of Roselle comprises the reduction of moisture content and the change of drying rate with time were reported. From Table 1, the initial moisture content for both calyx and petal for each respective experiment was indifferent. However, petal of HP and HA have higher initial moisture content in comparison with both SIHP and SD sample. Whereas, calyx of SD had the lowest initial moisture content among others. The variation of initial moisture content of Roselle samples between studies, probably due to harvest conditions, ecology, conditions of crop, soil type, and environmental effect such as rainfall [11, 51, 52].
ACCEPTED MANUSCRIPT In terms of final moisture content, both HP and HA samples show consistent results for both calyx and petal. This is because the sample was dried in a controlled and confined environment i.e. minimum interruption from ambient change. Conversely, both SD and SIHP samples have bigger variance in final moisture content when
T
environmental factor such as weather change influences the stability of final moisture content at the end of
IP
drying period. As shown in Table 1, corresponding water activities for SIHP and SD were both 0.51; whereas
SC R
HA and HP were measured at 0.52 and 0.54, respectively. Despite slight difference of final moisture content between various drying strategies, however, all the dried samples have approximate water activities well below the maximum threshold (𝑎w < 0.60).These results showed that the low temperature drying able to reduce the
NU
moisture contents to a safe level that could prevent microbial spoilage and minimize deteriorative reactions[53]. 3.2 SD
MA
In Fig. 4, the dried Roselle demonstrated five different stages of moisture reduction trend. The first 400 minutes shows a drastic reduction of moisture followed by modest reduction at between 500 to 1500 minutes. Again, the
D
moisture loss was reported in between 1500 to 2000 minutes before steady plateau was formed near the end of
TE
the drying session. A significant change in moisture content for the first 400 minutes was recorded for petals whereas calyx has slightly lower moisture reduction rate. This drastic change was due to petals (RR721 and
CE P
RR11_21) received higher coverage of solar irradiation especially in the middle and rear of SGD. Additionally, the available surface of petals exposed to the sunlight is bigger than the calyx. According to Fatouh et al.[34], whole plants required longer drying time than that of leaves and drying time increased with increasing surface
AC
area and small size herbs exhibited short drying hour. By comparison, more water loss can be observed from petals than calyx sample. On the contrary, drying temperature was the key parameter that significantly influenced the drying rate[54-56]. Hence, the SGD’s temperature also contributes to the rapid drying of sample. In Fig.9, the temperature of SGD was above 40 °C between 12 pm and 5pm while highest temperature was recorded during 2pm to 3pm.Similar outcome was reported by Rabha et al.[57] where the ambient temperature was found highest during 11 am to 2 pm. In this hour, the solar irradiation position is directly vertical to the sample at the noon while slightly slanted during late afternoon. In terms of drying rate, both calyx and petal at front of SGD (RR211 and RR221) recorded highest drying rate at -1
-1
0.036 g H2O·(g DM)-1·min and 0.042 g H2O·(g DM)-1·min , respectively at the first 20 minutes of drying. In Fig. 5, the sharp increase in drying rate within a short duration was in fact due to the sample position at the SGD in which samples received maximum amount of solar irradiation and causing temperature raise and rapid water
ACCEPTED MANUSCRIPT losses. In the meantime, calyx samples only have proximate moisture reduction trend and slower moisture loss rate when compared to that of petals. It was observed that an unsteady drying rate trend happened from 0 to 335 minutes. The major cause for this
T
unusual trend was due to weather interference such as cloudy day and rainfall that will increase the room RH.
IP
Besides, this phenomenon can be explained by the shifting of solar irradiation pointing from west of SGD (refer
SC R
to Fig.1) during late afternoon. In this case study, increasing trend of drying rate was observed in subsequent days falls between 1500-2000 minutes and at 3000 minutes, respectively as an effect of hot weather during the mid-day. However, these drying rates were insignificant in comparison with the drying rate obtained from the
NU
first day of drying as most of the free moisture was removed. Low drying rate was observed at 695-1500 minutes and 2100-2800 minutes, respectively suggested the sample’s moisture migration was dominated by internal
MA
diffusion. On the other hand, the total drying time for petals was 67.5% shorter than the calyx in the same drying condition. In fact, agricultural product dried with SD usually consumed longer drying hours e.g. four days for tomato[58] ,35 h for Roselle[59], 193 h for ghost chilli pepper [57].
D
Fig.6 illustrated the variation of temperature and relative humidity recorded in SGD when SD was employed.
TE
Average temperature recorded from the SGD from SD was( 40.16±7.24)°C, whereas RH was (37.56 ±15.06) %. As aforementioned, the interference of cloudy weather has adverse effect toward the drying temperature and
CE P
RH[60]. A reduction of SGD temperature is causing the increase of RH. Indirectly, this will slow down the whole drying process. It was observed that the room RH can reach more than 70% over the night as shown in Fig. 9. This is not an ideal drying environment for hygroscopic material such as herb or spices due to its
AC
susceptibility of reabsorb moisture from the surrounding air when humidity is high[61]. The risk of microbial contamination is high if drying by rain or slow drying rate[62]. 3.3 SIHP The performance of a SIHP was influenced by four ambient parameters such as solar irradiation, ambient relative humidity, ambient wind velocity and ambient temperature[63]. Moisture loss profile of both petals and calyx in Fig. 7 exhibited four major falling rate period with a sharp moisture reduction in the first 300 minutes and followed by a constant plateau. The constant plateau indicated a gradual decrease of moisture removal from samples especially at night. Obvious moisture reduction with a steep slope was recorded on the next day of drying and similar pattern occurred in the third and fourth drying period due to overnight drying. Similar result to SD in terms of quicker moisture removal rate of petal than calyx was found in SIHP too.
ACCEPTED MANUSCRIPT Fig.8 depicted highest drying rate was achieved by petal located at middle (RR721) with 0.059 g H2O·(g DM)1
·min-1; however, calyx exhibited lower drying rate despite sharing the same drying location. In comparison to
SD, SIHP’s sample had consistent drying rate in the first 300 minutes. In addition, the fluctuation of drying rate
T
has been minimized and average drying rate for both petal and calyx was slightly higher than SD’s samples. On
IP
the next day, the drying rate for both calyx and petal once again increased and reached as high as 0.017 g H2O·(g
SC R
DM)-1·min-1 for petal and calyx located at the middle section. Similar trend of drying rate was formed in others samples and drying rate of calyx was marginally improved thereafter. Unlike SD, SIHP drying shows constant drying rate in 1700-2400 minutes’ region followed by a small increase of drying rate before it reaching
NU
equilibrium moisture content. This slow drying process can be explained by the domination of internal moisture diffusion mechanism over the external free surface evaporation[63]. With SIHP, the room RH’s was maintained
MA
at desired lower level and hence the water removal rate was consistent even at night drying[34, 64]. Evidently, the drying rate of SD with heat pump assisted had higher drying rate than SD alone.
D
In this case study, the heat pump was set up to operate intermittently when drying room RH rises above 55%.
TE
This has assisted in the continuity of the drying operation at night. When using the SIHP strategy, average temperature and RH inside the SGD were measured at (40.0±6.97)°C and (37.96± 14.17) % respectively. The
CE P
SGD’s drying condition for SIHP was fairly similar to SD deduced a fair comparison between these two experiments. In Fig.9, the room’s RH with HP operated intermittently measured at 57.8%-67% (during night) which was slightly lower than SD (58.4%-75.5%). On the other hand, a huge spike of RH measured at 75.5%
AC
was due to heavy rain that causing higher ambient RH in that particular of drying period. In a nutshell, solar dryer integrated with heat pump warrants sustainable drying performance and shorter drying time with controlled drying condition at low RH. Additionally, the drying rate was extended beyond sunset. Similar observation with different products was reported by Yahya et al.[65],Gan et al.[66] ,Best et al.[67] and Seyfi et al.[68]. 3.4 HP In this experiment, a vertical type two chamber HP was applied to dry Roselle sample without expose them to solar irradiation. As shown in Fig.10, petals demonstrated faster moisture reduction rate in comparison to the calyx flower which have similar outcomes obtained from both SD and SIHP strategy. Besides, it is noteworthy to highlight that the moisture reduction rate was higher for those sample located near the bottom shelf of HP, especially at the first 1000 minutes. At this stage, moisture particles were picked from surface by convective heat transfer. In the air flow design of HP (Fig.3), samples located at bottom shelf received fresh dry air and greater air flow than the top sample. The air turbulence created by recirculating fan inside the dryer helps in moisture
ACCEPTED MANUSCRIPT removal[69, 70]. Eventually, this sample experiences rapid water migration and loss of moisture content. After 1200 minutes of drying hours, the moisture reduction shown insignificant variation as the dried sample either top or bottom has gradually approaching equilibrium moisture content. With HP, the drying time of calyx was
T
shorter by 45.04% and 37.60% in comparison with SD and SIHP respectively. This was supported by the fact
IP
that lowering air relative humidity in the drying air would create a greater drying force for moisture removal on
SC R
the solid surface hence, the increase the drying rate and shorter drying hours[71, 72].
Both petals and calyx were subjected to substantial drying rate as shown in Fig. 11. Petals exhibited significant -1
-1
drying rate ranging from 0.103 g H2O·(g DM)-1·min to 0.212 g H2O·(g DM)-1·min followed by calyx which
NU
was slightly lower than petals. Similarly, the average drying rate for top petal and calyx was lower than bottom sample due to air flow design as aforementioned[70]. However, this phenomenon was only apparent in the
MA
beginning of the drying test. The drying rate of petals and calyx approximate to each other as soon as the drying time reached 400 minutes and above. In other word, the Roselle samples was reaching the falling rate drying
D
period in which the change of moisture was insignificant. In a nutshell, the average drying rate for HP was found
TE
two to three folds faster than SD and SIHP strategy. Other successful testimonials with HP drying were demonstrated by Minea et al. [73] ,Chua et al. [74] and Fatouh et al.[34], respectively.
CE P
For herb application, HP is recommended to operate at temperature lower than 50 °C[75, 76]. It was clearly shown from Fig. 12 that the HP chamber humidity well controlled between (21.1± 3.52) %RH and drying room temperature at (32.1±2.0)°C. The temperature and RH trend demonstrated an increasing and decreasing trend,
AC
respectively during the drying test. However, there was a slight drop in temperature measured in the morning (8 am) of the second day of drying due to a lower ambient temperature at the test venue. Also, the RH recorded below 20% before the sample reach equilibrium moisture content. A sustainable low RH and controlled temperature environment has enhanced the dehydration process of Roselle, thus accelerated the drying rate and drying time is reduced. A reduction in drying time using HP was also reported by Phoungchandang et al. [77] in the drying of lime leaf too. Moreover, the HP helps in minimize the rehydration issue, especially overnight drying through continuous drying at controlled environment.
3.5 HA A universal drying oven (HA) has 30 % shorter drying time in comparison with HP. The oven’s humidity level and temperature were assumed constant over the drying period. The variation of moisture ratio demonstrated that the higher the drying temperature, the faster the moisture reduction in the sample. As illustrated in Fig. 13, petal
ACCEPTED MANUSCRIPT has faster moisture removal rate at 45 °C, however there was no difference in terms of moisture reduction rate in between 35 °C and 40 °C. Saeed et al.[29] reported that at different temperatures (35,45,55 and 65°C ), the drying time was reduced with increased temperature. This suggested that temperature beyond 40°C can improve
T
the moisture removal rate for Roselle.
IP
On the other hand, the drying rate of petals was substantial in the first 30 minutes as illustrated at Fig.14. This
SC R
was mainly due to the continuous hot air circulation inside the oven removes the surface water from the petals which have bigger area exposed to hot air in comparison to calyx. Similarly, the drying rate for the petals dried -1
at 45°C reached highest at 0.11 g H2O·(g DM)-1·min . This was followed by the petal and calyx drying at 40 -1
NU
°C and 45 °C respectively with a drying rate of range of 0.10 g H2O·(g DM)-1·min
or a 10% dropped in the
average drying rate. Likewise, the drying impact of HA was more prominent in petal than the calyx which also
D
3.6 Colour analysis of dried Roselle
MA
applied to SD, SIHP and HP strategies.
TE
Table 2 demonstrated the colour parameters CIE L*, a* and b* values and other derived parameters such as total colour change (ΔE), chroma and hue from different drying methods. Total colour changes, ΔE from solar drying
CE P
(both SD and SIHP) exhibited marginal difference between calyx and petal. Both experiments suggested higher colour change was found in Roselle petal. Conversely, total colour change from HA’s dried calyx was slightly higher (both 35°C and 40°C) than SD and SIHP’s dried calyx. Whereas, HA’s petals exhibited lower colour
AC
changed when 40°C and 45°C was applied, respectively in drying. Instead, the HP dried Roselle are showing consistent colour results particularly in L*, b* and ΔE regardless calyx or petal (p>0.05). The degree of redness (a*) from HP dried sample was higher than sample from others drying strategy, especially with SD’s sample. According to Wong et al.[78], the calyxes comprises of brilliant red pigments of four anthocyanins including dephinidin 3-sambubioside and cyanidin 3-sambubioside as the major pigments and delphinidin 3-glucoside and cyanidin 3-glucoside as the minor ones. The anthocyanins are derivative of the basic flavylium cation structure which are highly reactive and involve in decolourization of the anthocyanin pigments. The rate of anthocyanin decomposition depends on factors such as temperature, oxygen, temperature and etc.[79, 80]. Similarly, drying temperature significantly induced the increase of a* and b* colourimetric parameters due to non-enzymatic browning reaction, which turned the samples more reddish and yellowish when the temperature rise.[44]. This phenomenon was further demonstrated by HA Roselle calyx whereby the a* and b* increased proportionally
ACCEPTED MANUSCRIPT with temperature. On the other hand, the increases of chroma value from all the samples was due to the present of high level of oxygen which stimulated the enzymatic browning reaction between the oxygen[45, 81]. The hue value for dried Roselle measured at between 12° and 19° was indicating a dark red colour of final product. In
T
conclusion, low temperature drying for Roselle warrant a total colour change within 10% (mean value) whereas
IP
HP assures consistency of colour for both petals and calyx.
SC R
3.7 Quality analysis
In Fig.15 (a), HA yield lowest percentage solution of PCA in comparison with other drying methods. The average PCA% was merely (0.0176±0.0006)wt%. The reason for this is unknown but probably caused by the
NU
reaction change such as oxidative degradation during the drying period. Literature reviews suggested that the stability of polyphenols compound can be altered by different conditions such as light, high temperature ,oxygen,
MA
solvents, the presence of enzymes, proteins, metallic ions, or association with other food constituents[82]. Cheng’s investigation in phenolic compound in high temperature water suggested the decomposition of PCA increased with rising temperature and the acids became less stable with longer heating time[83]. In this case
D
study, both SIHP and SD demonstrated high retention of PCA with a highest percentage solution from calyx
TE
measured at SIHP:0.1058 wt% and SD:0.1211 wt%, respectively. From Fig.15 (b), it was noticed that the catechin retention from HPwas two to three times higher than other drying strategies. SD and SIHP have average
CE P
catechin content in both calyx and petals whereas HA recorded low catechin value .According to Li et al, catechin degradation kinetics was affected by RH and temperature, but temperature was the dominant factor[84].
AC
Thus, with lower RH and consistent low drying temperature, the HP can retain more bio-active compounds. By comparing different drying strategies, HA is a less desirable drying method particularly when higher retention of bio-active ingredient is desired. On the other hand, while retaining good amount of PCA content, HP’s dried Roselle also contain high retention of catechin acid among the other drying techniques. Alternately, the solar drying (both SD and SIHP) produced balanced compounds retention between PCA and catechin acid respectively as exemplified in Fig.15.
4.0 Conclusions By comparing the drying kinetics of four different drying methods, the highest drying rate was achieved by HP, followed by HA, SIHP and SD. The results suggested confine dryer such as HP and HA can speed up the drying process and increase the output of the product, meanwhile SD has poor drying performance due to environmental factor e.g. weather condition and product rehydration during overnight drying. Likewise, HP had yield consistent
ACCEPTED MANUSCRIPT red colour of dried Roselle for both calyx or petal which is an added value property to finished product. Although HA had significantly reduced the total drying time of Roselle, the retention of bio-active ingredient was undesirable. HPLC analysis revealed that both SD and SIHP have significant retention of PCA in dried
T
Roselle (𝑝 < 0.05) whereas higher catechin acid was detected in HP(𝑝 < 0.05), followed by SD and SIHP,
IP
respectively. Overall, HP or heat pump assisted solar drying (SIHP) is a better drying option for Roselle as dried
SC R
Roselle could have better colour quality and high retention of bio-active compounds.
5. 6. 7.
8.
9.
10. 11.
12.
MA
D
4.
TE
3.
CE P
2.
Ross, I.A., Medicinal plants of the world: Chemical constituents, traditional and modern medicinal uses. Vol. 1. 2003: Humana Press Inc. Tjukup Marnoto., Endang Sulistyowati., Budiyastuti, P., Sumarwoto, P., M.Syahri., Bambang Sugiarto., Yusuf Hanafi., Girman., and Kristianingrum., Drying of Rosella (Hibiscus sabdariffa) flower petals using solar dryer with double glass cover collector. International Journal of Science and Engineering, 2014. 7(2): p. 150-154. Ashaye, O.A., Studies on moisture sorption isotherm and nutritional properties of dried Roselle calyces. International Food Research Journal 2013. 20(1): p. 509-513. Duke, J.A., Handbook of Energy Crops. 1983, Center for new crops and plants products: Purdue University,Indiana. Esselen, W.B. and Sammy, G.M., Applications for roselle as red color food colorant. Food Product Development, 1975. 9: p. 37-40. Beristain, C.I., García, H.S., and Vazquez, A., Foam mat dehydration of Jamaica (Hibiscus sabdariffa L.) instant drink. Drying Technology, 1993. 11: p. 221-228. Carbajal, O., Waliszewski, S.M., Barradas, D.M., Orta, Z., Hayward, P.M., Nolasco, C., Angulo, O., Sanchez, R., Infanzon, R.M., and Trujillo, P.R.L., The consumption of Hibiscus sabdariffa dried calyx ethanolic extract reduced lipid profile in rats. Plant Food for Human Nutrition, 2005. 60: p. 153-159. Akindahunsi, A.A. and Olaleye, M.T., Toxicological investigation of arqueousmethanolic extract of the calyces of Hibiscus sabdariffa L. Journal of Ethnopharmacology, 2003. 89: p. 161-164. Arroyo, S.F., Inmaculada, C., Rodriguez, M., RaulBeltran-D., Federica, P., Jorge, J., Vicente, M., Antonio, S.C., and Alberto, F.G., Quantification of the polyphenolic fraction and in vitro antioxidant and in vivo anti-hyperlipemic activities of Hibiscus sabdariffa aqueous extract. Food Research International, 2011. 44: p. 1490-1495. Patel, S., Hibiscus sabdariffa: An ideal yet under exploited candidate for nutraceutical applications. Biomedicine & Preventive Nutrition, 2014. 4: p. 23-27. Da-Costa-Rocha, I., Bonnlaender, B., Sievers, H., Pischel, I., and Heinrich, M., Hibiscus sabdariffa L. – A phytochemical and pharmacological review. Food Chemistry, 2014. 165: p. 424-443. Musa, Y., Engku Ismail EA., Yahaya,H., Manual of Roselle's Cultivation Technology (Manual teknologi penanaman rosel). 2006, Kuala Lumpur: Institut Penyelidikan dan Kemajuan Pertanian Malaysia (MARDI).
AC
1.
NU
References
ACCEPTED MANUSCRIPT
17.
18.
19. 20.
24.
25. 26.
27. 28. 29.
30. 31.
T
CE P
23.
AC
22.
TE
D
21.
IP
16.
SC R
15.
NU
14.
Hsieh, C.C., Lee, M.Y., Chen, C.C., Hsu, J.J., Lu, H.K., and Wang, C.J., Hibiscus protocatechuic acid supplementation reducess oxidative stress induced by exhaustive exercise in rat muscle. Journal of Exercise Science and Fitness, 2006. 4(1): p. 59-64. Kakkar, S. and Bais, S., A review on protocatechuic acid and its pharmacological potential. ISRN Pharmacology, 2014. 2014: p. 1-9. Tseng, T.H., Wang, C.J., Kao, E.S., and Chu, H.Y., Hibiscus protocatechuic acid protects against oxidative damage induced by tertbutylhydroperoxide in rat primary hepatocytes. Chemico-Biological Interactions, 1996. 101: p. 137-148. Tseng, T.H., Hsu, J.D., Lo, M.H., Chou, F.P., Huang, C.L., Chu, C.Y., and Wang, C.J., Inhibitory effect of Hibiscus protocatechuic acid on tumor promotion in mouse skin. Cancer Letters, 1998. 126: p. 199-207. Chao, C.Y.Y., M.C., Antibacterial effects of roselle calyx extracts and protocatechuic acid in ground beef and apple juice. Foodborne Pathogens and Disease, 2009. 6(2): p. 201-6. Hammerstone, J.F., Lazarus, S.A., and Schmitz, H.H., Procyanidin content and variation in some commonly consumed foods. Journal of Nutrition, 2000. 130: p. 2086S-92S. Han, X.Z., Shen, T., and Lou, H., Dietary polyphenols and their biological significance. International Journal of Molecular Sciences, 2007. 8(9): p. 950-988. Lotito, S.B. and Fraga, C.G., Catechin prevents human plasma oxidation. Free Radic. Biol.Med., 1998. 24: p. 435-441. Mangiapane, H., Thomson, J., Salter, A., Brown, S., Bell, G.D., and White, D.A., The inhibition of oxidation of low density lipoprotein by (+)-catechin, a naturally occurring flavonoid. Biochem. Pharmacol., 1992. 43: p. 445-450. Teresa, S.d.P., Moreno, D.A., and Viguera, C.G., Flavanols and anthocyanins in cardiovascular health: a review of current evidence. Int. J. Mol. Sci., 2010. 11: p. 1679-1703. Prakash, O. and Kumar, A., Historical Review and Recent Trends in Solar Drying Systems. International Journal of Green Energy, 2013. 10(7): p. 690-738. Miranda, A.C., R.C. Miranda., and Jimenez, J.M., Solar drying system for the agroproducts dehydration. Journal of Agricultural and Social Sciences, 2008. 4: p. 135140. Mady, C. Lietrature review and background information of Bissap (Hibiscus sabdariffa L.). 2010. 9. Daniel, D.L., Huerta Barragan, B.E., Anaya Sosa, I., and Mendoza Vizcarra, M.G., Effect of fixed bed drying on teh rentention of phenolic compounds,anthocyanins and antioxidant activity of roselle (Hibiscus sabdariffa L.). Industrial Crops and Products, 2012. 40: p. 268-276. Plotto, A., Hibiscus: post production management for improved market access. 2004, FAO: Food and Agriculture Organization EcoCrop, Hibiscus sabdariffa var. sabdariffa. 2007, FAO: Food and Agriculture Organization Saeed, I.E., Sopian, K., and Zainol Abidin, Z., Thin layer drying of Roselle (I): Mathematical modeling and drying experiments. Agricultural Engineering International: the CIGR Journal, 2008. X: p. 1-25. Alves-Filho, O. and Strommen, I., Application of heat pump in drying of biomaterials. Drying Technology, 1996. 14: p. 2061-2090. Li, H., Review of the heat pump technologies and applications. 2011, Sheffield University. p. 1-64.
MA
13.
ACCEPTED MANUSCRIPT
35. 36.
41. 42. 43.
44.
45.
46.
47.
48.
D
TE
40.
CE P
39.
AC
38.
MA
NU
37.
T
34.
IP
33.
Kivevele, T. and Huan, Z., A review on opportunities for the development of heat pump drying system in South Africa. South African Journal of Science, 2014. 110(5/6): p. 1-11. Fayose, F. and Huan, Z., Heat Pump Drying of Fruits and Vegetables: Principles and Potentials for Sub-Saharan Africa. International Journal of Food Science, 2016. 2016: p. 9673029. Fatouh, M., Metwally, M.N., Helali, A.B., and Shedid, M.H., Herbs drying using a heat pump dryer. Energy Conversion and Management, 2006. 47(15-16): p. 26292643. SelectiveAsiaLtd. Peninsular Malaysia: Weather & when to go. 2010 [cited 2015 3 August]; Available from: http://www.selectiveasia.com/malaysia-holidays/weather. Romer, U. Climate of the world: Malaysia. 2015 [cited 2015 4 August]; Available from: http://www.weatheronline.co.uk/reports/climate/Malaysia.htm. MetMalaysia. General climate of Malaysia: Sunshine and solar radiation. 2015 [cited 2015 4 August]; Available from: http://www.met.gov.my/web/metmalaysia/climate/generalinformation/malaysia?p_p_i d=56_INSTANCE_zMn7KdXJhAGe&p_p_lifecycle=0&p_p_state=normal&p_p_mo de=view&p_p_col_id=column1&p_p_col_pos=1&p_p_col_count=2&_56_INSTANCE_zMn7KdXJhAGe_page=3. Abdullah, K. and Mursalim, Drying Of Vanilla Pods Using A Greenhouse Effect Solar Dryer. Drying Technology, 1997. 15(2): p. 685-698. AOAC, Official Methods of Analysis. 1996, Association of Official Analytical Chemists: Arlington,VA. Hii, C.L., Law, C.L., Michael, C., and Suzannah, S., Improving Malaysian cocoa quality through the use of dehumidified air under mild drying conditions. Journal Science of Food Agriculture, 2011. 91: p. 239-246. Hii, C.L., Law, C.L., Cloke, M., and Suzannah, S., Thin layer drying kinetics of cocoa and dried product quality. Biosystems Engineering, 2009. 102(2): p. 153-161. Guiné, R.P.F. and Fernandes, R.M.C., Analysis of the drying kinetics of chestnuts. Journal of Food Engineering, 2006. 76(3): p. 460-467. Izli, N. and Isik, E., Color and Microstructure Properties of Tomatoes Dried by Microwave, Convective, and Microwave-Convective Methods. International Journal of Food Properties, 2014: p. null-null. Djendoubi Mrad, N., Boudhrioua, N., Kechaou, N., Courtois, F., and Bonazzi, C., Influence of air drying temperature on kinetics, physicochemical properties, total phenolic content and ascorbic acid of pears. Food and Bioproducts Processing, 2012. 90(3): p. 433-441. Ong, S.P. and Law, C.L., Microstructure and Optical Properties of Salak Fruit Under Different Drying and Pretreatment Conditions. Drying Technology, 2011. 29(16): p. 1954-1962. Chong, C.H., Law, C.L., Cloke, M., Abdullah, L.C., and Wan Daud, W.R., Drying Models and Quality Analysis of Sun-Dried Ciku. Drying Technology, 2009. 27(9): p. 985-992. Sasidharan, S., Chen, Y., Saravanan, D., Sundram, K.M., and Yoga Latha, L., Extraction, Isolation and Characterization of Bioactive Compounds from Plants' Extracts. African Journal of Traditional, Complementary, and Alternative Medicines, 2011. 8(1): p. 1-10. Yao, H., Li, X., Liu, Y., Wu, Q., and Jin, Y., An optimized microwave-assisted extraction method for increasing yields of rare ginsenosides from Panax quinquefolius L. Journal of Ginseng Research, 2016. 40(4): p. 415-422.
SC R
32.
ACCEPTED MANUSCRIPT
55. 56.
57.
58.
59.
60.
61.
62.
63.
64. 65. 66.
T
IP
SC R
NU
54.
MA
53.
D
52.
TE
51.
CE P
50.
Escarpa, A. and González, M.C., Approach to the content of total extractable phenolic compounds from different food samples by comparison of chromatographic and spectrophotometric methods. Analytica Chimica Acta, 2001. 427(1): p. 119-127. Mattila, P. and Kumpulainen, J., Determination of Free and Total Phenolic Acids in Plant-Derived Foods by HPLC with Diode-Array Detection. Journal of Agricultural and Food Chemistry, 2002. 50(13): p. 3660-3667. D'Heureux-Calix F. and Badrie, N., Consumer acceptance and physicochemical quality of processed red sorrel/roselle (Hibiscus sabdariffa L.) sauces from enzymatic extracted calyces. Food Serv. Technol., 2004. 4: p. 141-148. Morton, J.F., Fruits of Warm Climates. 2013, Vermont, USA: Echo Point Books & Media. 550. Ong, S.P. and Law, C.L., Drying Kinetics and Antioxidant Phytochemicals Retention of Salak Fruit under Different Drying and Pretreatment Conditions. Drying Technology, 2011. 29(4): p. 429-441. Chen, Z. and Lamb, F.M., Analysis of the vacuum drying rate for red oak in a hot water vacuum drying system. Drying Technology:An International Journal, 2007. 25(3): p. 497-500. Arora, S., Bharti, S., and Sehgal, V.K., Convective drying kinetics of red chillies. Drying Technology, 2006. 24(2): p. 189-193. Lingayat, A., Chandramohan, V.P., and Raju, V.R.K., Design, Development and Performance of Indirect Type Solar Dryer for Banana Drying. Energy Procedia, 2017. 109: p. 409-416. Rabha, D.K., Muthukumar, P., and Somayaji, C., Experimental investigation of thin layer drying kinetics of ghost chilli pepper (Capsicum Chinense Jacq.) dried in a forced convection solar tunnel dryer. Renewable Energy, 2017. 105: p. 583-589. Sacilik, K., Keskin, R., and Elicin, A.K., Mathematical modelling of solar tunnel drying of thin layer orgainc tomato. Journal of Food Engineering, 2006. 73(3): p. 231238. Kareem, M.W., Habib, K., Ruslan, M.H., and Saha, B.B., Thermal performance study of a multi-pass solar air heating collector system for drying of Roselle (Hibiscus sabdariffa). Renewable Energy. Dina, S.F., Ambarita, H., Napitupulu, F.H., and Kawai, H., Study on effectiveness of continuous solar dryer integrated with desiccant thermal storage for drying cocoa beans. Case Studies in Thermal Engineering, 2015. 5: p. 32-40. King, K., Packaging and storage of herbs and spices, in Handbook of herbs and spices, K.V. Peter, Editor. 2006, Woodhead Publishing Limited: Cambridge,England. p. 86-101. Janjai, S. and Tung, P., Performance of a solar dryer using hot air from roofintegrated solar collectors for drying herbs and spices. Renewable Energy, 2005. 30(14): p. 2085-2095. Mohanraj, M., Performance of a solar-ambient hybrid source heat pump drier for copra drying under hot-humid weather conditions. Energy for Sustainable Development, 2014. 23: p. 165-169. Minea, V., Overview of heat pump-assisted drying systems-Part II: Data provided Vs. results reported. Drying Technology: An International Journal, 2014. Yahya, M., Fudholi, A., Hafizh, H., and Sopian, K., Comparison of solar dryer and solar-assisted heat pump dryer for cassava. Solar Energy, 2016. 136: p. 606-613. Gan, S.H., Chua, L.S., Aziz, R., Baba, M.R., Abdullah, L.C., Ong, S.P., and Law, C.L., Drying characteristics of Orthosiphon stamineus Benth by solar assisted heat pump drying. Drying Technology, 2017: p. null-null.
AC
49.
ACCEPTED MANUSCRIPT
74. 75.
76. 77.
78.
79.
80. 81. 82.
83.
84.
T
IP
SC R
73.
NU
72.
MA
71.
D
70.
TE
69.
CE P
68.
Best, R., Soto, W., Pilatowsky, I., and Gutierrez, L.J., Evaluation of a rice drying system using a solar assisted heat pump. Renewable Energy, 1994. 5(1): p. 465-468. Şevik, S., Aktaş, M., Doğan, H., and Koçak, S., Mushroom drying with solar assisted heat pump system. Energy Conversion and Management, 2013. 72: p. 171-178. Gazor, H.R. and Minaei, S., Influence of Temperature and Air Velocity on Drying Time and Quality Parameters of Pistachio (Pistacia vera L.). Drying Technology, 2005. 23(12): p. 2463-2475. Vega-Galvez, A., et al, Effect of temperature and air velocity on drying kinetics, antioxidant capacity, total phenolic content, colour, texture and microstructure of apple (var.Granny Smith) slices. Food Chemistry, 2012. 132(1): p. 51-59. Jangam, S.V., Joshi, V.S., Mujumdar, A.S., and THorat, B.N., Studies on dehydration of sapota (Achras zapota). Drying Technology, 2008. 26(3): p. 369-377. Krokida, M.K., Karathanos, V.T., Marinos-Kouris, D., and Maroulis, Z.B., Drying kinetics of some vegetables. Journal of Food Engineering, 2003. 59: p. 391-403. Minea, V., Heat-Pump–Assisted Drying: Recent Technological Advances and R&D Needs. Drying Technology, 2013. 31(10): p. 1177-1189. Chua, K.J., Chou, S.K., and Yang, W.M., Advances in heat pump systems: A review. Applied Energy, 2010. 87(12): p. 3611-3624. Lee, K.H., Kim, O.J., and Kim, J., Investigation on drying performance and energy savings of the batch type heat pump dryer. Drying Technology, 2010. 28(5): p. 683689. Sosle, V., Raghavan, G.S.V., and Kittler, R., Low-Temperature Drying Using a Versatile Heat Pump Dehumidifier. Drying Technology, 2003. 21(3): p. 539-554. Phoungchandang, S., Srinukroh, W., and Leenanon, B., Kaffir Lime Leaf (Citrus hystric DC.) Drying Using Tray and Heat Pump Dehumidified Drying. Drying Technology, 2008. 26(12): p. 1602-1609. Wong, P.K., Yusof, S., Ghazali, H.M., and Man, Y.B.C., Physico-chemical characterisitcs of roselle (Hibiscus sabdariffa L.). Journal of Nutrition Food Science, 2002. 32: p. 68-73. Chumsri, P., Sirichote, A., and Itharat, A., Studies on the optimum conditions for the extraction and concentration of roselle (Hibiscus sabdariffa Linn.) extract. Songklanakarin Journal of Science and Technology, 2008. 30 ( Suppl.1) p. 133-139. Bridle, P. and Timberlake, C.F., Anthocyanins as natural food colours-selected aspects. Food Chemistry, 1997. 58(1-2): p. 103-109. Palzer, S., Dubois, C., and Gianfrancesco, A., Generation of Product Structures During Drying of Food Products. Drying Technology, 2011. 30(1): p. 97-105. Castañeda-Ovando, A., Pacheco-Hernández, M.d.L., Páez-Hernández, M.E., Rodríguez, J.A., and Galán-Vidal, C.A., Chemical studies of anthocyanins: A review. Food Chemistry, 2009. 113(4): p. 859-871. Cheng, Y., Xu, Q.Z., Liu, J., Zhao, C.S., Xue, F.M., and Zhao, Y.Z., Decompositon of five phenolic compounds in high temperature water. Journal of the Brazilian Chemical Society, 2014. 25(11): p. 2102-2107. Li, N., Taylor, L.S., and Mauer, L.J., Degradation kinetics of catechins in green tea powder: effects of temperature and relative humidity. Journal of Agricultural and Food Chemistry, 2011. 59: p. 6082-6090.
AC
67.
SC R
IP
T
ACCEPTED MANUSCRIPT
MA
NU
Table 1: Corresponding water activity, initial and final moisture content of calyx and petals in different drying techniques Average final Water activity Drying strategies Average initial moisture moisture content/% aw content/% (db.) (db.) SD Calyx
712.02 ±109.01
13.05±1.44
Petal
896.55±149.68
10.99±1.53
D
SIHP
973.28±139.42
19.41±4.77
TE
Calyx Petal HA
956.46±46.76
16.16±0.22
1028.55±43.73
15.55±1.93
1043.20±72.22
15.46±1.80
1078.84±72.16
16.22±1.02
1042.40±82.90
16.38±0.09
CE P
Calyx Petal HP Calyx
0.51
0.52
0.54
AC
Petal
0.51
Table 2: Colour kinetics under different drying conditions and parameters
Drying methods Fresh Roselle
Total colour change, ΔE
Colour Parameters L*
a*
Chroma
Hue
b*
18.433±2.57a
17.36±2.57 b
5.58±1.12c
15.20±3.54a
17.12±0.65a
Calyx
21.38 ±4.45b
11.67±3.77a
3.97±2.77f
7.28±2.67b
12.61±3.86 d
18.19±0.84b
Petal
22.54±4.47 c
13.49±4.98a
3.48±2.29f
8.95±5.11c
14.19±4.64 e
14.76±0.41c
Calyx
20.57±1.87a
15.95±3.80 b
4.82±2.18c
6.47±2.78 a
16.77±3.91 a
16.22±0.51d
Petal
24.40±0.95c
17.81±3.33 b
3.70±2.53f
8.59±3.04c
18.50±3.53 b
12.52±0.77e
19.53±2.11a
17.51±4.10 b
3.74±2.99f
8.53±3.40 c
18.23±4.12 b
12.55±0.55e
-
SD
SIHP
HA (calyx) at 35 °C
ACCEPTED MANUSCRIPT at 40 °C
22.03±0.99c
17.12±5.09 b
4.76±2.07 c
8.39±4.16 cd
17.86±5.19 b
15.15±0.35c
at 45 °C
21.74±1.31b
19.30±3.68c
5.03±1.72 c
6.57±2.02 a
20.03±3.60 bc
14.35±0.70c
at 35 °C
21.20±3.08 b
19.41±6.30 c
6.18±3.02 d
8.96±5.33 c
20.43±6.51 bc
17.56±0.52ab
at 40 °C
20.68±2.36 ab
16.59±2.86 b
5.29±1.84 c
7.56±3.92 b
17.49±2.83 b
17.82±0.16ab
at 45 °C
21.37±2.90 b
18.08±2.82c
5.71±1.31 c
7.61±2.31 b
19.71±3.17 b
17.14±0.34a
23.19±0.92 c
21.42±2.90 d
6.56±2.29 d
7.27±2.32 b
Calyx
IP
HP
T
HA (petal)
21.98±3.85 c
16.97±0.36ad
SC R
18.80±0.23b 24.53±1.28 c 18.44±4.28 b 6.30±2.49 d 7.79±4.01 bd 19.96±4.41 b Petal Mean values ± standard deviation (n=3 replications) within the same column with the same letter are not
NU
significantly different (p>0.05)
MA
Front Entrance
AC
CE P
TE
D
HP
S1 S2 S3
S4
S5
S6
S7
S8
S9
S10
S11
S12
S13
Rear
D
MA
NU
SC R
IP
T
ACCEPTED MANUSCRIPT
AC
CE P
TE
Fig. 1: The layout of SGD (from top view), location of drying shelves and heat pump
Fig. 2 : Low temperature heat pump assisted dryer (HP)
ACCEPTED MANUSCRIPT
Moist air to dehumidify
T
Heat pump assisted dryer
IP
Shelf 1 T_C
Shelf 3 M_C
NU
Shelf 4 M_P
SC R
Shelf 2 T_P
Shelf 5 B_C
Dry air to drying chamber
D
MA
Shelf 6 B_P
TE
Fig. 3: Position of Roselle samples and direction of air flow
CE P
1.2
0.8
AC
Moisture ratio (dimensionless)
1
0.6
RR211
RR711
RR11_11
RR221
RR721
RR11_21
0.4
0.2
0 0
500
1000
1500
2000
2500
Drying time (min) Fig. 4: Changes in moisture ratio with time using SD strategy
3000
3500
ACCEPTED MANUSCRIPT 0.045 0.04
RR221
RR721
0.02 0.015
T
RR711
IP
0.025
RR211
SC R
0.03
RR11_11
RR11_21
NU
Drying rate, (gH20/gDM.min)
0.035
0.01
0 0
500
1000
MA
0.005
1500
2000
Drying time (min)
2500
3000
3500
45 40 35 30
70 60 50 40
25
30
20 20
15
T
10
RH 10
Time
Fig. 6: Variation of temperature and RH in SGD (SD)
Relative humidity,%RH
Room Temperature ,(°C )
50
CE P
55
80
AC
60
TE
D
Fig. 5: Changes in drying rate with time using SD strategy
ACCEPTED MANUSCRIPT 1.2
RR211
RR711
RR11_11
RR221
RR721
RR11_21
T
Moisture ratio (dimensionless)
1
SC R
IP
0.8
0.6
NU
0.4
0 0
500
1000
MA
0.2
1500
2000
2500
3000
D
Drying time (min)
TE
Fig. 7: Changes in moisture ratio with time using SIHP strategy
CE P
0.07
0.05
AC
Drying rate, (gH20/gDM.min)
0.06
0.04
RR211
RR711
RR11_11
RR221
RR721
RR11_21
0.03
0.02
0.01
0 0
500
1000
1500
2000
2500
Drying time (min) Fig. 8: Changes in drying rate with time using SIHP strategy
3000
3500
ACCEPTED MANUSCRIPT 60
80 70
50
30
40
20
20 T
NU
10
30
10
RH 0
MA
0
Relative humidity,(%RH)
T
50
IP
40
SC R
Temperature,(°C)
60
D
Time
TE
Fig.9: Variation of temperature and RH in SGD (SIHP)
CE P
1.2
0.8
AC
Moisture ratio, (dimensionless)
1.0
0.6
T_P
M_P
B_P
T_C
M_C
B_C
0.4
0.2
0.0 0
200
400
600
800
1000
1200
1400
1600
Drying Time (min)
Fig. 10: Changes in moisture ratio with time using HP strategy
1800
2000
ACCEPTED MANUSCRIPT 0.25
T IP
0.15
T_P T_C
M_P
B_P
M_C
B_C
SC R
Drying rate, (gH2O/gDM.min)
0.20
0.10
0.00 200
400
600
800
1000
MA
0
NU
0.05
1200
1400
1600
1800
2000
Drying Time (min)
D
Fig. 11: Changes in drying rate with time using HP strategy
27.0 25.0 23.0 21.0
20.0 19.0 15.0 17.0 10.0
15.0
Time Fig. 12: Temperature and moisture evolution trend in the HP chamber
Relative humidity, %RH
25.0
29.0 RH(%)
CE P
30.0
Temperature (°C )
AC
Temperature, (°C)
35.0
31.0
TE
40.0
ACCEPTED MANUSCRIPT 1.2
1
0.6
T
IP
HA35_P
HA40_P
HA45_P
HA40_C
HA45_C
SC R
Moisture ratio
0.8
HA35_C 0.4
0 200
400
600
800
MA
0
NU
0.2
1000
1200
1400
Time (Minutes)
TE
D
Fig. 13: Changes in moisture ratio with time using HA strategy
Drying rate, (gH20/gDM.min)
CE P
0.14
0.12
AC
0.1
0.08
0.06
HA35_P
HA40_P
HA45_P
HA35_C
HA40_C
HA45_C
0.04
0.02
0 0
200
400
Time (Minutes) 600 800
1000
Fig. 14: Changes in drying rate with time using HA strategy
1200
1400
ACCEPTED MANUSCRIPT 0.16
a
0.14 Protocatechuic Acid
T
b
c
IP
bc
0.10
SC R
Protocatechuic acid, %w,w
0.12
0.08 0.06
d
d
d
MA
0.02 0.00
HA 35
HA 40
HA 45
e
NU
0.04
e
SIHP_C
SIHP_P
SD_C
SD_P
HP_C
HP_P
Drying strategies
TE
D
(a)
8.00
Catechin
Catechin,%w/w
5.00 4.00 3.00
c
AC
7.00 6.00
d
CE P
9.00
a
a
b
b
SIHP_C
SIHP_P
b
b
SD_C
SD_P
a
2.00 1.00 0.00 HA 35
HA 40
HA 45
Drying strategies
(b)
HP_C
HP_P
ACCEPTED MANUSCRIPT Fig. 15: Retention of PCA (a) and catechin (b) in dried Roselle calyx and petals under different drying strategies. Oven drying with different temperature (HA35, HA40, HA45); SIHP (solar with intermittent heat pump drying for Roselle calyx, C and petal, P); SD (solar drying for Roselle calyx, C and petal, P) and HP (heat pump drying
T
for Roselle calyx, C and petal, P)
AC
CE P
TE
D
MA
NU
SC R
IP
Vertical bar and line graph indicated with the same letter are not significantly different (p>0.05)
ACCEPTED MANUSCRIPT Highlights
CE P
TE
D
MA
NU
SC R
IP
T
A unique drying technique with heat pump for Roselle processing is proposed. The color kinetics of dried Roselle from different drying techniques were compared. The study has demonstrated the potential of innovative drying for Roselle due to its noteworthy drying efficiency as well as retention of bio-active ingredient.
AC