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Manuscript Number: FOODCHEM-D-19-04956

Title: Impact of thermal pretreatment on crystallization of Thompson

raisins

Article Type: Research Article (max 7,500 words)

Keywords: Chilean raisins; crystallization; sugaring; temperature;

relative humidity

Corresponding Author: Dr. Lorena Alvarez,

Corresponding Author's Institution:

First Author: Lorena Alvarez

Order of Authors: Lorena Alvarez; Paulina Urrutia; Araceli Olivares;

Agustin Flores; Bhesh Bhandari; Tuyen Truong; Sergio Almonacid

Abstract: After prolonged storage or during the shipment of raisins, a

crystalline material may be developed on their surface, affecting the
final acceptability of the product. The mild thermal pre-treatment (50°C
for a period of 12 and 48 hours) was applied to dissolve any potential
tiny crystals and nuclei already present in the raisins. The thermal
pretreatment of raisins resulted in a reduction on the percentage of
crystallized raisins (w/w) from more than 46% in control samples to less
than 10% after 30 days of storage at 57 and 66% of relative humidity and
15 and 25 ºC. X-ray diffraction analysis identified D-Glucose monohydrate
as the main crystalline component. All the thermal treatments increased
the hardness of the raisins, when they were incubated at 57% RH. To
mitigate the problems of crystallization of raisins during shipping, it
is recommended that the raisins are thermally pretreated and the shipping
conditions are controlled.
*Cover Letter

Valparaiso, 22 Julio, 2019

Prof. Paul Finglas, Editor

Food Chemistry Journal

Dear Prof. Finglas:

We are pleased to submit a manuscript entitled " Impact of thermal pretreatment on
crystallization of Thompson raisins" for exclusive consideration of publication as an
article in Food Chemistry Journal.

Representing all authors, I would like to undertake that this manuscript has not been
previously published and is not under consideration in the same or substantially similar
form in any other peer-reviewed media. No conflict of interest, financial or other, exists.
We have included acknowledgements and funding sources after the discussion.
We have carefully followed your manuscript preparation guidelines for formatting and
style, and we look forward to receiving your comments on our efforts.

Sincerely yours,

Lorena Alvarez A.
Centro Regional de Estudios en Alimentos Saludables (CREAS), Valparaíso, Chile.

Email addresses lalvarez@creas.cl; lorenaangelica@msn.con

*Highlights (for review)

Highlights

 The increase in the ambient temperature from 15 to 25 ºC favored the

crystallization.

 Thermal pretreatment of raisins at 50 °C for 12 and 48 h reduced sugar

crystallization.

 During pretreatment, the crystallization was temperature- and humidity

independent.
*Manuscript
Click here to download Manuscript: Manuscript.docx

1 Impact of thermal pretreatment on crystallization of Thompson raisins

2 Lorena Alvarez1*, Paulina Urrutia1,2; Araceli Olivares1; Agustín Flores1; Bhesh Bhandari3;
3 Tuyen Truong4, Sergio Almonacid1,5

4 1
Centro Regional de Estudios en Alimentos Saludables (CREAS), Valparaíso, Chile.

5 2
Pontificia Universidad Católica de Valparaíso, Valparaíso, Chile.

6 3
School of Agriculture and Food Sciences, The University of Queensland, St Lucia, QLD,
7 Australia 4072.
8 4
RMIT University, Bundoora Campus (West), Melbourne, VIC 3083, Australia
9 5
Departamento de Ingeniería Química y Ambietal, Universidad Técnica Federico Santa
10 María, Valparaíso, Chile.

11 * Corresponding author: lalvarez@creas.cl

12

13 Abstract

14 After prolonged storage or during the shipment of raisins, a crystalline material may be
15 developed on their surface, affecting the final acceptability of the product. The mild
16 thermal pre-treatment (50°C for a period of 12 and 48 hours) was applied to dissolve any
17 potential tiny crystals and nuclei already present in the raisins. The thermal pretreatment of
18 raisins resulted in a reduction on the percentage of crystallized raisins (w/w) from more
19 than 46% in control samples to less than 10% after 30 days of storage at 57 and 66% of
20 relative humidity and 15 and 25 ºC. X-ray diffraction analysis identified D-Glucose
21 monohydrate as the main crystalline component. All the thermal treatments increased the
22 hardness of the raisins, when they were incubated at 57% RH. To mitigate the problems of
23 crystallization of raisins during shipping, it is recommended that the raisins are thermally
24 pretreated and the shipping conditions are controlled.

25 Keywords: Chilean raisins, crystallization, sugaring, temperature, relative humidity.

26
27 1. INTRODUCTION

1
28 Raisins are one of the most commonly consumed dried fruits, usually eaten out-of-hand. In
29 addition to their appealing appearance, good taste and aroma, raisins among other dried
30 fruits add important vitamins, minerals and bioactive compounds to the human diet (Khiari
31 et al., 2018).

32 World production of raisins reached 1.149 million metric tons during 2017–2018. The main
33 producer was Turkey, followed by the United States, China and Iran, representing together
34 73 % of the world production. Chile is another important producer, accounting for 57,000
35 metric tons, most of which (96.5%) exported (USDA, 2018). The main markets of Chilean
36 raisins are the United States, United Kingdom, Netherlands, Russia and Colombia
37 (González, 2018).

38 Different types for raisins defects, including presence of pieces of stems, and cap-stems,
39 sugared, discolored, damaged or moldyare considered for the classification of the products
40 to different grades. Sugared raisins are those with either, external or internal sugar crystals
41 and its accumulation, in the flesh or on the surface, is readily apparent (USDA, 2016).
42 Crystallized raisins are unattractive in appearance and have unpleasant texture (Ghorbani &
43 Darijani, 2009; Balbi, 2015; Sikuka, 2017; González, 2018). United States Standard for
44 processed raisins specifies that the maximum percentage (by weight) of crystallized or
45 sugared raisins, controlled by visual inspection, is 5, 10 and 15% for grade A, B and C,
46 respectively (USDA, 2016). It has been reported that sugar crystallization is favored after
47 considerable time of storage, especially under hot and humid climates, fluctuating storage
48 conditions (temperature and relative humidity), excessive handling, abrasion, among others
49 (Ghorbani & Darijani, 2009; Balbi, 2015; Sikuka, 2017). Since several factors are involved
50 in the generation of sugared raisins, until this moment there is no a clear solution to avoid
51 or delay this phenomenon. Crystallization remains one of the main concerns for Chilean
52 raisin producers, especially considering that products graded A and B are mainly exported,
53 and storage conditions fluctuate during shipping and customer storage.

54 Water activity and glass transition temperature (Tg) are parameters that have been utilized
55 to understand the interrelationship between changes in physicochemical properties and
56 influential factors governing the stability of foods (Bhandari & Howes, 1999; Roos &
57 Karel, 1991). The Tg of a substance is a function of moisture content, molecular weight and

2
58 composition and nature of its dry matter. During solid-rubbery glass transition the food
59 material changes from highly viscous brittle state to liquid-like viscoelastic state (Bhandari
60 & Howes, 1999). Rate of nucleation and crystal growth vary according the temperature. It
61 has been reported that nucleation rate is highest just above Tg while the maximum crystal
62 growth rate is between Tg and equilibrium melting temperature (Sperling, 1986). Bazardeh
63 & Esmaiili (2014) determined that onset and midpoint Tg of sultana raisins equilibrated at a
64 water activity of 0.536 corresponds to -32.28 and -28.39 ºC, respectively, using a scan rate
65 of 10 ºC min-1. The major sugar components of raisins are glucose and fructose, and the
66 glucose is in supersaturated state in the existing moisture (<20% w/w) of raisins (Liu et al.,
67 2006). Considering the infeasibility of keeping the raisins at a temperature lower than Tg,
68 the presence of sugar crystals (of glucose) is unavoidable and rate of crystal growth is a
69 critical factor in order to guarantee the quality of the product during its shelf life.

70 Very limited studies have been published to investigate the sugaring problem in raisins. As
71 early as in 1976, Bolin (1976) found that formation of excessive crystals can be retarded
72 when mild heat treatment (49 oC for 48 h) is applied to whole raisins, which showed no
73 crystals under visual control up to 10 months of storage at 22 oC. The heat treatment
74 resulted in slight darkening and moist appearance in the heat-treated raisins. On the other
75 hand, Akev, Koyuncu, & Erbaş (2018) analyzed the impact of low temperature storage (0
76 o
C, 75-85 % relative humidity) and found that raisins packaged under controlled
77 atmospheric condition (1 % O2 and 3% CO2) also showed no sugaring after 10 months at
78 low temperature storage as evaluated by sensory analysis. Both of above studies provided
79 important information but did not undertake in-depth research using various other
80 analytical tools and parameters.

81 Since a pretreatment at high temperature can be a feasible way to control the sugaring
82 phenomenon and it does not require the additional cost of maintaining the raisins at low
83 temperature during their whole shelf life, it is necessary to further investigate the impact of
84 thermal pre-treatment on sugar crystallization using visual inspection (according to
85 international standards) and also more sophisticated methods such as X-ray diffraction and
86 polarized light microscopy to better understand and control the sugaring process.

3
87 The aim of the present study is to evaluate the influence of high temperature pretreatment
88 on the rate of sugars crystallization in Thompson seedless raisins, which is reported to show
89 frequent sugaring under transport and storage conditions. In this study, X-ray diffraction
90 was used to analyze crystalized sugars after raisins pretreatment while visual inspection and
91 polarized light microscopy were used to measure sugaring rate and observe and determine
92 the sugar crystals size when raisins are stored at different conditions (temperature and
93 relative humidity). Additionally, texture and color analysis of pretreated samples were
94 analyzed after one month of storage.

95 2. MATERIALS & METHODS

96 2.1 Materials

97 The raisins selected for this study was the Thompson seedless variety size Jumbo (> 12
98 mm), provided by the Chilean company Frutexsa, located in the Aconcagua Valley, Chile.
99 The raisins were harvested and processed between the periods of 2017-2019. The raisins
100 used in this work were the finished product, ready for storage or commercialization.

101 All chemicals used in this study were of analytical grade unless otherwise specified.

102 2.2 Analyses on chemical composition and physico-chemical properties of initial

103 samples

104 The raisins samples were ground using a low speed grinder. The raisin paste was then
105 subjected to determination of sugar composition, total soluble solids, pH, acidity, moisture
106 content and water activity.

107 2.2.1 Sugar composition

108 Analysis of glucose and fructose in the initial raisin samples was undertaken using high-
109 performance liquid chromatography (HPLC) with a refractive index detector (IR), JASCO
110 brand. A Benson 1400-0BP-100Ag + Carbohydrate column was used, with a flow rate of
111 0.35 mL /min at 55 °C, and detector temperature of 45 °C. Each run required 35 min to
112 complete. Stock solutions of glucose and fructose (10% w/w) were prepared, whereby
113 working standard solutions within the concentration ranges of 25 – 500 mg L-1 were
114 prepared fresh. Quantification of sugar level was based on integrated peak areas as against

4
115 the corresponding external standards. Samples were filtered using syringe filters (0.45 m
116 nylon).

117 2.2.2 pH

118 The ground raisin samples were diluted with distilled water to prepare 10% w/w raisin
119 solution. pH was determined by using a pH meter (Jenco-pH meter) according to Dehghan-
120 Shoar et al., (2010).

121 2.2.3 Titrable acidity

122 Distilled water was added to the ground raisins to make up a raisin solution (20% w/w).
123 The raisin solution was mixed well and filtered through cheese cloth to remove insoluble
124 parts. Twenty-five mL of the filtered raisin solution was titrated with NaOH (0.1%) using
125 phenolphthalein as an indicator. The titrable acidity of raisin samples was expressed as
126 percentage of anhydrous tartaric acid (Bongers et al., 1991) using following equation:

127 % dry weight= 0.1NVm(75gmol) 25mL (100) in which N is normality of NaOH used, Vm
128 is volume (mL) of NaOH consumed by titrant.

129 2.2.4 Water activity

130 Determination of water activity of ground raisin samples was undertaken at 25 oC using a
131 water activity meter (Aqua Lab meter, Decagon, Washington, US).

132 2.2.5 Moisture content

133 Approximately 2 g of the raisin ground samples was spread thinly onto the aluminum
134 dishes, which were then allowed to dry under vacuum using a vacuum drying oven (DZ-2B
135 CII oven) at 60 ºC until reaching the constant weight. The moisture content was calculated
136 based on the difference in weight.

137 2.2.6 X-ray diffraction analysis of pretreated raisins

138 The raisin pretreated at high temperature were subjected to X-ray diffraction analysis using
139 Bruker D8 Advance X-ray diffractometer (Bruker UK Limited, Coventry, UK). The
140 diffractometer used consists of a graphite monochromator, a copper target and a
141 scintillation counter detector. The samples were scanned from 0.02o for 0.5 seconds. The

5
142 wavelength of radiation was 1.5406 Å. The current and the voltage used were 30 mA and
143 40 kV, respectively. The XRD patterns of raisins were acquired by Diffract Plus, V15.2009.
144 Software whereby comparison with database PDF-2, permited the understanding of crystal
145 forms present in the raisins investigated.

146 2.2.7 Texture profile analysis (TPA)

147 For the evaluation of the textural parameters the equipment Food Technology TMS-pro was
148 used. Analysis was carried out using two compression cycles using a flat 45 mm diameter
149 plunger. Interval between cycles was 5 s. 40 g of raisins (approximately 35 raisins) was
150 used to load a cylindrical probe and test rate was 100 mm/min. The compression used was
151 20%. Five TPA`s were obtained for each sample. Figure 1 represents typical double
152 compression or TPA test of fresh raisin (load or force/time).

153 The texture parameters of hardness, springiness (elasticity), cohesiveness and chewiness
154 were calculated by the following equations based in definitions of TPA (Caine et al. 2003;
155 Guiné et al. 2015).

156 Hardness (N)= F1

157 Springiness (%)= ∆T2∆T1 x 100

158 Cohesiveness (dimensionless)= A2A1

159 Chewiness (N)= F1 x ∆T2∆T1 x A2A1

160 Where, T1, T2= times; A1, A2= Areas

161
162 2.2.8 Color attributes of raisins

163 The color parameters of raisins were measured using a colorimeter (Konica MINOLTA
164 CHROMA METER CR-400) without and with thermal pretreatment of raisins after 30 days
165 of incubation at different storage conditions (temperature and relative humidity). The
166 values were expressed by the CIE L* (brightness–darkness), a* (+ a*: red, − a*: green)
167 and b* (+ b*: yellow, − b*: blue) system. The values obtained of L*, a* and b* parameters
168 were the average of 20 samples examined.

6
169 ΔE, represents total color difference and considered for the overall color evaluation
170 between fresh raisins (without pretreatment) and thermal pretreated samples (after 30 days).
171 Raisins without thermal pretreatment or fresh raisins samples (L*0, a*0, b*0) were used as
172 initial samples (reference) and low ΔE value corresponds to a low color change from the
173 reference raisins (Bai et al., 2013; Wang et al., 2017b).

174 ΔE: total color difference

175 ΔΕ= (L0*-L*)2 + (a0*-a*)2+(b0*-b*)2]

176 Where, a* = redness/greenness, b* =yellowness/blueness, L* =lightness [brightness from

177 black (0) to white (100)]

178
179 2.2.9. Visual inspection and microscopic analysis of raisin samples

180 A visual inspection of the crystallized raisins was made according to USDA standards for
181 processed raisins (Petrucci and Clary, 2002; McCoy et al., 2015; USDA 2018). For this
182 purpose, 400 g of raisins from each pretreatment were weighed and visual inspection of one
183 by one of raisins under magnifying glass was carried out. The crystallized raisins are
184 weighed and the percentage of crystallized raisins was determined. According to USDA
185 standards, a sugared sample means presence of either external or internal sugar crystals and
186 the accumulation of such crystallized fruit sugars in the flesh or on the surface of the raisins
187 are readily apparent. Considering this classification of crystallized raisins, the size of the
188 readily apparent crystals was determined under the advice of industrial quality control
189 experts and corresponded to 200 μm.

190 For the microscopic analysis, samples of raisin flesh were gently spread onto the
191 microscopic slide, following microscopic observation under a polarized light microscopy
192 (Olympus U-CTR30-2, Tokyo, Japan) at 4X magnification.

193 2.3 Thermal pretreatment and crystallization kinetics of raisins

194 Thermal pretreatment consisted in the thinly spreading of ⁓ 400g of raisins (finished
195 product) in aluminum trays and their incubation in oven at 50 °C for a period of 12 and 48
196 h. The crystallization was monitored for a period of 30 days at two temperatures (15 and

7
197 25ºC) and relative humidity (57 and 66%) by visual inspection and polarized microscopy.
198 The temperature and humidity conditions were selected based on the actual range of
199 temperature and humidity likely to be realized by raisins in practice. The RH conditions
200 were obtained using supersaturated salt solutions of NaBr (57% HR) and NaNO2 (66%
201 HR).

202 Physico-chemical analysis was carried out every 10 days. The results obtained were
203 compared with the control samples that correspond to the raisins without thermal
204 pretreatment.

205 2.4 Statistical analysis

206 All measurements were carried out at least in duplicate. One-way Analysis of Variance
207 (ANOVA) and Fisher’s test was used to detect the difference between the mean values at P
208 < 0.05 using Minitab Release 16 (Minitab Co., US).

209 3. RESULTS AND DISCUSSION

210 3.1 Crystallization kinetics and physico-chemical properties of raisins without

211 pretreatment (control)

212 Raisins used in this study showed a moisture content of 15.8 ± 0.5 %, and a corresponding
213 water activity of 0.586 ± 0.011. The results of the crystallization kinetics obtained when
214 finished products without thermal pretreatment were stored under different conditions are
215 shown in Figure 2. The storage conditions used were 57 and 66% RH and 15 and 25 ºC.

216 In case of control samples, the increase of storage temperature favored crystallization,
217 particularly after 20 days of storage, independent of the relative humidity value. On 30 days
218 of storage, the percentage of crystallized raisins incubated at 57% RH increased from 4% to
219 29 ± 3 and 46 ± 6 % (w/w) when storage temperature was 15 and 25ºC, respectively. In the
220 case of 66% RH, crystallization increased to 25 ± 4 and 56 ± 7 % (w/w) when storage
221 temperature was 15 and 25ºC, respectively. On the other hand, it may be observed that at
222 constant temperature the increase of RH from 57 to 66% did not affect significantly
223 (P>0.05) the percentage of crystallized raisins.

8
224 Samples of raisin flesh were analyzed by polarized light microscopy (Figure 3 A). The use
225 of polarized light allowed improving the visualization of the crystals inside the product,
226 which appeared as a bright region surrounded by the dark background. Crystal size were
227 measured and distribution is presented in Figure 3 B. The tiny crystals existed even in the
228 fresh sample (0 day) as seen in Figure 3A1. Initially, major part of the crystals was in the
229 rage 0.09-0.3 μm, while after 30 days of storage the size distribution changed and crystals
230 of higher sizes were observed, which may be explained by the crystals growth. Crystals of
231 higher size were obtained in samples stored at 66% RH. The higher size of crystals after 30
232 days is consistent with the kinetic obtained by visual inspection, since a raisin will be
233 classified as crystallized according USDA standards only when crystals may be observed
234 by naked eye.
235 The water activity of raisins is presented in Table 1. The initial water activity and moisture
236 content value for control samples were 0.586 and 17% (w/w), respectively. These values
237 are higher than the values reported for Afghan raisins that averaged 0.52 aw and
238 corresponded to moisture contents of 13 to 15 % (McCoy et al., 2015). As may be observed
239 in Table 1, aw of control samples increased along the 30 days of storage, obtaining a higher
240 increment when raisins were stored at 66% RH, which is expected as the raisins will
241 eventually equilibrate with the headspace RH (aw=RH/100). The higher aw after 30 days of
242 storage may explain the higher proportion of raisins crystallized, as can also be seen in the
243 samples stored at 57% RH. As during the crystallization process the sugar gives up the
244 moisture (solid glucose monohydrate crystals will carry less moisture), the moisture of the
245 remaining fraction will be higher so the water activity will increase until the sample
246 equilibrates with the RH of the headspace. The equilibration time appears to be longer than
247 the observation time of 30 days. (Roos, 2016).

248 The analysis of the sugars shows that the glucose/fructose ratio increases slightly as the
249 storage time increases, to the different temperature and humidity conditions (Table 1).
250 Similar results were obtained by Liu et al. (2006) in raisins obtained from Vitis
251 rotundifolia, Vitis labrusca, and Vitis vinifera.
252 The acidity range of the control raisins after 30 days of storage was 2.02 ± 0.01 - 2.11 ±
253 0.02 g of tartaric acid per g of dried raisins. No significant differences were observed
254 according to Fisher’s test (p < 0.05), between the various storage conditions during 30 days

9
255 of the raisins pre-treated at 50 °C for 12 h and the controls, while samples pretreated at 50
256 °C for 48 h, showed a significant increase in acidity after 30 days of storage at 15 °C and
257 25 °C at 57% RH (Figure 4).

258 3.2 Crystallization kinetic and physico-chemical properties of raisins with thermal
259 pretreatment

260 The results of the crystallization kinetics of raisins with thermal pretreatment at 50 °C for a
261 period of 12 and 48 h are presented in Figure 2.

262 Thermal pretreatment of raisins caused a significant decrease of crystallization rate,

263 obtaining less than 10 % (w/w) of crystallized raisins after 30 days of storage at all
264 conditions (temperature and relative humidity) evaluated. However, the best results were
265 obtained when samples were stored at 25 °C and 57 % RH, obtaining less than 5 % (w/w)
266 of crystallized raisins after 30 days of storage. This results are in contrast to the control
267 raisins, where percentage of crystallized raisins at these conditions exceeded 46 % (w/w).
268 No significant difference (P>0.05) was observed between the raisins pretreated at 50 ° C for
269 12 or 48 h.

270 Similar studies were undertaken by Bolin (1976) to delay crystallization, evidencing the
271 impact of thermal pretreatment on raisins crystallization through visual inspection and
272 organoleptic test. After a series of exploratory experiments where raisins were heated for 48
273 h at 49 °C, the author found that the thermal treatment also had an effect on the texture of
274 the whole raisins. The author observed that, when subjected to a certain minimum heating,
275 raisins presented a softer texture than untreated raisins. The visual inspection of the heat-
276 treated raisins stored at 22 °C for 10 months, revealed no evidence of crystal formation.

277 Analysis of the aw of raisins thermally pretreated is shown in Table 1. Initial aw was
278 significantly lower than control (P < 0.05). This result can be explained by the evaporation
279 of water during thermal process. Even though, initial aw was lower, samples with 12 h of
280 thermal pretreatment showed an increment of aw along the 30 days of storage, especially at
281 25ºC. As may be observed, final aw of pretreated samples were increasing while
282 equilibrating with the RH of the headspace conditions. The actual time for such
283 equilibration would have been longer than 30 days as the water activity was lower than the

10
284 RH/100 of the headspace. However, crystallization was significantly lower than control at
285 these conditions.
286
287 The samples treated thermally for 12 h and 48 h show an increase in the glucose/fructose
288 ratio, as the storage time increases to the different conditions (15 °C and 25 °C, at the two
289 humidity conditions 56% RH and 66% RH), (Table 1).

290 On the other hand, when comparing the thermally pretreated samples during 12 h stored for
291 30 days concerning their respective controls, no significant variation in the glucose/fructose
292 ratio was obtained. On the other hand, samples treated thermally for 48 h presented a
293 significant difference according to Fisher's test, p <0.05 concerning their stored controls
294 under the same conditions. (15 ° C, 25 ° C, 56% RH and 66% RH) (Table 1). Through the
295 thin-layer chromatography analysis of skin of the fruit in the pericarp, Miller and
296 Chichester (1960) reported that the "sugar" of the raisin consisted of glucose, fructose and
297 tartaric acid, but they did not determine the crystalline form of these sugars. Our
298 microscope examination of the surface of the raisins revealed a few scattered large
299 individual crystals. X-ray diffraction analysis identified D-Glucose hydrated as the main
300 crystalline component in the control samples, and highly possible beta-D-Glucose. In the
301 case of samples pretreated at 50 °C, only alpha-D-Glucose was identified without the
302 presence of other crystalline species (Appendix 1). These crystals were very thin and
303 fragile and broke easily. The major part of crystals observed by naked eye occurred in the
304 large crease (wrinkle) of the raisins. This could be due to a greater permeability of the skin
305 at the point. The surface of a raisin is composed of a network of interspersed wax platelets.
306 Possibly, when drying, the formation of the obtuse angles of the skin causes a stretch and
307 separation of the wax platelets, which allows the solution of sugars to pass through the skin
308 to the outer surface in these areas. On the surface, the rest of the water evaporates easily,
309 leaving a saturated sugar solution that crystallizes easily in the presence of a few small seed
310 crystals (Possingham, 1972). In addition, the large crystals may also pierce the weakest
311 point and grow internally pushing the grown crystals out, appearing as white granular
312 surface.

313 3.3 Texture profile analysis (TPA)

11
314 Appendix 2 and 3 present the results obtained for the determinations of hardness (N),
315 springiness (%), cohesiveness and chewiness (N) of the raisins stored for 30 days at 57%
316 RH and 66% RH.
317 Hardness is the force required to compress a food between the teeth or between the tongue
318 and mouth to cause deformation (Guiné et al., 2015). All thermal pretreatments increased
319 the hardness compared with fresh raisin and control, when they were incubated at 57% RH.
320 The thermal treatment of 50 oC for 12 h (incubated at 25 oC) and treatment of 50 oC for 48
321 h (incubated at 15 oC) showed significant difference (p<0.05) with respect to fresh raisin
322 (on day 0).
323 Regarding the samples stored at 66% RH, thermal treatment for 48 h (incubated at 15oC)
324 decreased in hardness parameters, but this difference was not significant. The increased
325 hardness is mainly contributed by the loss of moisture during the thermal treatment. From
326 Table 1 one can see that the control samples had higher water activity on 30 days than the
327 thermally treated samples.

328 The springiness (elasticity) is the ability to recover the shape after compression and
329 measures the speed of return to the initial state after the elimination of the force that causes
330 the deformation (Guiné et al., 2015; Singh et al., 2013) and was defined as the ratio
331 (percentage) of the time from the start of second and first compression to the peak. The
332 springiness values of each treatment did not show significant difference (p<0.05) compared
333 with fresh raisins (on day 0) and between them for both relative humidity conditions
334 (Appendix 2B and Appendix 3B).

335 Cohesiveness (Appendix 2C and Appendix 3C) represents the internal forces in the food,
336 and which maintains the sample cohesive (Guiné et al., 2015). It was found that the
337 cohesiveness for samples with thermal treatment by 48h were equal (0.55, incubated at
338 57% RH at 15oC and 25oC) and the difference with fresh raisin (day 0) were statistically
339 significant (P<0.05). Regarding at 66% RH, just thermal treatment at 48 h and incubation at
340 15oC showed significant difference (p<0.05). Then, these raisins were relatively more
341 cohesive.

342 The chewiness measures the energy required to disintegrate a food as to be swallowed
343 (Guiné et al., 2015). At 57% relative humidity, the samples with thermal treatment for 12 h

12
344 (incubated at 25oC) and 48 h (incubated at 15oC) showed significant differences, but at 66%
345 relative humidity no significant difference was found (p<0.05).

346 Bolin H.R. (1976) was one of the first authors to investigate the raisin crystallization during
347 storage. That work also determined texture parameter (hardness, expressed as shear force)
348 after a mild heat-treatment (48h at 49oC) and reported that treated raisins had a softer
349 texture immediately after heating and hardness increased during storage time.

350 Wang et al. (2017), who studied the effects of ripeness on the physicochemical properties
351 and pulsed vacuum drying characteristics of Thompson seedless grapes. They showed the
352 TPA parameters of raisins after different drying processes, but the parameters depended on
353 the initial ripeness of grapes. Our results showed that some parameters, such as springiness,
354 was not affected by thermal treatment and were independent of relative humidity.
355 Meanwhile, hardness, cohesiveness and chewiness were more affected at 57% RH and
356 when the thermal treatment was for 48 h and incubated at 15oC.

357 3.4 Color attributes of raisins

358 Color parameters were investigated to evaluate the effects of thermal pretreatment of raisins
359 to avoid crystallization of sugar at different storage conditions. Color is one of the most
360 important criteria for the determination quality and consumer preference of raisins (Guiné
361 et al., 2015; Jairaj et al., 2009). Color parameters and ΔE of controls (without thermal
362 treatment, but incubated at 57% RH and 66% RH) and thermal treatment (at 50 ºC for 12 h
363 and 48 h) incubated at different temperatures (15 ºC and 25 ºC) are shown in Table 2.

364 The results showed in Table 2 indicate that thermal pretreatment affected all color
365 parameters and were lower than fresh raisin. L* parameter, represent lightness in terms of
366 whiteness or brightness, and the values obtained ranged from 24 to 25.3 for all thermal
367 treatments with decrease of 4 to 8.7% in relation to fresh raisin. This value is low as
368 compared to other works that published L* parameters of raisin (Guiné et al., 2015) and
369 indicated that raisins were darker, but still acceptable to consumers. Bai et al. (2013) who
370 used high-humidity hot air impingement blanching as thermal treatment in seedless variety
371 Thompson found values of L* parameter between 22.20 and 54.33 depending on the
372 temperature applied to dry seedless grapes. All a* and b* parameters were less than fresh

13
373 raisin, indicating that raisins with or without thermal treatment had less red and yellow
374 coloration, respectively.

375 Table 2 shows total color difference (ΔE) and considered the total color difference
376 between samples without thermal treatment (control) and with thermal treatment by 50 ºC
377 at 12 h and 48 h at 57 % RH and 66% RH at different incubation temperature (15 ºC and 25
378 ºC). In general, lower ΔE values represent less color changes during the thermal treatment,
379 which make the products to be accepted by the customers. The higher ΔE* was obtained
380 for 12 h of thermal treatment incubated at 25 ºC and 66% RH (similar value at 57% RH).
381 The color differences of raisins with 12 h of thermal pretreatment were not affected by
382 different relative humidity and no significant difference was found between the samples
383 stored at the same incubation temperatures. Color is considered as the key quality index due
384 to its relation with flavor and aroma and dried foods are susceptible to color deterioration
385 (Wang et al., 2014) and all samples showed a desirable color with low ΔE* value.

386 4. CONCLUSIONS

387 The control of crystallization kinetic of Thompson raisins by their thermal pretreatments at
388 50 °C for a period of 12 and 48 hours was studied, analyzing the impact of different storage
389 conditions (temperature and relative humidity).

390 The increase in the ambient temperature from 15 to 25 ºC favored the crystallization of the
391 raisins without pretreatment, its effect being more significant than the increase of the
392 relative humidity from 57 to 66%. When the ambient temperature increased to 25ºC, the
393 crystallization rate presented an exponential tendency, obtaining a percentage of sugaring
394 higher than 10% after 20 days of storage at 57% RH and 66% RH. Analysis of raisins flesh
395 by optical polarized light microscopy showed that crystals size distribution changed in 30
396 days of storage at all conditions and crystals with larger sizes were observed.

397 The thermal pretreatment of the raisins at 50ºC decreased the rate of crystallization (less
398 than 10% of sugaring in 30 days of storage) and the phenomenon of crystallization was
399 independent of the temperature and relative humidity. The thermal pretreatment of the
400 raisins decreased their initial moisture (from 17% to 13-15%), resulting in a lower aw

14
401 compared to the control. However, storage of raisins at 57% and 66% RH increased aw as
402 observed in control.

403 The thermal pretreatment of the samples decreased the average color parameters of the
404 raisins, with respect to the control. The greatest color difference was obtained for the raisins
405 stored at 25ºC. Texture parameters, such as springiness, was not affected by thermal
406 pretreatment and were independent of relative humidity, meanwhile, hardness,
407 cohesiveness and chewiness were more affected at 57% RH and when the thermal
408 treatment was for 48 h and at storage t temperature of 15 °C.

409 Declaration of interests

410 None.

411 Acknowledgements

412 THE AUTHORS ACKNOWLEDGE THE GRANT FUNDED BY CONICYT CHILE

413 CODE R16F10010 AND CONICYT REGIONAL/ GORE VALPARAÍSO/CREAS/CODE
414 R17A10001.

15
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18
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501

502 LEGEND FIGURES

503 Figure 1. Representative Texture Profile Analysis (TPA) curve of fresh raisins. Peak 1 and
504 Peak 2 are the maximum load or force (N) for first and second cycle of compression,
505 respectively.

506 Figure 2: Crystallization rate of raisins (finished product) stored at (A) 57 and (B) 66%
507 relative humidity at 15 and 25 °C. Control: samples without pretreatment TP1: thermal
508 pretreatment at 50 ° C for 12 h. TP2: thermal pretreatment at 50ºC for 48 h.

509 Figure 3. Analysis of sugar crystals size of thermally untreated samples by polarized light
510 microscopy. (A) Photography (4 X magnification) of control sample stored at 66% RH and
511 25ºC, (A.1) initial sample and (A.2) 30 days’ sample. (B) Crystal size distribution of
512 samples stored at 15 and 25ºC for 30 days and with a relative humidity of (B.1) 57% and
513 (B.2) 66%.

514 Figure 4: Titrable acidity content of raisins (finished product) determined as tartaric acid.
515 Raisins were stored at (A) 57 and (B) 66% relative humidity and at 15 and 25 ° C. Control:
516 samples without pretreatment TP1: thermal pretreatment at 50 ° C for 12 h. TP2: thermal
517 pretreatment at 50ºC for 48 h.

518

519
520

19
Table(s)

1 TABLES
2
3 Table 1: Effect of storage conditions (relative humidity and temperature) on the water
4 activity (aw) and glucose/fructose ratio of the raisins with and without thermal
5 pretreatment (the values presented are the average of all replicate analyze, the
6 standard deviation is not presented but the coefficient of variation of mean was less
7 than 10%)
8
aw
57% RH 66% RH
Time
Control TP1 TP2 Control TP1 TP2
(d)
15°C 25°C 15°C 25°C 15°C 25°C 15°C 25°C 15°C 25°C 15°C 25°C
A a a b b c c a a b b c
0 0.586 0.586 0.508 0.508 0.458 0.458 0.586 0.586 0.508 0.508 0.458 0.458c

20B 0.589 a 0.595 b 0.555 c 0.553 c 0.502 d 0.486 e 0.634f 0.603f 0.560b 0.612g 0.555 c 0.557 c

30C 0.624a 0.632a 0.574b 0.565c 0.509d 0.495d 0.644e 0.663f 0.588g 0.659e 0.579b 0.603h

Glucose/Fructose ratio
57% RH 66% RH
Time
Control TP1 TP2 Control TP1 TP2
(d)
15°C 25°C 15°C 25°C 15°C 25°C 15°C 25°C 15°C 25°C 15°C 25°C
0 0.93
0.93a,A a,A
0.96b,A 0.96b,A 0.93a,A 0.93a,A 0.93a,A 0.93a,A 0.96b,A 0.96b,A 0.93a,A 0.93a,A

20 0.98a,B 1.06b,B 0.99a,A 0.99a,A 0.91c,B 0.96a,A 1.03d,B 1.01d,B 1.01d,B 0.97d,A 0.86a,B 0.97d,B
30 1.15a,C 1.09b,C 1.11b,C 1.16a,B 1.01c,C 0.99c,B 1.16a,C 1.13a,C 1.14a,B 1.16a,B 1.02c,C 1.06c,C
9 TP1: thermal pretreatment at 50ºC for 12 h; TP2: thermal pretreatment at 50ºC for 48 h
10 Different lowercase letters in same row denote a significant difference according to Fisher’s test, p < 0.05.
11 Different capital letters in same column denote a significant difference according to Fisher’s test, p < 0.05.
12
13

14

15

16

17

1
18

19 Table 2. Color parameters of raisins without and with thermal treatment at 50 ºC for
20 12 and 48 h and stored at different conditions of temperature and relative humidity.

21

Sample RH (%) T oC L* a* b* E*

Fresh raisin (Day 0) --- --- 26.35 ± 2.16 6.92 ± 2.06 7.53 ± 2.39 ---

Control-15 °C 15 24.90 ±2.17 5.28 ± 1.41 6.24 ± 1.57 2.54 ± 0.127a

57
Control- 25 °C 25 25.43 ± 1.64 4.89 ± 1.32 5.99 ± 1.42 2.71 ± 0.145b

Control-15 °C 15 27.03 ± 4.26 4.82 ± 1.71 5.93 ± 1.88 2.73 ± 0.136b

66
Control-25 °C 25 25.55 ± 1.87 5.34 ± 1.12 6.36 ± 1.71 3.13 ± 0.105c

TP1- 15 °C 15 24.37 ± 2.17 5.32 ± 1.68 6.11 ± 1.55 2.91 ± 0.145d

57
TP1- 25 °C 25 24.06 ± 1.55 4.82 ± 1.56 5.52 ± 1.30 3.70 ± 0.185e

TP1- 15 °C 15 24.78 ± 2.35 5.32 ± 1.72 6.37 ± 1.74 2.53 ± 0.126a

66
TP1- 25 °C 25 24.14 ± 1.91 4.60 ± 1.37 5.44 ± 1.36 3.83 ± 0.191e

TP2- 15 °C 15 25.30 ± 2.21 5.22 ± 1.52 5.82 ± 2.01 2.63 ± 0.131b

57
TP2- 25 ºC 25 24.43 ± 1.60 4.74 ± 1.44 5.23 ± 1.16 3.68 ± 0.148e

TP2- 15 °C 15 24.84 ± 1.71 4.66 ± 1.70 5.22 ± 1.95 3.57 ± 0.178e

66
TP2- 25°C 25 24.24 ± 1.90 5.48 ± 1.49 5.67 ± 1.53 3.16 ± 0.158c

22 TP1: thermal pretreatment at 50ºC for 12 h; TP2: thermal pretreatment at 50ºC for 48 h.
23 Different letters in same column denote a significant difference according to Fisher’s test, p < 0.05.
24
25

2
Figure(s)
Click here to download Figure(s): Figures.docx

1 FIGURES
2

4 Figure 1. Representative Texture Profile Analysis (TPA) curve of fresh raisins. Peak 1
5 and Peak 2 are the maximum load or force (N) for first and second cycle of
6 compression, respectively.

70 70
(A) Control-15°C (B)
Crystallized raisins (% w/w)

Crystallized raisins (% w/w)

60 Control-25°C
TP1-15°C
60
TP1-25°C
50 TP2-15°C 50
TP2-25°C
40 40
30 30
20 20
10 10
0 0
0 10 20 30 0 10 20 30
Time (days)
Time (days)

8 Figure 2: Crystallization rate of raisins (finished product) stored at (A) 57 and (B)
9 66% relative humidity at 15 and 25 °C. Control: samples without pretreatment TP1:
10 thermal pretreatment at 50 ° C for 12 h. TP2: thermal pretreatment at 50ºC for 48 h.

11

1
12

(A1) (A2)

9
(B1) 0 day -15°C 9
8 30 days- 15°C 8
(B2)
7 0 day - 25°C
30 days- 25°C Sugar crystals (%) 7
Sugar crystals (%)

6 6
5 5
4 4
3 3
2 2
1 1
0 0
0.02
0.18
0.34
0.50
0.66
0.82
0.98
1.14
1.30
1.46
1.62
1.78
1.94
2.10
2.26
2.42
2.58
2.74
2.90
0.02
0.18
0.34
0.50
0.66
0.82
0.98
1.14
1.30
1.46
1.62
1.78
1.94
2.10
2.26
2.42
2.58
2.74
2.90

Crystal size (µm) Crystal size (µm)

13 Figure 3. Analysis of sugar crystals size of thermally untreated samples by polarized

14 light microscopy. (A) Photography (4 X magnification) of control sample stored at
15 66% RH and 25ºC, (A.1) initial sample and (A.2) 30 days sample. (B) Crystal size
16 distribution of samples stored at 15 and 25ºC for 30 days and with a relative humidity
17 of (B.1) 57% and (B.2) 66%.

18

2
 5 5
A) Control-15°C
B)
% Tritable acidity (tartaric acid)
Control- 25°C

% Titrable acidity (tartaric acid)

TP1- 15°C
4 TP1- 25°C 4
TP2- 15°C
TP2- 25°C
3 3

2 2

1 1

0 0
0 Time20
(days) 30 0 20(days)
Time 30

19 Figure 4: Titrable acidity content of raisins (finished product) determined as tartaric

20 acid. Raisins were stored at (A) 57 and (B) 66% relative humidity and at 15 and 25 °
21 C. Control: samples without pretreatment TP1: thermal pretreatment at 50 ° C for 12
22 h. TP2: thermal pretreatment at 50ºC for 48 h.

23

3
Supplementary Material
Click here to download Supplementary Material: Appendix.docx

1 Appendix

A)

2 Appendix 1. XRD diffraction of the samples of Thompson raisins stored at 57%RH

3 and 25 ° C for 30 days. (A), control raisins (B), raisins pre-treated at 50 °C for 48 h.
4
5
6
7
8
9
10
11
12
13
14
15
16
600 80
A) Fresh fruit B)
Control- 15°C 70
500 Control- 25°C
TP1- 15°C 60
Springiness (%)

TP1- 25°C
400 TP2- 15°C
Hardness (N)

50
TP2- 25°C
300 40

200
30

20
100
10
0 0

1
 0.7 200
C) D)
0.6

Chewiness (N)
0.5 150
Cohesiveness

0.4
100
0.3

0.2
50
0.1

0 0

17
18 Appendix 2. Hardness (A), springiness (B), cohesiveness (C) and chewiness (D) for
19 different thermal pre-treatment incubated at 57 %RH. Control: samples without
20 pretreatment TP1: thermal pretreatment at 50 ° C for 12 h. TP2: thermal
21 pretreatment at 50ºC for 48 h.
22
23
24
25
26
27
28
29
30
31
600 80
A) Fresh fruit to B)
500 Control, incub 15°C 70
Control, incub 25°C
60
Springiness (%)

TP1, incub 15°C

Hardness (N)

400 TP1, incub 25°C

TP2, incub 15°C 50
TP2, incub 25°C
300 40

200 30
20
100
10
0 0

2
 0.7 180
C) D)
160
0.6
140

Chewiness (N)
0.5
Cohesiveness

120
0.4 100

0.3 80
60
0.2
40
0.1 20
0 0

32
33 Appendix 3. Hardness (A), springiness (B), cohesiveness (C) and chewiness (D) for
34 different thermal pretreatment incubated at 66 %RH. Control: samples without
35 pretreatment TP1: thermal pretreatment at 50 ° C for 12 h. TP2: thermal
36 pretreatment at 50ºC for 48 h.
37
38
39
40
41
42

3
*Declaration of Interest Statement

Declaration of interests

☒ The authors declare that they have no known competing financial interests or personal
relationships
that could have appeared to influence the work reported in this paper.
☐The authors declare the following financial interests/personal relationships which may be
considered
as potential competing interests: