Accepted Manuscript

Extruded black gram : partial substitute for improving quality characteristics of Indian traditional snack

Laxmi Ananthanarayan, Yogesh Gat, Vikas Kumar, Anil Panghal, Narinder Kaur

PII: S2352-6181(17)30132-4 DOI: 10.1016/j.jef.2017.10.001 Reference: JEF 128

To appear in: Journal of Ethnic Foods

Received Date: 24 July 2017 Revised Date: 6 October 2017 Accepted Date: 10 October 2017

Please cite this article as: Ananthanarayan L, Gat Y, Kumar V, Panghal A, Kaur N, Extruded black gram flour: partial substitute for improving quality characteristics of Indian traditional snack, Journal of Ethnic Foods (2017), doi: 10.1016/j.jef.2017.10.001.

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 Extruded black gram flour: partial substitute for improving quality characteristics of Indian traditional snack Laxmi Ananthanarayan a, Yogesh Gat b* , Vikas Kumar b, Anil Panghal b and Narinder Kaur b aDepartment of Food Engineering and Technology Institute of Chemical Technology, Matunga, Mumbai-400 019, India bDepartment of Food Technology and Nutrition, Lovely Professional University, Phagwara-144 411, India

*Corresponding author: Dr. Yogesh Gat, (Email: [email protected]), Food Technology and Nutrition Department, Lovely Professional University, Jalandhar- 144 411 (India). Abstract Background : During extrusion of black gram flour formation of amylose-lipid complexes lowers down the gelatinization enthalpy of extrudates. While partially gelatinized black gram starch leads to lowering down the water holding capacity and alter functional properties resulting in changing quality attributes of end product upon frying/microwaving/roasting. Methodology : Attempts have been made to improveMANUSCRIPT quality of Indian traditional snack (e.g. papad ) by incorporating extruded black flour as partial substitute for raw (un-extruded) black gram flour. In present work overall quality improvement was achieved by analyzing (a) pre and post frying characteristics (diameter, moisture content, expansion ratio, oil uptake, texture and colour) of papad and, (b) physical properties (colour and viscosity) of fried oil. Results : Four different papad samples were prepared (control papads without addition of papadkhar , papads with use of 3% papadkhar , papads with incorporation of extruded black gram flour at 25% concentration, papads with incorporation of extruded black gram flour at 50% concentration along with 1% papadkhar ) and analyzed along standard market sample. Incorporation of extruded black gram flour in papad resulted in greater expansion with lower oil uptake in fried papad . Further addition of extruded black gram flour permitted use of lower concentrationACCEPTED of papadkhar . Post-frying quality of oil was characterized after numerous frying cycles. Conclusion : Oil used for frying of papads containing highest concentration of papadkhar was effective only up to two frying cycles, after which colour and viscosity increased significantly, adversely affecting quality fried oil. Keywords ACCEPTED MANUSCRIPT Black gram flour; extrusion; pre and post frying characteristics of papad; quality of fried oil

MANUSCRIPT

ACCEPTED ACCEPTED MANUSCRIPT

1 Extruded black gram flour: partial substitute for improving quality characteristics of 2 Indian traditional snack

3 Abstract 4 Background : During extrusion of black gram flour formation of amylose-lipid complexes lowers 5 down the gelatinization enthalpy of extrudates. While partially gelatinized black gram starch 6 leads to lowering down the water holding capacity and alter functional properties resulting in 7 changing quality attributes of end product upon frying/microwaving/roasting. 8 Methodology : Attempts have been made to improve quality of Indian traditional snack (e.g. 9 papad ) by incorporating extruded black flour as partial substitute for raw (un-extruded) black 10 gram flour. In present work overall quality improvement was achieved by analyzing (a) pre and 11 post frying characteristics (diameter, moisture content, expansion ratio, oil uptake, texture and 12 colour) of papad and, (b) physical properties (colour and viscosity) of fried oil. 13 Results : Four different papad samples were prepared (control papads without addition of 14 papadkhar , papads with use of 3% papadkhar, papads with incorporation of extruded black 15 gram flour at 25% concentration, papads with incorporation of extruded black gram flour at 50% 16 concentration along with 1% papadkhar ) and MANUSCRIPT analyzed along standard market sample. 17 Incorporation of extruded black gram flour in papad resulted in greater expansion with lower oil 18 uptake in fried papad . Further addition of extruded black gram flour permitted use of lower 19 concentration of papadkhar . Post-frying quality of oil was characterized after numerous frying 20 cycles. 21 Conclusion : Oil used for frying of papads containing highest concentration of papadkhar was 22 effective only up to two frying cycles, after which colour and viscosity increased significantly, 23 adversely affecting quality fried oil.

24 Keywords 25 Black gram flour; extrusion; pre and post frying characteristics of papad; quality of fried oil

26 1. Introduction ACCEPTED 27 India is the centre of diverse food cultures comprising more than 1,000 major and minor ethnic 28 fermented and non-fermented foods [1]. One of the key players in ethnic foods which have been 29 locally and globally marketed is papad . Papad , the traditional ethnic food of India is also known 30 by different names ( papar, , poppadom ) around the country, but this delectable snack ACCEPTED MANUSCRIPT

31 has made itself a vital item in every household. The Indian papad can best be described as a type 32 of tortilla, wafer or flat bread. An integral part of meals in some parts of the country, while just 33 an appetizer in others, the papad has been part of for what seems like forever. 34 They can come in a variety of types, spices flavored, plain or made of different lentils. However, 35 the papad has been developed mostly over the past couple of centuries or so is having a 36 fascinating history. Traditional ethnic food, viz., papads, pickles and bhujia are predominantly in 37 the hands of small scale sectors having an interesting link to women’s empowerment in the 38 country. However, following economic liberalization, and growth in purchasing power and needs 39 of the consuming class of population, the market for ethnic foods like papad has been growing 40 rapidly both in India and abroad.

41 Papad is a dehydrated snack food made from appropriate mixture of black gram ( Phaseolus 42 mungo ) flour salt and spice powders. Preparation of papad mainly involves rolling dough into a 43 circular shape of 0.5–2.5 mm thickness and then drying to a moisture level of 10–15%. Papads 44 are normally consumed after roasting or frying as an appendage to the full meal. During deep fat 45 frying, heat and mass (moisture and fat) transfer, both within and around the food takes place. 46 Mass transfer (moisture loss and oil uptake), colouMANUSCRIPTr development and texture are the most 47 important factors for describing the quality of fri ed food products. Kinetics of mass transfer, 48 colour and texture change during deep fat frying depend on several factors, such as nature of raw 49 material, initial moisture content, nature of oil, frying temperature and time, product shape and 50 size, pre-treatment [2,3].

51 Extrusion cooking is a continuous cooking, mixing, and forming process which plays a key role 52 in many food processing industries as a versatile, low cost, and very efficient technology [4]. 53 During extrusion cooking raw materials undergo many chemical and structural transformations. 54 Important transformation occurred during extrusion are starch gelatinization, 55 denaturation, complex formation between amylose and lipids, and degradation reactions of 56 , pigments,ACCEPTED etc [5]. Extrusion cooking has been used increasingly in the production of 57 new and traditional food such as cereals, baby foods, flat breads, snacks, meat and 58 cheese analogues, and modified starches, etc [6].

59 Black gram (Phaseolus mungo Roxb ) a major pulse crop of Asian countries is extensively used 60 in preparation of Indian traditional products like idli, dosa and papad . Processing of black gram ACCEPTED MANUSCRIPT

61 has several problems as black gram is difficult to mill due to the presence of vitreous layer of 62 gums and mucilages, which makes it difficult in its use. To overcome these limitations it is 63 necessary to alter the properties of black gram by giving a pretreatment with the help of 64 extrusion and use extruded black gram flour as a processing aid in papad manufacturing to 65 enhances quality of end product upon frying/microwaving/roasting. During extrusion of black 66 gram flour, (i) formation of amylose-lipid complexes lowers down the gelatinization enthalpy of 67 extrudates, (ii) partially gelatinized black gram starch leads to lowering down the water holding 68 capacity and alter functional properties resulting in changing quality attributes of end product 69 upon frying/microwaving/roasting. Some of the researchers have worked on use of extruded 70 flour for the quality improvement of idli [7, 8]. Similarly present study was also undertaken for 71 quality improvement of Indian traditional fried product (e.g. papad ). In this paper quality 72 improvement of papad was undertaken with use of extruded black gram flour as a partial 73 substitute for raw (un-extruded) black gram flour.

74 Very limited information is available on effect of pre-treatment (extrusion processing) on quality 75 of fried papad as well as fried oil. As the consumer perspective expensive nature as well as effect 76 of papad on the frying oil is very important. To checkMANUSCRIPT suitability of frying oil on basis of its 77 quality it is necessary to determine the appropriat e point between usage of frying oil and the 78 safety of final product. Nowadays a major concern is growing with increasing fat in the average 79 diet, so the ability to reduce oil uptake is gaining importance. Current study was undertaken with 80 the objective of comparing commercially available samples with the optimized levels of 81 incorporated extruded for pre- and post-frying quality of papads (moisture content, oil 82 content, oil uptake ratio, % expansion ratio, colour and texture) and their effects on frying oil 83 characteristics (colour and viscosity) after numerous frying cycles.

84 2. Methodology 85 2.1 Materials used 86 Black gram dal (ACCEPTEDVigna Mungo L .) was purchased from a local market of Mumbai city and milled 87 to prepare fine flour passing through 80 mesh sieve. Common salt (Annapurna), asafetida 88 (Ramdev premium), papad khar (Laxmi), market sample (Lijat papad) and refined groundnut oil 89 (Fortune) were used in the study.

90 2.2 Preparation of sample for extrusion ACCEPTED MANUSCRIPT

91 For making extrudates pre-conditioning of sample is undertaken in which, initial moisture 92 content of black gram flour was estimated and a calculated amount of water was added to obtain 93 moisture content of about 14 %. After addition of calculated amount of water into sample, the 94 sample was packed in sealable polyethylene bags and stored at refrigerated condition for uniform 95 distribution and equilibration of moisture throughout the sample.

96 2.3 Extrusion cooking 97 Extrusion cooking was performed with the help of laboratory-scale-co-rotating twin-screw 98 extruder (KETSE 20/40 Brabender GmbH and Co. KG, Duisburg, Germany) suggested by Gat 99 and Ananthanarayan [9]. During extrusion processing feed rate, screw speed and die temperature 100 were kept constant at 14 kg/hr, 300 rpm and 180 °C respectively. After completion of extrusion 101 process black gram extruded were cooled to room temperature (25±3 °C). Ground extruded black 102 gram flour was passed through 80 mesh sieve and then incorporated with raw un-extruded black 103 gram flour at different desired proportions (25% and 50%) for preparation of papad .

104 2.4 Preparation of papad 105 Papads were prepared by following the standardized recipe and procedure devised by Patil et al. 106 [10] with few modifications. Papad dough was prepared MANUSCRIPT by mixing desired amount of black gram 107 flour, salt, papadkhar (as an additive made up of combination of sodium carbonate and sodium 108 bicarbonate) and water. Dough was kneaded until it becomes soft and then it was divided into 109 small balls, which were rolled to have uniform diameter and thickness. Papads were dried in a 110 tray drier at 60 °C to a achieve moisture level of about 14% and then packed in polyethylene bags 111 until further analysis. Four different types of papads were prepared by following the above 112 mentioned procedure with slight modifications in recipe as, (1) control papads (without addition 113 of papadkhar ), (2) papads with use of 3% papadkhar , (3) papads with incorporation of extruded 114 black gram flour at 25% concentration along with 1% papadkhar , (4) papads with incorporation 115 of extruded black gram flour at 50% concentration along with 1% papadkhar .

116 2.5 Frying of papadACCEPTED 117 All five different types of papads were fried in refined groundnut oil for a total period of 40 118 seconds at 175°C. Until further analysis un-fried and fried papad samples (Figure 1 ) were 119 packed in polyethylene bags and stored in air-tight containers. ACCEPTED MANUSCRIPT

120 2.6 Physicochemical analysis 121 2.6.1 Diameter: The diameter of the papad was measured as mentioned by Math et al. [11].

122 2.6.2 Moisture content: The moisture content was determined by oven method [12].

123 2.6.3 Oil content: Oil content was determined by using soxhlet extraction method [12].

124 2.6.4 % expansion: Expansion was calculated by using formula given by Annapure et al. [13].

125 2.6.5 Oil uptake ratio: The (UR) was calculated from the moisture content of papad before and 126 after frying and the oil content of the papad using formula given by Pinthus et al. [14].

127 2.7 Colour measurement 128 Hunter colour parameters (L*, a*, b*) for fried papads were measured with the help of 129 HunterLab colourimeter (LabScan XE, Hunter associates laboratory, Reston, VA, USA) coupled 130 with EasyMatch QC software as suggested by Gat and Ananthanarayan [15].

131 2.8 Texture analysis 132 Texture of the fried papads was determined with the help of a Stable Micro System TAXT2i 133 texture analyzer (Serial No.4650, TEE version 2.64,MANUSCRIPT UK) by using ball probe and a 5 kg load cell 134 with test speed of 1 mm/s up to a distance of 2 mm, using a trigger force of 5 g, and a post-test 135 speed of 10 mm/s. Ten measurements were performed for each sample and their average was 136 taken as the mean value.

137 2.9 Sensory analysis 138 Prepared papads were subjected to sensory analysis based on 9-point hedonic scale for 139 appearance (oily), colour (yellowness), texture (crispness), flavour (black gram aroma), taste 140 (salty) and overall acceptability using a panel of 10 semi-trained panelists (research students and 141 staff members) from Department of Food Engineering, University Institute of Chemical 142 Technology, Mumbai, India who were familiar with the product since childhood. The scores 143 were based on theACCEPTED following criteria: Like extremely: 9; Like moderately: 7-8; like slightly: 5-6; 144 dislike slightly: 3-4; and dislike extremely: 0-2. Each panelist evaluated all samples (identified 145 by unique three-digit codes) in a balanced sequential order. Training sessions were held until 146 panel members could identify the same sample that was coded differently in a session. The 147 scores were averaged and rounded to the nearest whole number. ACCEPTED MANUSCRIPT

148 2.10 Analysis of frying oil 149 Papads were fried in batches as suggested by Patil et al. [10] with few modifications as 150 temperature of frying oil was 175°C for 40 seconds. Frying of each lot of papads was done for 151 four cycles using the same oil. After each frying cycle oil was analyzed for colour and viscosity 152 as reported by Sunisa et al. [16]. Color of oil sample was measured using lovibond tintometer. 153 Viscosity of fried oil was measured according to the modified method of Sanchez-Gimeno et al. 154 [17] using rheometer (Haake, RheoStress RS75, Germany).

155 2.11 Statistical analysis 156 Means and standard deviations of five replicates were determined for all the analysis. Significant 157 difference of mean values was assessed with one-way analysis of variance (ANOVA) followed 158 by Duncan’s LSD test using SPSS software at a significance level of (P ≤0.05). Cluster analyses 159 of data were performed to get comparative comprehensive overview of physico-chemical 160 properties of fried papad. The output obtained was plotted as a dendrogram and the interpretation 161 of data was made, accordingly. Physico-chemical data were subjected to principal component 162 analysis (PCA) to group the related variables into smaller components for the interpretation of 163 their relationship. PCA and cluster analysis was performed using SPSS 16.0 software. MANUSCRIPT 164 3. Results and Discussion 165 3.1 Effect of incorporation of extruded flour and papadkhar on pre- and post- frying quality of 166 papad 167 Table 1 shows the effect of addition of papadkhar on the pre- and post-frying quality of black 168 gram papads . Papad dough prepared without papadkhar , offered resistance to rolling and were 169 poor in diametrical expansion on frying. After addition of 3% papadkhar , dough became easier 170 to roll and helps to expand during frying due to the alkaline nature of the papadkhar . Diameter of 171 both the samples before frying for control sample (without papadkhar ) and papads with added 172 papadkhar (3%) were maintained to near about 11 cm (±0.05). While after frying it was 173 observed that dueACCEPTED to addition of papadkhar , diameters of papads were increased from 12.01 to 174 12.48 cm which leads to increase the percent expansion. Papads prepared without addition of 175 papadkhar gave very poor expansion (8.98%). Increase in level of papadkhar increased 176 expansion as well as oil absorption. Increase in expansion of papad was observed due to action

177 of CO 2 from the sodium carbonate of papadkhar during frying [18]. ACCEPTED MANUSCRIPT

178 From Table 1 it was observed that before frying moisture content of papad was almost similar 179 (i.e. near about 12%), but a significant difference in moisture content of papad samples after 180 frying was observed. As compare to control sample as well as market sample, extruded flour 181 incorporated samples showed higher values for moisture content (6.45%) after frying. These 182 higher moisture content values were might be due to higher water holding capacity of extruded 183 flour incorporated samples during frying. High water holding capacity during frying leads to less 184 oil absorption and so less oil uptake ratio was observed for extruded flour incorporated samples. 185 Texture (crispness) of the fried papad increased with increase in concentration papadkhar 186 (Table 1 ). Due to addition of papadkhar rolling properties as well as expansion of papads 187 increased, with increase in crispness of fried papads as compare to control sample ( papad s 188 without papadkhar ).

189 Colour of fried product is an important parameter and to be controlled during processing together 190 with texture, moisture and oil contents. Colour of the fried product is a result of moisture loss, oil 191 migration and Maillard reaction that depends on the amount of reducing and amino acids 192 of at the surface, temperature and time of frying [19]. Experimental data of hunter 193 colour parameters were shown in Table. 2 . ColourMANUSCRIPT properties of fried papad were determined 194 with the help of lightness (L*) and redness (a*) values. From Table. 2 it was observed that 195 addition of papadkhar gave lighter products, with low red intensity. Besides increasing the 196 brightness incorporation of extruded flour also impart crispness to the fried papad .

197 3.2 Effect of incorporation of extruded flour and papadkhar on PCA and cluster analysis 198 The results of principal component analysis (PCA) indicated that samples (control, sample A, 199 sample B and sample C) were grouped together in the same quadrant, which represents fairly 200 high levels of four attributes (before frying moisture content, after frying moisture content, after 201 frying diameter, crispness and expansion) ( Figure 2). Cluster analysis output of data on the 202 effect of addition of papadkhar and extruded black gram flour in preparation of papad , using 203 flexible strategy ACCEPTED with Euclidean distance as an index was plotted as a dendrogram ( Figure 3). 204 Based upon the sensory properties, cluster analysis distinctly grouped the different papad 205 samples, showing that the influence of market sample was more than the influence of addition of 206 papadkhar and extruded black gram flour in papad preparations.

207 3.3 Effect of incorporation of extruded flour and papadkhar on sensory properties of papad ACCEPTED MANUSCRIPT

208 Sensory analyses showed addition of papadkhar caused a soapy and oily taste with disagreeable 209 mouth feel which is not desirable. Similar results have also been reported earlier by Chaudhary et 210 al. [18]. Extruded flour incorporated papad s had better sensory scores with maximum overall 211 acceptability than papad s prepared with 3% papadkhar (Table 3 ).

212 3.4 Effect of incorporation of extruded flour and papadkhar on quality of fried oil 213 During frying operations, temperature and time was kept constant as 175°C and 40 seconds 214 respectively. As a general rule, with increase in frying time the viscosity of fried oil increases. 215 Therefore to minimize the effect of frying time and frying temperature, both parameters were 216 kept constant. Oil to solid ratio also gives the significant effect on quality of fried oil. Sunisa et 217 al. [16] observed that the color of the fried oil slightly darkened with higher proportion of solid. 218 Therefore, in each batch a constant number of papad from each lot were fried in 500 g of refined 219 groundnut oil and maintained throughout for all four frying cycles. After each frying cycle oil 220 was analyzed for color and viscosity which are considered as physical indicators of oil 221 deterioration caused by oxidation and polymerization.

222 From Table 4 it was observed that for all five samples colour and viscosity of un-fried (control) 223 oil was 0.8 and 65.5cP respectively. While for MANUSCRIPT all samples colour and viscosity increased 224 significantly after different frying cycles. In agreement with this work similar results were 225 observed by Sanchez-Gimeno et al. [17] for sunflower oil. Maximum increase in colour was 226 observed for market samples (4.4-7.9) followed by 3% papadkhar added samples (3.9-7.1). 227 Market samples showed maximum increase in colour value due to the accumulation of non- 228 volatile decomposition products from papad s. After frying cycle one maximum viscosity were 229 observed for market sample (67.1cP), which was increased significantly after each frying cycle. 230 While maximum increase (74.8cP) was observed after frying cycle four. Increase in viscosity of 231 frying oil is may be due to the formation of high molecular weight polymers [20].

232 Control (without papadkhar ) sample showed desirable colour as well as viscosity (3.2 and 233 66.2cP respectively)ACCEPTED values after frying cycle one. While after each frying cycles colour and 234 viscosity of control sample increased minimally. Extruded flour incorporated samples showed 235 minimum deterioration which were having comparable colour and viscosity values as that for 236 control samples. Repeated frying of market sample for more than 2 times (frying cycles) caused 237 more oil deterioration in terms of increase in viscosity and darkening of colour. However, ACCEPTED MANUSCRIPT

238 analysis of the fried oil quality of market samples indicates that it is effective for up to two frying 239 cycles, which would be increased for one more frying cycle with incorporation of extruded flour 240 and by keeping lower concentration of papadkhar .

241 4. Conclusion 242 Addition of papadkhar in control sample resulted in increase of diameter of papad s from 12.01 243 to 12.48cm which leads to increase the percent expansion. After frying extruded flour 244 incorporated papad s showed higher moisture content values, due to the ability of high water 245 holding capacity of extruded flour incorporated samples during frying, which leads to less oil 246 uptake ratio. Papads containing extruded flour had better colour, flavour, texture, taste and 247 overall acceptability scores than papads prepared with 3% papadkhar . 248 Acknowledgement 249 This work was supported by funding from University Grants Commission (UGC), India. 250 References 251 1. Tamang JP. Indian dietary culture. Journal of Ethnic Foods 2016;3:243–5. 252 doi:10.1016/j.jef.2016.11.005. 253 2. Krokida M, Oreopoulou V, Maroulis Z, Marinos-KourisMANUSCRIPT D. Effect of pre-drying on quality 254 of french fries. Journal of Food Engineering 2001;49:347–54. doi:10.1016/s0260- 255 8774(00)00233-8. 256 3. Moyano PC, Berna AZ. Modeling Water Loss During Frying Of Potato Strips: Effect of 257 solute impregnation. Drying Technology 2002;20:1303–18. doi:10.1081/drt-120005854. 258 4. Gat Y, Ananthanarayan L. Effect of extrusion process parameters and pregelatinized rice 259 flour on physicochemical properties of ready-to-eat expanded snacks. Journal of Food 260 Science and Technology 2014;52:2634–45. doi:10.1007/s13197-014-1378-7. 261 5. Ding Q-B, Ainsworth P, Tucker G, Marson H. The effect of extrusion conditions on the 262 physicochemical properties and sensory characteristics of rice-based expanded snacks. 263 Journal of Food Engineering 2005;66:283–9. doi:10.1016/j.jfoodeng.2004.03.019. 264 6. Gujral HS,ACCEPTED Singh N, Singh B. Extrusion behaviour of grits from flint and sweet corn. Food 265 Chemistry 2001;74:303–8. doi:10.1016/s0308-8146(01)00156-x. 266 7. Singh N, Bawa AS, Sekhon KS. Quality improvement of idli using extruded rice flour. 267 Journal of Food Quality 1995;18:193–202. doi:10.1111/j.1745-4557.1995.tb00374.x. ACCEPTED MANUSCRIPT

268 8. Kaur K, Singh N, Singh H. The effect of extruded flour and fermentation time on some 269 quality parameters of idli. Journal of Food Quality 2000;23:15–25. doi:10.1111/j.1745- 270 4557.2000.tb00192.x. 271 9. Gat Y, Ananthanarayan L. Physicochemical, phytochemical and nutritional impact of 272 fortified cereal-based extrudate snacks. Nutrafoods 2015;14:141–9. doi:10.1007/s13749- 273 015-0036-7. 274 10. Patil SJ, Singhal RS, Kulkarni PR. Studies of a 2:1 sodium carbonate:sodium bicarbonate 275 mixture as papadkhar substitute for papads. Food Chemistry 2005;91:51–6. 276 doi:10.1016/j.foodchem.2004.06.006. 277 11. Math R, Velu V, Nagender A, Rao D. Effect of frying conditions on moisture, fat, and 278 density of papad. Journal of Food Engineering 2004;64:429–34. 279 doi:10.1016/j.jfoodeng.2003.11.010. 280 12. AOAC, Official Methods of Analysis, 13th edn. (AOAC, Washington DC, 2002), pp. 1094 281 13. Annapure US, Michael M, Singhal RS, Kulkarni PR. Low-fat papadams from black gram- 282 tapioca blends. International Journal of Food Sciences and Nutrition 1997;48:261–3. 283 doi:10.3109/09637489709028571. 284 14. Pinthus EJ, Weinberg P, Saguy IS. Criterion MANUSCRIPT for Oil Uptake during Deep-fat Frying. 285 Journal of Food Science 1993;58:204–5. doi:10.1111/j.1365-2621.1993.tb03245.x. 286 15. Gat Y, Ananthanarayan L. Use of paprika oily extract as pre-extrusion colouring of rice 287 extrudates: impact of processing and storage on colour stability. Journal of Food Science 288 and Technology 2016;53:2887–94. doi:10.1007/s13197-016-2271-3. 289 16. Sunisa W, Worapong U, Sunisa S, Saowaluck J, Saowakon W. Quality changes of chicken 290 frying oil as affected of frying conditions, International Food Research Journal 2011; 18: 291 615-20. 292 17. Sánchez-Gimeno A, Negueruela A, Benito M, Vercet A, Oria R. Some physical changes in 293 Bajo Aragón extra virgin olive oil during the frying process. Food Chemistry 294 2008;110:654–8.ACCEPTED doi:10.1016/j.foodchem.2008.02.057. 295 18. Chaudhary NM, Rajgopal MV, Roy SP, Mudambi SR. Effect of incorporating papadkhar 296 in papad doughs on the physico-chemical properties of the frying medium, Journal of Food 297 Science and Technology 1985; 22:119–22. ACCEPTED MANUSCRIPT

298 19. Krokida M, Oreopoulou V, Maroulis Z, Marinos-Kouris D. Colour changes during deep fat 299 frying. Journal of Food Engineering 2001;48:219–25. doi:10.1016/s0260-8774(00)00161- 300 8. 301 20. Abdulkarim S, Long K, Lai O, Muhammad S, Ghazali H. Frying quality and stability of 302 high-oleic Moringa oleifera seed oil in comparison with other vegetable oils. Food 303 Chemistry 2007;105:1382–9. doi:10.1016/j.foodchem.2007.05.013. 304 Figure caption: Figure 1 : Photographic image of un-fried and fried papad samples prepared with mixture of 74% of raw un-extrudate black gram flour and 25% of extruded black gram flour along with 1% papadkhar . (Extrudate black gram flour was prepared with the help of laboratory-scale-co- rotating twin-screw extruder by keeping constant feed rate, screw speed and die temperature at 14 kg/hr, 300 rpm and 180 °C respectively. Papadkhar was used as an additive which is made up of combination of sodium carbonate and sodium bicarbonate to improve the quality of fried papad. Frying of papad was carried out in refined groundnut oil for a total period of 40 seconds at 175 ± 5°C).

Figure 2: Principal component plot of descriptive analysis of the papad samples (Control, Sample A: papads with use of 3% papadkhar ; Sample B: papads with incorporation of extruded black gram flour at 25% concentration along with 1% papadkhar ; Sample C: papads with incorporation of extruded black gram flour at 50%MANUSCRIPT concentration along with 1% papadkhar ; Market sample) and physico-chemical properties (AFMC: after frying moisture content; BFMC: before frying moisture content; BFD: before frying diameter; AFD: after frying diameter; OUR: oil uptake ratio; OC: oil content; crispness; expansion).

Figure 3: Dendrogram of sensory analysis data of papad samples (Control, Sample A: papads with use of 3% papadkhar ; Sample B: papads with incorporation of extruded black gram flour at 25% concentration along with 1% papadkhar ; Sample C: papads with incorporation of extruded black gram flour at 50% concentration along with 1% papadkhar ; Market sample) as affected by addition of papadkhar and extruded black gram flour on sensory properties.

ACCEPTED ACCEPTED MANUSCRIPT

Table 1: Effect of incorporation of extruded flour and papadkhar on pre- and post-frying physicochemical properties of black gram-based papad

Physicochemical properties Control Sample A Sample B Sample C Market sample Before frying a a a a a Diameter (cm) 11.03±0.03 11.08±0.05 11.07±0.03 11.04±0.03 11.05±0.03 Moisture content (%) 12.54±0.04 c 12.45±0.05 d 12.84±0.04 a 12.63±0.06 b 12.64±0.05 b After frying

Diameter (cm) 12.00±0.05 e 12.47±0.04 d 12.56±0.02 c 13.12±0.05 b 13.54±0.02 a Moisture content (%) 5.61±0.03 d 5.55±0.03 e 6.28±0.03 b 6.45±0.04 a 5.72±0.02 c % expansion 8.98 12.53 13.36 18.84 22.51 b a d e c Oil content (%) 17.12±0.07 18.55±0.05 13.55±0.04 13.13±0.06 15.00±0.05 Oil uptake ratio 2.48 2.68 2.17 2.13 2.27 MANUSCRIPT Texture-crispness (N) 2.31±0.80 e 2.62±0.10 d 2.69±0.50c 2.82±0.40b 2.95±0.40 a

All the values are mean ± SD of five replicates. Mean values with different superscripts on the same row differ significantly (Duncan’s LSD test, P < 0.05). Where, Sample A: papads with use of 3% papadkhar , Sample B: papads with incorporation of extruded black gram flour at 25% concentration along with 1% papadkhar , Sample C: papads with incorporation of extruded black gram flour at 50% concentration along with 1% papadkhar .

ACCEPTED

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Table 2: Effect of incorporation of extruded flour and papadkhar on pre- and post-frying colour properties of black gram-based papad

L* a* b* Before frying After frying Before frying After frying Before frying After frying Control 65.48±0.06 d 63.72±0.03 d 3.58±0.05 c 5.03±0.02 c 27.87±0.02 b 28.23±0.06 c Sample A 67.34±0.04 c 64.13±0.02 c 3.75±0.05 b 5.36±0.07 b 27.34±0.04 c 29.55±0.05 b Sample B 63.53±0.03 d 62.02±0.02 e 3.93±0.06 a 5.77±0.07 a 28.10±0.05 a 29.91±0.04 a Sample C 71.03±0.02 b 69.26±0.03 b 3.65±0.05 c 4.75±0.05 d 26.87±0.03 d 27.74±0.04 e Market sample 75.44±0.04 a 73.75±0.05 a 3.60±0.02 c 4.83±0.08 d 26.76±0.06 e 27.87±0.07 d All the values are mean ± SD of five replicates. Mean values with different superscripts on the same column differ significantly (Duncan’s LSD test, P < 0.05). Where, Sample A: papads with use of 3% papadkhar , Sample B: papads with incorporation of extruded black gram flour at 25% concentration along with 1% papadkhar , Sample C: papads with incorporation of extruded black gram flour at 50% concentration along with 1% papadkhar .

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Table 3: Effect of incorporation of extruded flour and papadkhar on sensory analysis of black gram-based fried papad

Control Sample A Sample B Sample C Market sample

Appearance (oily) 6.7±0.2 b 7.2±0.2 a 6.6±0.2 b 6.5±0.1 b 5.5±0.2 c Colour (yellowness) 7.2±0.1 c 7.4±0.3b c 6.2±0.2 d 7.7±0.2 b 8.2±0.2 a Flavour (blackgram aroma) 7.1±0.3 a 6.8±0.2 ab 6.4±0.1b c 6.2±0.2 c 7.2±0.4 a Texture (crispness) 6.6±0.3 d 7.2±0.2 c 7.4±0.2b c 7.9±0.4 ab 8.0±0.2 a Taste (salty) 5.4±0.4 c 7.3±0.3 b 5.6±0.1 c 7.2±0.2 b 7.8±0.2 a Overall acceptability 6.8±0.2 c 7.3±0.2 b 7.8±0.3 a 8.0±0.2 a 8.1±0.1 a All the values are mean ± SD of five replicates. Mean values with different superscripts on the same row differ significantly (Duncan’s LSD test, P < 0.05). Where, Sample A: papads with use of 3% papadkhar , Sample B: papads with incorporation of extruded black gram flour at 25% concentration along with 1% papadkhar , Sample C: papads with incorporation of extruded black gram flour at 50% concentration along with 1% papadkhar .

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Table 4: Effect of multiple frying cycles on colour and viscosity of fried oil

Un-fried Frying cycle 1 Frying cycle 2 Frying cycle 3 Frying cycle 4 Colour (tintometer units) Control 0.7±0.01a 3.0±0.02 c 4.0±0.01c 5.3±0.03b 6.5±0.01a Sample A 0.8±0.02a 3.9±0.04b 4.8±0.02 b 5.9±0.03b 7.1±0.04 b Sample B 0.8±0.03a 3.5±0.02b 4.5±0.01b 5.6±0.04b 6.8±0.03c Sample C 0.8±0.01a 3.7±0.02b 4.7±0.04b 5.8±0.03b 7.0±0.02b Market sample 0.8±0.02 a 4.4±0.02a 5.2±0.02a 6.5±0.04a 7.9±0.01a

Viscosity (cP) Control 65.5±0.4 a 66.2±0.3 b 67.3±0.3 a 68.9±0.1 c 70.5±0.5 c Sample A 65.6±0.3 a 66.8±0.3 ab 67.9±0.1 a 69.7± 0.2 b 71.2±0.2 b Sample B 65.6±0.5 a 66.5 ± 0.5ab 67.4±0.4 a 69.5±0.5 b 70.8±0.2 bc Sample C 65.5±0.5 a 66.7 ± 0.3ab 67.8±0.2 a 69.9±0.1 b 71.1±0.1 b Market sample 65.5±0.5 a 67.1± 0.1a 69.0±0.2 a 72.1±0.1 a 74.8±0.2a All the values are mean ± SD of five replicates. MANUSCRIPT Mean values with different superscripts on the same column differ significantly (Duncan’s LSD test, P < 0.05). Where, Sample A: papads with use of 3% papadkhar , Sample B: papads with incorporation of extruded black gram flour at 25% concentration along with 1% papadkhar , Sample C: papads with incorporation of extruded black gram flour at 50% concentration along with 1% papadkhar .

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Figure 1 : Photographic image of un-fried and fried papad samples MANUSCRIPTprepared with mixture of 74% of raw un-extrudate black gram flour and 25% of extruded black gram flour along with 1% papadkhar. (Extrudate black gram flour was prepared with the help of laboratory-scale-co-rotating twin-screw extruder by keeping constant feed rate, screw speed and die temperature at 14 kg/hr, 300 rpm and 180 °C respectively. Papadkhar was used as an additive which is made up of combination of sodium carbonate and sodium bicarbonate to improve the quality of fried papad. Frying of papad was carried out in refined groundnut oil for a total period of 40 seconds at 175 ± 5 °C).

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Figure 2: Principal component plot of descriptive analysis of the papad samples (Control, Sample A: papads with use of 3% papadkhar ; Sample B: papads with incorporation of extruded black gram flour at 25% concentration along with 1% papadkhar ; Sample C: papads with incorporation of extrudedACCEPTED black gram flour at 50% concentration along with 1% papadkhar ; Market sample) and physico-chemical properties (AFMC: after frying moisture content; BFMC: before frying moisture content; BFD: before frying diameter; AFD: after frying diameter; OUR: oil uptake ratio; OC: oil content; crispness; expansion). ACCEPTED MANUSCRIPT

MANUSCRIPT Figure 3: Dendrogram of sensory analysis data of papad samples (Control, Sample A: papads with use of 3% papadkhar ; Sample B: papads with incorporation of extruded black gram flour at 25% concentration along with 1% papadkhar ; Sample C: papads with incorporation of extruded black gram flour at 50% concentration along with 1% papadkhar ; Market sample) as affected by addition of papadkhar and extruded black gram flour on sensory properties.

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