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Accepted Manuscript Improving 3D printing process of lemon juice gel based on fluid flow numerical simulation Fanli Yang, Chaofan Guo, Min Zhang, Bhesh Bhandari, Yaping Liu PII: S0023-6438(18)31089-2 DOI: https://doi.org/10.1016/j.lwt.2018.12.031 Reference: YFSTL 7692 To appear in: LWT - Food Science and Technology Received Date: 17 August 2018 Revised Date: 25 November 2018 Accepted Date: 9 December 2018 Please cite this article as: Yang, F., Guo, C., Zhang, M., Bhandari, B., Liu, Y., Improving 3D printing process of lemon juice gel based on fluid flow numerical simulation, LWT - Food Science and Technology (2019), doi: https://doi.org/10.1016/j.lwt.2018.12.031. 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.

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Accepted Manuscript

Improving 3D printing process of lemon juice gel based on fluid flow numericalsimulation

Fanli Yang, Chaofan Guo, Min Zhang, Bhesh Bhandari, Yaping Liu

PII: S0023-6438(18)31089-2

DOI: https://doi.org/10.1016/j.lwt.2018.12.031

Reference: YFSTL 7692

To appear in: LWT - Food Science and Technology

Received Date: 17 August 2018

Revised Date: 25 November 2018

Accepted Date: 9 December 2018

Please cite this article as: Yang, F., Guo, C., Zhang, M., Bhandari, B., Liu, Y., Improving 3D printingprocess of lemon juice gel based on fluid flow numerical simulation, LWT - Food Science andTechnology (2019), doi: https://doi.org/10.1016/j.lwt.2018.12.031.

This is a PDF file of an unedited manuscript that has been accepted for publication. As a service toour customers we are providing this early version of the manuscript. The manuscript will undergocopyediting, typesetting, and review of the resulting proof before it is published in its final form. Pleasenote that during the production process errors may be discovered which could affect the content, and alllegal disclaimers that apply to the journal pertain.

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Improving 3D Printing Process of Lemon Juice Gel Based on Fluid Flow Numerical 1 Simulation 2

3

Fanli Yanga, Chaofan Guoa, Min Zhanga,b*, Bhesh Bhandaric, Yaping Liu d 4

5

aState Key Laboratory of Food Science and Technology, Jiangnan University, 14122 6

Wuxi, Jiangsu, China 7

bJiangsu Province Key Laboratory of Advanced Food Manufacturing Equipment and 8

Technology, Jiangnan University, China 9

cSchool of Agriculture and Food Sciences, University of Queensland, Brisbane, QLD, 10

Australia 11

d Guangdong Galore Food Co. Ltd, Zhongshan 528447, China 12

13

14

*Corresponding author: Dr. Min Zhang, Professor of School of Food Science and 15

Technology, Jiangnan University, 214122 Wuxi, P. R. China. 16

Tel.: 0086-510-85877225; Fax: 0086-510-85877225; 17

E-mail: [email protected] 18

19

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Abstract 20

Food 3D printing has received attention as a novel field in recent years, bringing 21

new ideas and opportunities for the development and transformation of food 22

processing technology. This work investigated the moisture and rheological properties 23

of lemon juice gels with different starches by experimental studies and simulated the 24

effect of different material properties and process parameters (material viscosity and 25

relaxation time, inlet volume flow rate and nozzle diameter) on the velocity, shear rate 26

and pressure fields in the flow channel by the POLYFLOW software. Results showed 27

that with the addition of different kinds of starches, the viscosity and mechanical 28

properties of the lemon juice gel were varied. Adding potato starch altered fluidity 29

with different relative degree of bound or immobilized water of lemon juice gel. 30

According to the simulation study, in the same shape of the flow path, the velocity and 31

shear velocity fields were determined by the inlet volume flow rate. The change of 32

different process parameters was found to cause changes in pressure field in the flow 33

channel to varying degrees, and the change of the nozzle diameter had the greatest 34

influence on the pressure distribution. In addition, the extruded material exhibited 35

swelling phenomenon. 36

Keywords: 3D printing, Lemon juice gel, POLYFLOW, Numerical simulation, NMR, 37

Rheology 38

39

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1. Introduction 40

Three-dimensional (3D) printing, also known as additive layer manufacturing, is 41

a new rapid prototyping technology, which integrates computer technology, precision 42

drive technology, numerical control technology and material science technology. In 43

the process of printing, the material is usually passed through a nozzle whose position 44

is controlled by a shape design model (Lee, Jia, & Chua, 2017). There are many 45

unique advantages of application of 3D printing in food field, such as food structure 46

customization, customized and digitalized nutrition (Godoi, Prakash, & Bhandari, 47

2016), broadening the source of food raw materials, and shortening the food supply 48

chain (Chen, 2016; Jia, Wang, Mustafee, & Hao, 2016). 49

There are several types of raw material formats used in 3D printing such as 50

powder and paste. For powder materials, the printing methods used can be categorized 51

as selective sintering (Gray, 2010), binder jetting (Yang, Wu, & Liu, 2001) and 52

hot-melt extrusion (Lanaro et al., 2017) methods. These methods are reported for 53

printing powder materials, such as sugar and chocolates (Sun, Zhou, Huang, Fuh, & 54

Hong, 2015). In the paste method extrusion, the material is ejected from the nozzle by 55

pressure. The extrusion method can be divided into three categories: (1) rotary screw 56

extrusion, (2) time pressure dispensing and (3) positive displacement (Liu, Zhang, 57

Bhandari, & Wang, 2017). In the rotary screw extrusion method, the extrusion of food 58

materials is driven by a rotational screw, where the extrusion rate is determined by the 59

speed of motor. This method feeds continuously and is suitable for materials with a 60

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wide viscosity range. However, it is very troublesome to clean and maintain in 61

practice. In addition, the material is directly in contact with the machine, which can 62

have potential food safety problems. In the time pressure dispensing method, the air 63

pressure controls the flow of food materials. The equipment used in this method is 64

cheap and easy to operate. However, it is difficult to fill/refill materials with high 65

viscosity without air bubbles (Sun, Zhou, Yan, Huang, & Lin, 2018). In the positive 66

displacement method, a piston connected to a stepping motor moves down and 67

extrudes the material out of nozzle. The material is stored in a special charging barrel 68

to facilitate the cleaning of the equipment. Moreover, this method has a good 69

sensitivity and high accuracy due to the direct connection between the piston and 70

stepping motor (Lille, Nurmela, Nordlund, Metsä-Kortelainen, & Sozer, 2018). 71

The POLYFLOW software based on finite element method (FEM) has powerful 72

functions in solving non-Newtonian fluid and nonlinear flow problems (Wilczyński, 73

Laczyński, & Czaplarski, 1998). This software has been widely used for 74

simulating/modeling of plastics processing (Wilczyński & Tyszkiewicz, 1996), 75

screw-based extrusion (T. Chen et al., 2017) and pipe flow simulation (Filali, Khezzar, 76

Siginer, & Nemouchi, 2012). For syringe-based extrusion 3D printing process, the 77

extruding process can be regarded as a pipe flow situation, and thus can be modeled 78

by FEM. Recently, 3D printing is being widely investigated for the application in food 79

sector. Many kinds of food materials have been printed using extrusion-based printing 80

technology, such as processed cheese (Le Tohic et al., 2017), pectin gel 81

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(Vancauwenberghe et al., 2017), mashed potatoes (Liu, Zhang, Bhandari, & Yang, 82

2017), fish surimi gels (Wang, Zhang, Bhandari, & Yang, 2017), fruit-based snacks 83

(Derossi, Caporizzi, Azzollini, & Severini, 2017), chocolate (Hao et al., 2010; Li et 84

al., 2014) and many other food products (Calvert, 2016). It is worth noting that these 85

materials are pseudoplastic before gelation and should be considered viscoelastic after 86

gelation. In addition, because of the closed environment of the printer, it is difficult to 87

observe the fluid characteristic changes of material flow during 3D printing process. 88

Therefore, the predictability of the flow properties of materials is important to 89

understand the 3D printing. Based on our previous study, lemon juice gel prepared 90

from lemon juice and starch was found to be suitable for 3D printing (F. Yang, Zhang, 91

Bhandari, & Liu, 2018). Thus, the effect of the addition of different starches on the 92

rheological properties of lemon juice gel was studied in this work. POLYFLOW 93

software was used to simulate the fluid characteristic of inks in the flow channel of 94

the positive displacement 3D printers under different technological parameters 95

(viscosity, relaxation time, inlet volume flow rate ratio and nozzle diameter), to 96

provide a theoretical basis for 3D printing of food materials. 97

98

2. Materials and Methods 99

2.1. Raw Material 100

Lemon juice was provided by Jiahao Co. Ltd. Guangdong, China. The moisture 101

content of the lemon juice was 59.82 g/100 g (determined by the vacuum-drying 102

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method). The pH of lemon juice was measured as 2.28. 103

Potato starch, sweet potato starch, wheat starch and corn starch were purchased 104

from Shanghai Tianyu Food Co. Ltd and stored at normal atmospheric temperature. 105

The moisture content determined by vacuum-oven drying method was 13.47±0.46 106

g/100g for potato starch, 14.35±0.48 g/100g for sweet potato starch, 12.96±0.55 107

g/100g for wheat starch and 12.83±0.58 g/100g for corn starch. Lemon juice was 108

firstly mixed with different kinds of starches (15 g/ 100g ) and then homogenized by 109

using a mixer (ULTRA-TURRAX® IKA® T18 basic, Model: T18BS25, Germany). 110

Afterwards, mixtures were transferred to glass containers and cooked in a water bath 111

for 15 minutes until the center temperature reached to 75±2°C. During the cooking 112

process, containers were wrapped with food grade plastic protective films to prevent 113

the water loss. Finally, samples were cooled down to room temperature to form a 114

weak gel-like structure and then stored at 4 °C for forth coming test and printing 115

process. These sample preparing methods are based on former study (Yang et al., 116

2018). 117

2.2. Low-field nuclear magnetic resonance (NMR) analysis 118

A low field pulsed NMI 20 analyzer (Shanghai Niumag Corporation, China) at 119

22.6 MHz was used in this experiment for determining status of moisture in the 120

sample. The measurement method and parameters setting were same as previous 121

study (Yang et al., 2018). Each sample (about 5 g) was analyzed three times. 122

2.3. Rheological measurements 123

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Rheological measurements of samples were undertaken by a hybrid rheometer 124

(Discovery HR-3, DHR, TA Instruments, USA) equipped with a parallel plate 125

(diameter=20 mm). The viscosity and dynamic viscoelastic measurements were 126

carried out similar to previous study (Yang et al., 2018). Before measurements, 127

samples were rested at 25 °C for 2 min. The viscosity parameters were obtained in the 128

shear rate ranging from 0.1 to 100/s. Dynamic viscoelastic properties were 129

characterized at frequencies from 0.01 to 10 rad/s, and all measurements were 130

performed within the identified linear viscoelastic region and made at 0.4% strain. 131

Experiments were conducted in triplicate for each type of sample. 132

2.4. POLYFLOW software Numerical analysis 133

2.4.1. Simulation scheme 134

The viscosity of materials, the inlet volume rate and the nozzle diameter are all 135

important factors that affect parameters of the flow channel. In this work, the 136

influence of different process parameters on rheological parameters in a convective 137

channel was investigated by changing certain parameters but keeping the other 138

parameters unchanged. 139

2.4.2. Hypothesis and model establishment 140

Due to the complexity of the flow state of materials, it is difficult to accurately 141

describe the flow characteristic, and some assumptions were employed to simplify the 142

flow behavior. 143

1) The material used for extrusion is an incompressible, highly viscous, 144

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non-Newtonian fluid. 145

2) The material is fully filled in the mold, and it is isothermal, steady and laminar 146

flow in the flow channel. 147

3) Due to the high viscosity of the material, its inertia force and gravity are far 148

less than viscous force thus are ignored. 149

4) No slip between the material and the wall of the channel during the extrusion 150

process. 151

The Carreau model is a special form of Carreau-Yasuda rheological model. The 152

model has wide application scope and can accurately describe the rheological curve of 153

fluid at low and moderate shear rates. Its constitutive equation is as follows: 154

( ) ( )1

2 20 1

n

η η η η λγ−

∞ ∞ = + − + 155

η is viscosity, η0 is zero shear viscosity, η∞ is infinite shear viscosity, λ is 156

relaxation time, γ is shear rate, n is the rheological index. 157

2.4.3. Physical model 158

According to the shape of the charging barrel structure of the syringe used in 3D 159

printing (Fig. 1), physical models created by the Repetier Host V2.0.5 and Slic3r 160

software (Hot-World GmbH & Co. KG, Willich, Germany) are shown in Fig. 1. The 161

model numbered e used 2D 1/2 axisymmetric graphics to simplify the model. The 162

generation of meshing was set automatically with elements size as 0.8 mm, and three 163

faces (boundary input, output and wall) were assigned (Fig. 1). The task was set as 164

FEM, steady-state and isothermal, and then materials data was entered (type of 165

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viscosity model (Bird-carreau) 166

The boundary was set as following: Boundary 1, Input=inflow, set inlet volume 167

flow rate; Boundary 2, Output=outflow, zero normal force and zero surface force 168

condition fn=0, fs=0; Boundary 3, Wall=zero normal velocity and zero surface velocity 169

condition vn=0, vs=0. 170

2.4.4. Solution and result 171

Contours of output parameters (velocity, shear rate, pressure) are graphically 172

represented at every mesh of the structural geometry. On the Y axis, the part greater 173

than 0 represented the barrel, and the part less than 0 represented the nozzle. Planes 174

were set up at every 2 mm in the flow path to calculate the average value of 175

parameters. 176

2.5 Printing experiment 177

The printing experiment was carried out by a syringe-based extrusion 3D printing 178

unit (Shiyin Co. Ltd, Hangzhou, China), which is same as used by Liu, Bhandari, 179

Prakash, and Zhang (2018) as shown in Fig. 2. A template of cubical shape (10×10×1 180

mm3) was designed by Rhinoceros 5.0 and sliced by the Slic3r software into 181

stereolithography file. The printing parameters were set the same as in previous study 182

(Yang et al., 2018). 183

2.6. Statistical Analysis 184

Analysis of variance was performed and mean comparisons were run by 185

Duncan’s multiple-range test using SPSS software (SPSS 19.0; IBM SPSS Statistics, 186

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Chicago, IL, USA). Significant differences (p < 0.05) between mean values of 187

samples were determined. 188

189

3. Results and Discussion 190

3.1. LF-NMR spin-spin relaxation times (T2) of the materials 191

NMR analysis shows the distribution of water in different states in the material. 192

A small transverse relaxation time (T2) means that the moisture is tightly bound with 193

non-aqueous components, and the degree of moisture freedom is low. While a big T2 194

peak means that the moisture is not well-knit with non-aqueous components, and the 195

degree of moisture freedom is high. It can be observed from Fig. 3a that there were 196

three peaks in each sample. Three relaxation populations of samples were centered at 197

approximately 0.1-10 ms (T21), 10-100 ms (T22), and 100-1000 ms (T23), which were 198

assigned to the bound, partially immobilized, and free water, respectively (Wang et 199

al., 2017). 200

As shown in Fig. 3a, the moisture distribution of samples with different starches 201

was found to be different. The curve of samples added with wheat starch was found at 202

the most left, while the curve of the sample added with potato starch was found at the 203

most right, indicating that the sample added with potato starch had better fluidity with 204

less relative degree of bound or immobilized water. Our previous work also suggested 205

that with the addition of starch, the peak of samples shifted to the left, while 206

increasing the value of rheological parameters (G′, G″ and viscosity) presenting a 207

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better extrudate appearance (Yang et al., 2018). 208

Overall, from Fig. 3a, the free water and the bound water relative intensity were 209

found nearly zero, while the relative intensity of the partially immobilized water was 210

far greater. This suggested that the water state in the samples was mainly partially 211

immobilized water, thus, the samples had a certain fluidity and formability, which is 212

beneficial to the extrusion of 3D printing processes while maintaining the product 213

structure after printing. When the slurry revealed low fluidity with more solid-like 214

behavior, it was difficult extrude and the extruded filament was found to be broken 215

during deposition. Too much liquid-like slurries with high fluidity were also reported 216

to extrude larger amount of material extrusion than the set value affecting the 217

precision of geometry (Yang et al., 2018). It can be seen that the relative intensity of 218

free water of samples added with sweet potato starch is almost 0, indicating that the 219

internal water was mainly in the form of bound water and partially immobilized water, 220

which resulted in too much solid-behavior which may not be also suitable for the 221

extrusion. 222

3.2. Rheological behavior of the materials 223

Rheological properties are important indicators for evaluating the 3D printing 224

performance of materials (Derossi et al., 2017; Liu, Zhang, Bhandari, & Yang, 2017). 225

The viscosity of ideal food materials suitable for 3D printing should be low enough to 226

permit easy extrusion through a small nozzle and high enough to be cohesive without 227

deformation with the previous deposited layers (Lille, Nurmela, Nordlund, 228

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Metsä-Kortelainen, & Sozer, 2017). Flow curves, as shown in Fig. 3b, illustrate the 229

dependence of apparent viscosities on shear rate. This suggested that lemon juice gels 230

added with different starches were all pseudoplastic fluids displaying shear-thinning 231

performances. The shear-thinning performance signifies that the chain of molecules or 232

particles in materials are affected by the shear stress between the layers when the flow 233

rate increases, thereby reducing the force between the molecules or particles 234

(Demirkesen, Mert, Sumnu, & Sahin, 2010). This shear-thinning performance was 235

reported beneficial for slurries to be extruded through the nozzle (Liu, Zhang, 236

Bhandari, & Yang, 2018). 237

The storage modulus (G') is a measure of the elastic solid-like behavior, which 238

reflects the mechanical strength of samples. The material with high mechanical 239

strength will show excellent self-supporting property after deposition and maintain a 240

stable shape after printing (Avery et al., 2014; Liu, Zhang, Bhandari, & Yang, 2017). 241

The loss modulus (G'') is the viscous response which is a ratio of stress to strain under 242

the dynamic oscillation frequency analysis. The loss tangent (tan δ= G''/G') is used as 243

a characteristic parameter to illustrate the different viscoelastic behavior (Fischer & 244

Windhab, 2011). A tan δ smaller than 1 means predominantly elastic property which 245

exhibiting solid characteristics. And, conversely, when tan δ is greater than 1, the 246

viscous property exhibits liquid characteristics (Winter & Mours, 1997). 247

Considering the viscoelastic properties of lemon juice gel, G' was found all 248

higher than G'' (Fig. 3c and Fig. 3d), which indicated that the materials formed elastic 249

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gel or gel-like structures and the system of materials is in the state of elastic 250

dominance. Samples added with potato starch and wheat starch showed greater G' and 251

G'' than those added with corn starch and sweet potato starch. G' and G'' both 252

gradually increased with the increasing of oscillatory frequency, meanwhile tan δ was 253

found decreased at first, followed by an increase (Fig. 3e). However, tan δ for all 254

samples were found smaller than 1, indicating that all samples showed solid-like 255

behavior and poor fluidity. In addition, comparing the samples added with four kinds 256

of starches, it can be seen that the sample added with potato and corn starches had 257

smaller tan δ, showing that these two materials had stronger network structure and 258

more solid-like behavior. From the result of rheological tests of lemon-juice gel added 259

with four kinds of starches, the gel sample added with corn starch was found to have a 260

lower viscosity at high shear rates and relatively small tan δ. These results suggested 261

that the gel added with corn starch will be easy to be extruded by the syringe, which 262

offers a high shear rate at the exit (Fig. 4c), meanwhile presenting a good mechanical 263

properties (Liu, Zhang, Bhandari, & Wang, 2017; F. Yang et al., 2018; Zhang, Zhang, 264

Yang, & Chen, 2001). 265

3.3. Velocity distribution field analysis 266

The velocity field was reported to have a direct impact on the quality of the 267

material 3D printing, which is mainly reflected by the uniformity of the speed of the 268

material extrusion at the exit (Wang et al., 2017; Yang et al., 2018). 269

Fig. 4a and Fig. 4b show the distribution of velocity field at the channel and the 270

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outlet, respectively, at the condition of material viscosity 8000 Pa·s, relaxation time 271

10 s, inlet volume flow rate 24 mm3/s and nozzle diameter 1.0 mm. It can be seen 272

intuitively that the material in the barrel part was in a low speed state (0.08 mm/s), 273

and the velocity showed no obvious change (Fig. 4a), while the material in the nozzle 274

was found to have a high speed. Meanwhile, the velocity of the material increased 275

obviously with a shrinkage of the nozzle diameter (the average speed of the materials 276

increased from 1.59 mm/s to 40.1 mm/s). Fig. 4b shows that on the same horizontal 277

section, the velocity of fluids decreased from the center to the surrounding. The 278

velocity at the center of nozzle was found to be maximum, while the nearer the wall, 279

the velocity of the material was lower. This was mainly due to the fact that a greater 280

influence of the friction of the material on the solid wall results in a considerable 281

velocity gradient along the normal to the wall (Rueda et al., 2016). 282

3.4. Shear rate field analysis 283

The viscosity of materials belonging to the pseudoplastic group of fluid presents 284

an alterable value with the change of shear rates, which will affect the quality of the 285

3D printing products. Fig. 4c and Fig. 4d show the distribution of the shear rate field 286

at the channel and outlet, respectively. In the barrel, the shear rate was found not 287

greatly changed, while the shear rate increases obviously with the decrease of the 288

diameter in the nozzle (Fig. 4c). The change of the shear rate in the flow channel was 289

shown to be small, while it turned to be larger near the wall (Fig. 4d). This 290

phenomenon indicated that the material was subjected to a larger shear force at the 291

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wall, and also caused considerable velocity gradient along the normal direction of the 292

wall. Meanwhile, due to high shear rates at the exit of nozzle, the viscosity of the 293

material decreased indicating that the material was more easily extruded during 3D 294

printing process. 295

3.5. Pressure distribution field analysis 296

Pressure will have a significant impact on material extrusion process in a 297

continuous extrusion 3D printing process (Valkenaers, Jansen, Voet, Van Gysel, & 298

Ferraris, 2014). Fig. 4e shows the distribution of the pressure field at the channel and 299

the nozzle. As shown in Fig. 4e, the pressure on the same horizontal section showed to 300

be constant. Additionally, the pressure was stable in the barrel while it noticeable 301

changed in the nozzle. From the entrance to the exit of the nozzle, the pressure 302

gradually decreased, with no alteration observed, indicating that as long as the 303

material is under a sufficient pressure, the material flow can be stabile and 304

continuously extruded, meeting the requirements of 3D printing. 305

3.6. Effect of material viscosity on the parameters in the flow channel 306

From above sections, the viscosity of materials with different starches was found 307

to be different, which will affect the rheological parameters in the flow channel during 308

the 3D printing extrusion process. Thus, it is important to investigate effects of the 309

viscosity with changing values on the other parameters, such as shear rate and 310

pressure field. 311

The velocity field and shear rate field in the flow channel were found not to be 312

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changed with the change of the viscosity of the material (Fig. 5a and Fig. 5b), which 313

mainly depended on the inlet volume flow rate. The pressure field changed obviously 314

with the change of material viscosities (Fig. 5c). With the decreasing of the viscosity 315

of materials, the overall pressure in the channel was found to be decreased. When the 316

viscosity decreased from 12000 Pa to 8000 Pa (by 30%), the pressure at the inlet of 317

the nozzle presented a reduction from 1.36×107 to 9.10×106 Pa and the decrease is 318

about 33%, which was found to be similar with the decrease of material viscosity. At a 319

constant viscosity, the pressure on the barrel varied little along the extrusion direction 320

of the material. Whereas at the nozzle, the greater the viscosity was, the faster the 321

pressure dropped, and the pressure tended to be the same at the outlet of the nozzle. 322

In addition, the pressure required for extruding materials should be at 323

comfortable values below the maximum pressure provided by the 3D printer. 324

Therefore, in the actual operation of 3D printing, the material can be adjusted to a 325

proper viscosity by proportionating formulation ensuring that the pressure in the 326

process is in a reasonable range. In present work, different starch additions provided 327

diverse viscosity increments. Among them, the lemon-juice gel added with corn starch 328

presented relatively low viscosities at high shear rates indicating that the gel added 329

with corn starch will flow smoothly at the nozzle and close to the exit than that added 330

with other starches. 331

3.7. Effect of inlet volume flow rate on the parameters in the flow channel 332

In food 3D printing processes, the material needs to be extruded under certain 333

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pressure provided by the stepper motor of the 3D printer. In the syringe-based 334

extrusion printing process, the inlet volume flow rate is adjusted by changing the 335

speed of the piston, which is a key factor that affects the parameters of the flow path 336

and the 3D printing efficiency. Thus, this section investigated the effect of the inlet 337

volume flow rate at different values on the parameters in the flow channel. 338

The velocity, shear rate and pressure fields of the flow channel increased with the 339

increase of the entrance volume flow rate (Fig. 6a and Fig. 6b). With the increasing of 340

inlet volume flow rate from 20 mm3/s to 28 mm3/s (by 40%), the average velocity at 341

the outlet of the nozzle increased from 33.42 mm/s to 46.78 mm/s, while the average 342

shear rate increased from 86.44/s to 121.01/s (by 40%). This result was found to be 343

similar with the increase at the volume rate of the entrance (Fig. 6a and 6b). The 344

pressure at the inlet of the nozzle was found increased from 1.32×106 to 1.85×106 Pa, 345

and tended to be the same at the exit, indicating that the pressure gradually increased 346

in the flow channel (Fig. 6c). However, the trend of the rheological parameters in the 347

flow path was found to be similar, the rheological parameters in the barrel were 348

relatively stable, and the rheological parameters in the nozzle changed significantly. 349

3.8. Effect of nozzle diameter on the parameters in the flow channel 350

The diameter of the nozzle is reported as a critical parameter affecting the 351

printing time and printing precision of the printed object (Vaezi & Chua, 2011), and 352

has a certain influence on the rheological parameters in the flow channel. The nozzle 353

diameter was set as a variable to investigate its effects on the parameters in the flow 354

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channel. Since the inlet volume flow rate was constant, no obvious difference was 355

found in the velocity and shear rate field in the flow channel (Fig. 7a and Fig. 7b). 356

However, a significant change was observed in the pressure field in the flow channel 357

(Fig. 7c). 358

With the nozzle diameter increased from 0.5 mm to 2.0 mm, the pressure at the 359

inlet was greatly reduced from 4.95×107 Pa to 2.50×106 Pa, indicating that the smaller 360

the diameter of the nozzle, the greater the pressure required for extruding the material. 361

Meanwhile, at the axial position of the Y axis, the larger the diameter of nozzles, the 362

greater values of the corresponding Y axis value when the pressure started to change 363

(-24 mm at 0.5 mm and -4 mm at 2.0 mm). It also showed that the smaller nozzle 364

diameter resulting in more high-pressure areas in the flow channel might lead to 365

material storing elastic energy and its release after extrusion causing an extrudate 366

swelling. Therefore, in the process of 3D printing, a suitable nozzle diameter, which 367

can provide a smooth extrusion below the maximum pressure that the equipment can 368

provide, can achieve high precision products. 369

3.9. Simulation of extrudate swell and adjustment of filling ratio 370

The swell effect of the extrudate is that the viscous elastic fluid will be subjected 371

to strong tensile deformation when it passes through the diameter contraction section, 372

and a part of the elastic potential energy is stored. The elastic potential energy of the 373

material will be released completely when the material leaves the nozzle, resulting in 374

a swelling of extrudate. The swell phenomenon of extrusion process is quantitatively 375

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expressed by swell ratio, which is defined as the ratio of material diameter to nozzle 376

diameter after extrusion stabilization. On the basis of the previous model, the 377

simulation of the extrusion molding part is added. The results (Fig. 8A to Fig. 8E) 378

showed that the extrusion part presented a certain level of swelling. Fig. 8A-F showed 379

that the material after the extrusion showed to varying degrees of swelling at different 380

inlet volume flow rates. As the entrance volume flow rate was increased, the extrusion 381

swell ratio tended to decrease first and then increased. This is probably due to the fact 382

that the extrudate swell ratio will be influenced by the speed, shear rate, and pressure 383

at the same time. When the entrance volume flow rate was increased, the pressure in 384

the flow channel also increased, which will lead to the storage of more elastic 385

potential energy by the fluid. On the other hand, the shear rate of materials increased 386

correspondingly with the increase of entrance volume flow rate, the the shear-thinning 387

characteristic of gel resulted in the extrusion swell phenomenon reduced. When the 388

inlet volume flow rate was less than 24 mm3/s, the fluid was greatly affected by the 389

shear rate, which resulted in the extrusion swell ratio decreased with the inlet volume 390

flow rate. In contrast, when the inlet volume flow rate was greater than 24 mm3/s, the 391

fluid viscosity decreased, which was affected by the shear rate and the pressure. 392

Among two factors, the pressure affected more than by the shear rate. This 393

phenomenon resulted in a slight increase in the extrudate swell ratio when the 394

entrance volume flow rate was increased. However, due to the upper limit of the 395

elastic potential energy that the fluid can store, it can be predicted that the extrusion 396

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swell ratio will eventually become flat. Overall, although the extrusion swell ratio 397

fluctuates with the change in the entrance material volume flow rate, the amplitude is 398

not large enough to influence the printing precision at different volume flow rates. 399

From above study on swelling phenomenon, it can be considered that the filling 400

ratio at 100% may not be appropriate in the printing process. When the filling ratio 401

was set at 100%, the material appeared partly bulging due to swelling effect. When 402

the filling ratio was reduced to 90%, the material could be completely and smoothly 403

paved with the whole plane. The results (Fig. 9) showed that the products obtained by 404

a filling ratio of 60%-80% presented obvious pores. Besides, the selected material 405

(lemon-juice gel added with corn starch) was found to have a certain flow capacity, so 406

the low filling ratio might lead to unsupported deformation conditions. Although there 407

might be little difference on the same layer of printed object, but when the number of 408

printing layers increases, the small change of each layer will cause the large 409

cumulative change. Therefore, it is appropriate to choose 90% filling ratio, which is 410

also consistent with the results obtained from the simulation. 411

412

4. Conclusions 413

The material suitable for 3D printing should have a certain range of rheological 414

parameters. Besides, it was found that the material viscosity and relaxation time, the 415

material inlet volume flow rate and the nozzle diameter affected the different 416

parameters in the flow channel in this study. The flow parameters were found stable in 417

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the barrel section but varied greatly in the nozzle section. The velocity and shear 418

velocity fields were determined by the material inlet volume flow rate, and increased 419

with the increase of the volume flow rate. The pressure in the flow channel increased 420

in varying degrees with the increase of the material viscosity and the entrance volume 421

flow rate, and the decrease of relaxation time and the nozzle diameter. The change of 422

nozzle diameter was found to have the greatest influence on the pressure field. In 423

addition, the extruded material exhibited the phenomenon of swell. According to the 424

simulation calculation and the actual test, it was found that in the extrusion-based 3D 425

printing process the filling rate of 90% was suitable because of the swelling effect. 426

Although the parameter values obtained by the simulation have some deviations from 427

the actual values, this work provides a reference value for the optimization of 3D 428

printing food materials and the design of 3D printing extrusion flow channel. 429

430

Acknowledgments 431

The authors acknowledge the financial support from the 432

National Natural Science Foundation Program of China (No. 3187101297), China 433

State Key Laboratory of Food Science and Technology Innovation Project (Contract 434

No. SKLF-ZZA-201706),National First-class Discipline Program of Food Science 435

and Technology (No. JUFSTR20180205), Jiangsu Province Key Laboratory Project of 436

Advanced Food Manufacturing Equipment and Technology (No. FMZ201803), which 437

have enabled us to carry out this study. 438

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439 440

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Figure Captions

Fig. 1 3D model of charging barrel (a-e) and meshing of charging barrel model (f)

Fig. 2 Schematic diagram of the 3D printer setup used in this study (Liu, Bhandari, et

al., 2018).

Fig. 3 NMR signal (T2) (a) and rheological behavior (b. apparent viscosity, c. G’, d.

G” and e. tanδ) of the lemon juice gel added with different starches (□ in Black:

Potato starch; ○ in Red: Corn starch; △ in Blue: Sweet potato starch;

▽ in Pink:

Wheat starch)

Fig. 4 Velocity field (a: Channel section; b: Outlet section), shear rate field (c:

Channel section; d: Outlet section) and pressure field (e) in the channel of

POLYFLOW simulation

Fig. 5 The effect of material viscosity on the parameters (a. Velocity; b. Shear rate; c.

Pressure) in the flow channel based on POLYFLOW simulation (□ in Black:

4000 Pa·s; ○ in Red: 6000 Pa·s; △ in Blue: 8000 Pa·s;

▽ in Pink: 10000 Pa·s;

in Green: 12000 Pa·s) (The axial position of the Y axis (mm) of the barrel is

greater than 0 while the nozzle is less than 0)

Fig. 6 The effect of inlet volume flow rate on the parameters (a. Velocity; b. Shear rate;

c. Pressure) in the flow channel based on POLYFLOW simulation (□ in Black:

20 mm3/s; ○ in Red: 24 mm3/s; △ in Blue: 28 mm3/s) (The axial position of the Y

axis (mm) of the barrel is greater than 0 while the nozzle is less than 0)

Fig. 7 The effect of nozzle diameter on the parameters (a. Velocity; b. Shear rate; c.

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Pressure) in the flow channel based on POLYFLOW simulation (□ in Black: 0.5

mm; ○ in Red: 1.0 mm; △ in Blue: 1.5 mm;

▽ in Pink: 2 mm) (The axial position

of the Y axis (mm) of the barrel is greater than 0 while the nozzle is less than 0)

Fig. 8 Simulation diagram (A: 16 mm3/s, B: 20 mm3/s, C: 24 mm3/s, D: 28 mm3/s,

E:32 mm3/s) and broken line graph (F) of material extrusion swell at different

entrance volume rates

Fig. 9 The effect of filling rate on the quality of 3D printing (A:60%,B:70%,C:

80%,D:90%,E:100%)

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Fig. 1 3D model of charging barrel (a-e) and meshing of charging barrel model (f)

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Fig. 2 schematic diagram of the 3D printer setup used in this study (Liu, Bhandari, et al., 2018).

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a b

0.1 1 10 100 1000 10000-50

0

50

100

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T2(ms)

Rel

ativ

e in

ten

sity

)

0.01 0.1 1 10 100

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cosi

ty (

Pa

·s)

Shear rate (1/s)

c d

0.1 1 10 1000

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2000

3000

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G' (

Pa)

ω (rad/s)

0.1 1 10 1000

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(Pa)

ω (rad/s)

e

0.1 1 10 1000.15

0.20

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0.40

ω (rad/s)

tanδ

Fig. 3 NMR signal (T2) (a) and rheological behavior (b. apparent viscosity, c. G’, d. G” and e. tan δ) of the lemon juice gel added with different starches (□ in Black:

Potato starch; ○ in Red: Corn starch; △ in Blue: Sweet potato starch;

▽ in Pink: Wheat

starch)

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a b

c d

e

Fig. 4 Velocity field (a: Channel section; b: Outlet section), shear rate field (c:

Channel section; d: Outlet section) and pressure field (e) in the channel of

POLYFLOW simulation

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a b

-32 -28 -24 -20 -16 -12 -8 -4 0 4 8 12

0

10

20

30

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Ve

loci

ty (

mm

/s)

Axial position of Y axis (mm) -32 -28 -24 -20 -16 -12 -8 -4 0 4 8 12

0

20

40

60

80

100

120

Sh

ear

rate

(1

/s)

Axial position of Y axis (mm)

c

-32 -28 -24 -20 -16 -12 -8 -4 0 4 8 120

2

4

6

8

10

12

14

16

Pre

ssu

re/1

06 Pa

Axial position of Y axis (mm)

Fig. 5 The effect of material viscosity on the parameters (a. Velocity; b. Shear

rate; c. Pressure) in the flow channel based on POLYFLOW simulation (□ in Black:

4000 Pa·s; ○ in Red: 6000 Pa·s; △ in Blue: 8000 Pa·s;

▽ in Pink: 10000 Pa·s;

◇ in

Green: 12000 Pa·s) (The axial position of the Y axis (mm) of the barrel is greater than

0 while the nozzle is less than 0)

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a b

-32 -28 -24 -20 -16 -12 -8 -4 0 4 8 12

0

10

20

30

40

50

Ve

loci

ty (

mm

/s)

Axial position of Y axis (mm) -32 -28 -24 -20 -16 -12 -8 -4 0 4 8 12

0

20

40

60

80

100

120

140

Sh

ear

rate

(1

/s)

Axial position of Y axis (mm)

c

-32 -28 -24 -20 -16 -12 -8 -4 0 4 8 120

2

4

6

8

10

12

Pre

ssur

e/1

06 Pa

Axial position of Y axis (mm)

Fig. 6 The effect of entrance volume rate on the parameters (a. Velocity; b. Shear

rate; c. Pressure) in the flow channel based on POLYFLOW simulation (□ in Black:

20 mm3/s; ○ in Red: 24 mm3/s; △ in Blue: 28 mm3/s) (The axial position of the Y axis

(mm) of the barrel is greater than 0 while the nozzle is less than 0)

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a b

-36 -32 -28 -24 -20 -16 -12 -8 -4 0 4 8 12-20

0

20

40

60

80

100

120

140

160

180

Ve

loci

ty (

mm

/s)

Axial position of Y axis (mm) -36 -32 -28 -24 -20 -16 -12 -8 -4 0 4 8 12

0

200

400

600

800

1000

She

ar

rate

(1

/s)

Axial position of Y axis (mm)

c

-36 -32 -28 -24 -20 -16 -12 -8 -4 0 4 8 1210-1

100

101

Pre

ssu

re (

MP

a)

Axial position of Y axis (mm)

0.5 mm 1.0 mm 1.5 mm 2.0 mm

Fig. 7 The effect of nozzle diameter on the parameters (a. Velocity; b. Shear rate;

c. Pressure) in the flow channel based on POLYFLOW simulation (□ in Black: 0.5

mm; ○ in Red: 1.0 mm; △ in Blue: 1.5 mm;

▽ in Pink: 2 mm) (The axial position of

the Y axis (mm) of the barrel is greater than 0 while the nozzle is less than 0)

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Fig. 8 Simulation diagram (A: 16 mm3/s, B: 20 mm3/s, C: 24 mm3/s, D: 28

mm3/s, E:32 mm3/s) and broken line graph (F) of material extrusion swell at different

entrance volume rates

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Fig. 9 The effect of filling rate on the quality of 3D printing

(A:60%,B:70%,C:80%,D:90%,E:100%)

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Highlights:

� Moisture properties of lemon juice gels were investigated with different

starches.

� Rheological properties of lemon juice gels were investigated with different

starches.

� Using computer simulation to study the fluid characteristics during 3D

printing.

� Effects of different process parameters on fluid characteristics were

simulated.