Source: UNIVERSITY OF MISSOURI submitted to NRP
EXPLORING THE MECHANISMS AND APPLICATIONS OF 4D FOOD PRINTING
Sponsoring Institution
National Institute of Food and Agriculture
Project Status
COMPLETE
Funding Source
AFRI COMPETITIVE GRANT
Reporting Frequency
Annual
Accession No.
1021187
Grant No.
2020-67030-31336
Cumulative Award Amt.
$200,000.00
Proposal No.
2018-09318
Multistate No.
(N/A)
Project Start Date
May 1, 2020
Project End Date
Apr 30, 2024
Grant Year
2020
Program Code
[A1801]- Exploratory: Exploratory Research
Recipient Organization
UNIVERSITY OF MISSOURI
(N/A)
COLUMBIA,MO 65211
Performing Department
Food Science
Non Technical Summary
3D printing has gained huge interests recently in the food industry. However, 3D printed objects are static and their shapes or properties do not evolve over time. Recently, 4D printing has emerged to print objects with functions of dynamic shape changes, which is becoming a new frontier for innovation. This project aimsto explore the mechanisms and applications of 4D food printing by developing novel printable and programmable precursors using responsive biopolymers. The outcomes of this project will open new possibilities in the food industry ranging from flat packaging, customized and enriched foods, and interactive foods that can provide unique dining experience.
Animal Health Component
50%
Research Effort Categories
Basic
50%
Applied
50%
Developmental
(N/A)
Classification

Knowledge Area (KA)Subject of Investigation (SOI)Field of Science (FOS)Percent
50150102000100%
Knowledge Area
501 - New and Improved Food Processing Technologies;

Subject Of Investigation
5010 - Food;

Field Of Science
2000 - Chemistry;
Goals / Objectives
The overall goal of this project is to explore the mechanisms and applications of 4D food printing by developing novel printable and programmable precursors using responsive biopolymers. Particular stimuli, such as heat or water, will be applied to activate shape transformation in a fully controllable manner.
Project Methods
Methods are:(i) investigate the feasibility of using various responsive biopolymers in 4D printing, develop and evaluate different food formulations based on their printability; (ii) assess the effects of intrinsic and extrinsic factors/stimuli on the rheological properties of printed foods and the use of precursors in the 4D food printing process; (iii) incorporate selected precursors in 4D food printing and create novel printed foods with time-resolved shapes and geometries; conduct sensory analysis of printed foods.

Progress 05/01/20 to 02/07/24

Outputs
Target Audience:Target audiences were food scientists, students, professionals from academia, the food industry, and government agencies. Changes/Problems: Nothing Reported What opportunities for training and professional development has the project provided?This project provided training for two doctoral students and two master's students. How have the results been disseminated to communities of interest?The results of this project have been disseminated in peer-reviewed journals, at the professional conferences including International Food Technologists (IFT) and American Chemical Society (ACS) conference. What do you plan to do during the next reporting period to accomplish the goals?N/A. This is a final report.

Impacts
What was accomplished under these goals? During the reporting period, experiments were carried out to investigate the 4D printing of dysphagia foods using pea proteins and purple sweet potato.Dysphagia, the difficulty in swallowing, is a prevalent issue among elderly people, causing various health problems. Thus, the development of visually attractive, nutritious, and soft-textured foods is crucial. While 3D printing offers shape customization, it falls short offully satisfying the visual needs of dysphagia patients.This study used highly nutritious purple sweet potatoes (PSP) flour, pea proteins (PP), and hydroxypropyl methylcellulose(HPMC) for 4D printing of dysphagia foods. As a result, ink formulations combining 17% PSP, 4% PP, and 0.2% HPMC were selected,demonstrating superior 3D printing capabilities.Rheological analysis showcased pseudoplastic behavior and elastic structures crucial for printing and shape retention.Texture profile analysis and fork pressure, spoon tilt tests revealed balanced attributes with hardness of 74.16 g, cohesiveness of 42.75%, adhesiveness of -178.29 g.s, and gumminess of 31.70 g, which are suitable for dysphagia diets.Additionally, by leveraging the color-changing properties of anthocyaninsin PSP flour in response to acidic and alkaline environments, this study unlocked the potential of 4D printing to provide dynamic color-changing, high-protein, and engaging gastronomic experiences for individuals with dysphagia. In another study, ethyl cellulose (EC) was utilized in the osmotically-driven and anisotropically-actuated 4D printing of edible food composites. This study used EC as a shape-constraining and color-transforming material in 4D printing as exposed to external stimuli. Edible composites containing EC and gelatin were formed and submerged in water, resulting in osmotically-driven structural changes of the composites. The rheological properties, printing patterns, and the effects of constraint sites (EC) on the shape-morphing behaviors of composites were investigated. The composites' aspect ratio, film thickness, and swelling properties were quantified to investigate their shape-morphing properties. The results demonstrate that the printing patterns affected the symmetric/asymmetric deformation of the composites. Photomicrographs indicate that the color of EC strips turned from transparent to white due to self-assembly, which is related to the curing time. The swelling index and capacity values ranged between 127.55 - 471.43% and 219.58 - 700%. This study provides insight into the mechanism of 4D printing using edible materials to fabricate complex food structures with tunable properties.

Publications

  • Type: Journal Articles Status: Submitted Year Published: 2024 Citation: Su, C., Wu, Y., Vardhanabhuti, B., Lin, M. 2024. 4D Printing of dysphagia foods using pea proteins and purple sweet potato. Food Hydrocolloids. Submitted.
  • Type: Journal Articles Status: Published Year Published: 2024 Citation: Search, J., Mahjoubnia, A., Chen, A.C., Deng, H., Tan, A.J., Chen, S.-Y., Lin, J. 2023. 3D-printing of selectively porous, freestanding structures via humidity-induced rapid phase change. Additive Manufacturing, 68, 103514.
  • Type: Journal Articles Status: Published Year Published: 2022 Citation: Pulatsu, E., Su, J.-W., Lin, J., Lin, M. 2022. Utilization of ethyl cellulose in the osmotically-driven and anisotropically-actuated 4D printing concept of edible food composites. Carbohydrate Polymer Technology and Applications, 3, 100183.
  • Type: Journal Articles Status: Published Year Published: 2022 Citation: Pulatsu, E., Su, J.-W., Kenderes, S.M., Lin, J., Vardhanabhuti, B., Lin, M. 2022. Restructuring cookie dough with 3D printing: Relationships between the mechanical properties, baking conditions, and structural changes. Journal of Food Engineering, 319, 110911.
  • Type: Journal Articles Status: Published Year Published: 2022 Citation: Cheng, Z., Qu, M., Fu, X., Lin, J. 2022. Review on microscale sensors with 3D engineered structures: Fabrication and applications. Small Methods, 6(4), 2101384.
  • Type: Book Chapters Status: Published Year Published: 2022 Citation: Deng, H., Lin, J. 2022. 4D Printing: 3D Printing of responsive and programmable materials. 3D bioprinting and nanotechnology in tissue engineering and regenerative medicine. Pg 213-217.
  • Type: Journal Articles Status: Published Year Published: 2021 Citation: Su, J.-W., Li, D., Xie Y., Zhou, T., Zhang, C., Deng, H., Zhang, C., Xin, M., Lin, J. 2021. A machine learning workflow for 4D Printing: Predict and understand morphing behaviors of printed active structures. Smart Materials and Structures, 30, 015028.
  • Type: Journal Articles Status: Published Year Published: 2021 Citation: Zhang, C., Cai, D., Liao, P., et al. 2021. 4D printing of shape-memory polymeric scaffolds for adaptive biomedical implantation. Acta Biomaterialia. 122, 101-110.
  • Type: Journal Articles Status: Published Year Published: 2021 Citation: Pulatsu, E., Lin, M. 2021. A review on customizing edible food materials into 3D printable inks: Approaches and strategies. Trends in Food Science and Technology. 107, 68-77.
  • Type: Journal Articles Status: Published Year Published: 2021 Citation: Sattari, K., Xie, Y., Lin, J. 2021. Data-driven algorithms for inverse design of polymers. Soft Matter. 17, 7607.
  • Type: Journal Articles Status: Published Year Published: 2022 Citation: Wu, Y., Advincula, P.A., Giraldo-Londono, O., Yu, Y., Xie, Y., Chen, Z., Huang, G., Tour, J.M., Lin, J. 2022. Sustainable 3D printing of recyclable biocomposite empowered by flash graphene. ACS Nano, 16(10), 17326-17335.
  • Type: Journal Articles Status: Published Year Published: 2021 Citation: Pulatsu, E., Su, J.-W., Kenderes, S.M., Lin, J., Vardhanabhuti, B., Lin, M. 2021. Effects of ingredients and pre-heating on the printing quality and dimensional stability in 3D printing of cookie dough. Journal of Food Engineering. 294, 110412.
  • Type: Conference Papers and Presentations Status: Published Year Published: 2021 Citation: Pulatsu, E., Lin, M. Synergistic effect of oil type and self-assembled structures on the shape stability of 3D-printed cookies. 2021 ACS Meeting. April 5-9, 2021.
  • Type: Theses/Dissertations Status: Published Year Published: 2021 Citation: Type: Theses/Dissertations Status: Published Year Published: 2021 Citation: Pulatsu, E. (2021) Enhancing efficacy, performance, and applicability of additive food manufacturing (PhD Dissertation).


Progress 05/01/22 to 04/30/23

Outputs
Target Audience:Target audiences were food scientists, students, professionals from academia, the food industry, and government agencies. Changes/Problems: Nothing Reported What opportunities for training and professional development has the project provided?This project provided training for two doctoral students and one master's student.? How have the results been disseminated to communities of interest?The results of this project have been disseminated in peer-reviewed journals, at the professional conferences including International Food Technologists (IFT) and American Chemical Society (ACS) conference. What do you plan to do during the next reporting period to accomplish the goals?In the final reporting period, we will incorporate selected precursors in 4D food printing and create novel printed foods with time-resolved shapes and geometries; conduct sensory analysis of printed foods, summarize and analyze the data, and publish more articles.

Impacts
What was accomplished under these goals? During the reporting period, experiments were carried out to investigate the four-dimensional (4D) printing of starch-based food products with microwave heating-induced shape changes. Three-dimensional (3D) food printing technology is emerging as a novel technology and 4D food printing is an extension of 3D printing. It takes advantage of 3D printing but has unique characteristics such as designing moving structures, changing sensory properties, and flat packaging. This study aimed to determine the effects of microwave heating on the shape deformation of 3D-printed food samples. Different concentrations of potato starch gels were prepared to be printed by a 3D printer, and microwave heating was used to induce the physiochemical changes of printed samples with different treatment durations. The rheological properties of each concentration of potato starch were measured to investigate the 3D printing behaviors of the samples. In the printing process, a thin layer of potato starch gel was deposited onto parchment papers. After microwave treatments, the moisture loss and the degree of shape deformation of the printed sample were measured to determine specific time points. Various concentrations (5, 7.5, and 10%) of potato starch gels were used for printing. Samples of 7.5% and 10% concentrations had lower moisture losses compared to that of 5% due to higher solid components after microwave treatment. Furthermore, after 6 min of microwave treatment, the moisture loss of both samples of 7.5% and 10% concentrations were not significantly different. The degree of deformation had increased at 4 min of microwave treatment among three concentrations of the samples, but after 4 min, the degrees of deformation were not significant. During microwave treatment, the shape of the printed sample was deformed by migrating its moisture from the center to the side. The moisture content and the degree of deformation of printed samples were controlled by the duration of microwave treatment. The moisture content and shape deformation are related to each other under microwave treatment. The duration of microwave heating, the degree of shape deformation, the percent of moisture loss of printed samples, and the composition of printing samples played significant roles in the 4D printing of starch-based foods. This study established a protocol on the appropriate microwave treating time to have programmed appearances of printed foods for consumers. In another study, we utilized ethyl cellulose (EC) in the osmotically-driven and anisotropically-actuated 4D printing of edible food composites. This study used EC as a shape-constraining and color-transforming material in 4DP as exposed to external stimuli. Edible composites containing EC and gelatin were formed and submerged in water, resulting in osmotically-driven structural changes of the composites. The rheological properties, printing patterns, and the effects of constraint sites (EC) on the shape-morphing behaviors of composites were investigated. The composites' aspect ratio, film thickness, and swelling properties were quantified to investigate their shape-morphing properties. The results demonstrate that the printing patterns affected the symmetric/asymmetric deformation of the composites. Photomicrographs indicate that the color of EC strips turned from transparent to white due to self-assembly, which is related to the curing time. The swelling index and capacity values ranged between 127.55 - 471.43% and 219.58 - 700%. This study provides insight into the mechanism of 4DP using edible materials to fabricate complex food structures with tunable properties.

Publications

  • Type: Journal Articles Status: Published Year Published: 2022 Citation: Pulatsu, E., Su, J.-W., Lin, J., Lin, M. 2022. Utilization of ethyl cellulose in the osmotically-driven and anisotropically-actuated 4D printing concept of edible food composites. Carbohydrate Polymer Technology and Applications 3, 100183.
  • Type: Journal Articles Status: Published Year Published: 2022 Citation: Pulatsu, E., Su, J.-W., Kenderes, S.M., Lin, J., Vardhanabhuti, B., Lin, M. 2022. Restructuring cookie dough with 3D printing: Relationships between the mechanical properties, baking conditions, and structural changes. Journal of Food Engineering. 319, 110911.
  • Type: Journal Articles Status: Published Year Published: 2022 Citation: Wu, Y., Advincula, P.A., Giraldo-Londono, O., Yu, Y., Xie, Y., Chen, Z., Huang, G., Tour, J.M., Lin, J. 2022. Sustainable 3D printing of recyclable biocomposite empowered by flash graphene. ACS Nano. 16(10), 17326-17335.
  • Type: Journal Articles Status: Published Year Published: 2022 Citation: Cheng, Z., Qu, M., Fu, X., Lin, J. 2022. Review on Microscale Sensors with 3D Engineered Structures: Fabrication and Applications. Small Methods, 6(4), 2101384.
  • Type: Journal Articles Status: Published Year Published: 2022 Citation: Deng, H., Lin, J. 2022. 4D Printing: 3D Printing of Responsive and Programmable Materials. 3D Bioprinting and Nanotechnology in Tissue Engineering and Regenerative Medicine. Pg 213-217.


Progress 05/01/21 to 04/30/22

Outputs
Target Audience:Target audiences were food scientists, students, professionals from academia, the food industry, and government agencies. Changes/Problems: Nothing Reported What opportunities for training and professional development has the project provided?This project provided training for two doctoral students and one Master's student. How have the results been disseminated to communities of interest?The results of this project have been disseminated in peer-reviewed journals, at the professional conferences including American Chemical Society (ACS) conference. What do you plan to do during the next reporting period to accomplish the goals?In the next reporting period, we will continue to summarize and analyze the data, and publish more articles; use various responsive biopolymers in 4D printing; test different food formulations based on their printability; assess the effects of various factorson the rheological properties of printed foods and the use of precursors in 4D food printing process.

Impacts
What was accomplished under these goals? During the reporting period, experiments were carried out to utilize ethyl cellulose in the osmotically-driven and anisotropically-actuated 4D printing concept of edible food composites. We used ethyl cellulose (EC) as a shape-constraining and color-transforming material in four-dimensional printing (4DP) as exposed to external stimuli. Edible composites containing EC and gelatin were formed and submerged into water, resulting in osmotically-driven structural changes of the composites. The rheological properties, printing patterns, and the effects of constraint sites (EC) on shape-morphing behaviors of composites were investigated. The composites' aspect ratio, film thickness, and swelling properties were quantified to investigate their shape-morphing properties. The gelatin films and EC solution were prepared. The pure gelatin solution was cast into Petri dishes (8 cm diameter). Different volumes (10, 20, 30, and 40 mL) of solutions were poured and settled for about 20 min. After that, samples were placed in a fume hood and air-dried for at least 20 h. The same procedure was employed for the solutions containing glycerol as a plasticizer. EC (30 g) was dissolved in 100 mL of 95% ethanol solution to obtain 30% (w/v) at 50ºC. The solution was rested for 30 min before printing. A modified 3D printer with a digital air syringe dispenser was used. The nozzle (20-gauge, pink) diameter and printing pressure were 0.6 mm and 8-10 psi. The patterns and corresponding g-codes were created. A composite structure was obtained by printing EC patterns on gelatin substrates at room temperature. A texture analyzer equipped with a 50-kg load cell was used to determine the mechanical properties of the selected gelatin films. The flow behaviors of the printing materials were analyzed by a rheometer. The cross-sections of 3D-printed EC strips before and after water immersion films were acquired by a Quanta 600 FEG environmental SEM. The curvatures of selected transformed structures, defined as the reciprocal of the radius of a circle, were measured via IC Measure. The results demonstrate that the printing patterns affected the symmetric/asymmetric deformation of the composites. Photomicrographs indicate that the color of EC strips turned from transparent to white due to self-assembly, which is related to the curing time. The swelling index and capacity values ranged between 127.55 - 471.43% and 219.58 - 700%. This study provides insight into the mechanism of 4DP using edible materials to fabricate complex food structures with tunable properties.

Publications

  • Type: Journal Articles Status: Published Year Published: 2021 Citation: Su, J.-W., Li, D., Xie Y., Zhou, T., et al. 2021. A machine learning workflow for 4D Printing: Predict and understand morphing behaviors of printed active structures. Smart Materials and Structures, 30, 015028.
  • Type: Journal Articles Status: Published Year Published: 2021 Citation: Zhang, C., Cai, D., Liao, P., et al. 2021. 4D printing of shape-memory polymeric scaffolds for adaptive biomedical implantation. Acta Biomaterialia. 122, 101-110.
  • Type: Journal Articles Status: Published Year Published: 2021 Citation: Pulatsu, E., Lin, M. 2021. A review on customizing edible food materials into 3D printable inks: Approaches and strategies. Trends in Food Science and Technology. 107, 68-77.
  • Type: Journal Articles Status: Published Year Published: 2021 Citation: Sattari, K., Xie, Y., Lin, J. 2021. Data-driven algorithms for inverse design of polymers. Soft Matter. 17, 7607.
  • Type: Journal Articles Status: Published Year Published: 2021 Citation: Pulatsu, E., Su, J.-W., Kenderes, S.M., Lin, J., Vardhanabhuti, B., Lin, M. 2021. Effects of ingredients and pre-heating on the printing quality and dimensional stability in 3D printing of cookie dough. Journal of Food Engineering. 294, 110412.
  • Type: Conference Papers and Presentations Status: Published Year Published: 2021 Citation: Pulatsu, E., Lin, M. Synergistic effect of oil type and self-assembled structures on the shape stability of 3D-printed cookies. 2021 ACS Meeting. April 5-9, 2021.


Progress 05/01/20 to 04/30/21

Outputs
Target Audience:Target audiences were food scientists, students, professionals from academia, the food industry, and government agencies. Changes/Problems: Nothing Reported What opportunities for training and professional development has the project provided?This project provided training for two doctoral students and one Master's student. How have the results been disseminated to communities of interest?The results of this project have been disseminated in peer-reviewed journals, at the professional conferences including American Chemical Society (ACS) conference. What do you plan to do during the next reporting period to accomplish the goals?In the next reporting period, we will continue to investigate the feasibility of using various responsive biopolymers in 4D printing; evaluate different food formulations based on their printability; assess the effects of intrisic and extrisic factorson the rheological properties of printed foods and the use of precursors in 4D food printing process; and incorporate selected precursors in 4D food printing and create novel printed foods with time-resolved shapes and geometries.

Impacts
What was accomplished under these goals? During the reporting period, experiments were carried out to investigate the structural evolution of composite films containing gelatin and ethyl cellulose, which were subjected to water as a stimulus to trigger the shape transformation of the structures.Four-dimensional (4D) printing involves the shape transformation over time after deposition of the printing ink when subjected to external stimuli. More recently, it is redefined as the programmed evolution of the 3D-printed structure regarding shape, property, and functionality. The 4D printing has been recognized well in the area of material engineering and soft robotics. However, the adaptation of this novel technology in food application needs substantial work due to inherited material properties of foods, such as less responsiveness, irreversibility, and limited deformation capacity. In this study, the structural evolution of film composites based on gelatin and ethyl cellulose when subjected to water as a stimulus was explored to unravel the shape transformation basics. In addition, the effect of glycerol on the response capacity was also investigated. Below is a detailed report about the progress of 4D food printing studies and findings regarding the fabrication and use of composite films. Preparation of precursors and printing inks: Anappropriate amount of type B gelatin was dissolved in MiliQ water and cast in Petri dishes in varying amounts (10 - 60 mL) that were air-dried from 20 hours to 2 days, depending on the poured quantity. The prepared concentrations of gelatin were 5, 7, and 10% (w/v), and glycerol containing gelatin films (5 to 25 g / 100 g gelatin) were also prepared based on a similar procedure. A 30% (w/v) ethyl cellulose solution was prepared by dissolving an appropriate amount of ethyl cellulose powder in the ethanol solvent at 300 rpm for 30 min (50oC). The ethyl cellulose solution was then printed on dried gelatin films before water immersion to observe shape transformation.CAD models and 3D printing studies:Different printing patterns (parallel, angled strips, and more complex shapes like a flower) were drawn in a CAD program to be printed using an extrusion-based 3D printer with different nozzle sizes. Printing precision, material characterization, and swelling capacity under water immersion were studied. The effect of printing pattern and aspect ratio on the shape transformation were investigated.Statistical analysis:Minitab was used to perform one-way analysis of variance (ANOVA) and Tukey's tests (for the numerical findings) (P≤ 0.05) in which aP-value of ≤ 0.05 indicates a significant difference in the data. The established anisotropy in composite structures enabled shape-changing due to mismatching in their water-absorption behaviors. Printing patterns were shown to be effective ways of controlling shape-morphing behaviors. Printing precision studies indicated that the nozzle size is critical for obtaining the designed shape where 0.6 mm diameter resulted in a good match. Among three pure gelatin film concentrations, 10% (w/v) exhibited the most absorptive behavior due to the water-binding capacity of gelatin molecules. The addition of glycerol mitigated the absorption capacity of the film composites, although glycerol addition aided smooth and flat surface that is critical for 3D printing studies. The thickness of the films affected the shape-changing capacity of the film composites, which can be attributed to the swelling capacity of the films. The aspect ratio had a significant effect on the composite films in obtaining full curvature. The relationship was established between the film thickness, aspect ratio, and bending capacity for the geometrically-constrained composite films.

Publications

  • Type: Journal Articles Status: Published Year Published: 2021 Citation: Su, J.-W., Li, D., Xie Y., Zhou, T., Zhang, C., Deng, H., Zhang, C., Xin, M., Lin, J. 2021. A machine learning workflow for 4D Printing: Predict and understand morphing behaviors of printed active structures. Smart Materials and Structures, 30, 015028.
  • Type: Journal Articles Status: Published Year Published: 2021 Citation: Pulatsu, E., Lin, M. 2021. A review on customizing edible food materials into 3D printable inks: Approaches and strategies. Trends in Food Science and Technology. 107, 68-77.
  • Type: Journal Articles Status: Published Year Published: 2021 Citation: Pulatsu, E., Su, J.-W., Kenderes, S.M., Lin, J., Vardhanabhuti, B., Lin, M. 2021. Effects of ingredients and pre-heating on the printing quality and dimensional stability in 3D printing of cookie dough. Journal of Food Engineering. 294, 110412.
  • Type: Journal Articles Status: Published Year Published: 2020 Citation: Pulatsu, E., Su, J.-W., Lin, J., Lin, M. 2020. Factors affecting 3D printing and post-processing capacity of cookie dough. Innovative Food Science and Emerging Technologies, 61, 102316.
  • Type: Journal Articles Status: Published Year Published: 2020 Citation: Deng, H., Xu, X., Zhang, C., Su, J.-W., Huang, G., Lin, J. 2020. Deterministic self-morphing of soft-stiff hybridized polymeric films for acoustic metamaterials. ACS Applied Materials & Interfaces, 12, 13378-13385.
  • Type: Journal Articles Status: Published Year Published: 2020 Citation: Deng, H., Sattari, K., Xie, Y., Liao, P., Yan, Z., Lin, J. 2020. Laser reprogramming magnetic anisotropy in soft composites for reconfigurable 3D shaping. Nature Communications, 11, 6325.