Source: TUSKEGEE UNIVERSITY submitted to
DEVELOPMENT OF SUSTAINABLE FOOD PACKAGING SYSTEMS DERIVED FROM RENEWABLE BIOMASS
Sponsoring Institution
National Institute of Food and Agriculture
Project Status
EXTENDED
Funding Source
Reporting Frequency
Annual
Accession No.
1007644
Grant No.
2015-38821-24376
Project No.
ALX-MIN2015
Proposal No.
2015-05324
Multistate No.
(N/A)
Program Code
EQ
Project Start Date
Sep 1, 2015
Project End Date
Aug 31, 2019
Grant Year
2015
Project Director
Min, B.
Recipient Organization
TUSKEGEE UNIVERSITY
(N/A)
TUSKEGEE,AL 36088
Performing Department
Food and Nutritional Sciences
Non Technical Summary
This research focuses on the sustainable, transformative, and interdisciplinary science and technology demanded from global communities. The ultimate goal in this research is to use a novel sustainable and transformable extraction process, called "melt compounding process", for converting bio-polymeric components derived from biomass wastes of local residual crops to develop value-added food packaging systems equipped with advanced antimicrobial active food packaging technology. Besides, the proposed project will bring in intensive educational opportunities to minority students and rural small business stakeholders through collaboration across the states and institutions. This research includes: Stage-1 Extracting the potentially value-added bio-polymeric components such as cellulose and protein in types of bio-polymeric food packaging materials; Stage-2 Developing the sustainable food packaging systems using functional active ingredients, and its evaluation of mechanical, barrier, and thermal as a novel green packaging material; Stage-3 Developing antimicrobial bio-polymeric packaging films to enhance the safety and quality of food products; and Stage-4: Fostering minority professionals and accelerating creative rural small business in the field of food packaging. The exploration of enhanced bio-polymeric fractions in this research will, in the future, permit new green packaging systems to be developed for a variety of high-demand sustainable packaging products resulting in a reduction in the environmental impact of traditional packaging materials.
Animal Health Component
0%
Research Effort Categories
Basic
20%
Applied
80%
Developmental
(N/A)
Classification

Knowledge Area (KA)Subject of Investigation (SOI)Field of Science (FOS)Percent
5011499202070%
7124099110030%
Goals / Objectives
The goal of this study is to develop sustainable packaging systems using low profitable biomass wastes from residual crops and to enhance food safety and quality of food products by bio-polymeric films incorporated with natural antimicrobials. An ancillary goal is to train minority professionals in sustainable food packaging field. The specific objectives of the proposed research are:1) To extract the potentially value-added bio-polymeric components such as cellulose and protein in types of bioplastic.2) To develop the sustainable food packaging systems using extracted fractions, and its evaluation of mechanical, barrier, and thermal as a novel green packaging material.3) To develop multiple applications of new packaging films with selected natural antimicrobials for securing safety and quality of agricultural food products.4) To foster minority professionals in sustainable food packaging systems through collaborative team works among investigators and institutions.
Project Methods
The potentially high end value products such as cellulose, protein, and other bio-polymeric components will be extracted or fractionized from agricultural wastes including food wastes through "melt compounding processing technology". Key aspects of this technology is to use common tools to heat and shear the biomass on a continuous basis with an extruder. For characterization of "green" packaging material, the structural, mechanical, barrier, and thermal properties will be performed according to official testing methods such as the American Society of Testing and Materials Standards. A set of film fabrication processes such as casting, pouring, or extruding will be adapted to generate "products" for testing, and it will be functionalized using various active natural antimicrobial agents and its dynamic diffusion behavior. Fostering minority students and transferring technology to society will be closely performed through multidimensional collaborations across the colleges, universities, and states.

Progress 09/01/17 to 08/31/18

Outputs
Target Audience:The 3rd year of the project was designed to drive time and efforts to develop potential packaging applications using extracted nanocellulose. It also includes the further characterization and evaluation of fabricated nanocellulose packaging film using an analytical instrument. Upon discussion with the PI and the other project partner, BCI, the Virginia Tech research team determined that the properties of nano-cellulose gel/solution can be improved by chemical and physical treatments for packaging application, then the advanced processing technologies, such as high turbulent flow homogenization process and TEMPO oxidation process, were applied. In total ten undergraduate students were hired and trained for continuing the project. Two graduate students were involved in this project. This project provided an opportunity to collaborate with inter and intra department investigators at Tuskegee University as well as collaboration with Virginia Tech, which foster the undergraduate and graduate student to obtain the knowledge and skills on multidisciplinary subjects focused on bio-based materials. This collaboration not only benefits the student involved in the project but also corroborates to accomplish our targeted goals. Team work and collaboration on campus also help to disseminate our unique project goals and findings in the university community. Our research findings from the application study have been presented at the International conference. Changes/Problems:The extension of the project (12months) is applied. What opportunities for training and professional development has the project provided? Nothing Reported How have the results been disseminated to communities of interest?To disseminate our research findings, we presented to regional, national and international audiences and communities through various scientific and professional meetings such as Professional Agricultural Workers Conference (PAWC), annual meeting of the American Society of Microbiology (ASM) and the Annual meeting of the Institute of Food Technologist (IFT), USDA-ARS Food Safety Consortium Meeting, respectively. Also, research progress and highlights were presented at the USDA project director meeting in Washington DC in July 2018. What do you plan to do during the next reporting period to accomplish the goals?During the next year, research will be more focused on the development of bio-plastic packaging composite films in real food systems to extend the shelf-life. Also, research will be carried out in antimicrobial activities against a wide range of foodborne microorganisms. Further research will also be exploring in the applications of bio-polymer in different areas such as water filter and purification and smart packaging. Research findings will be disseminated through publications and conference presentations. Further study will also be carried out to quantify the total hemicellulose and lignin loss during the treatment process. Collaboration with other investigators and institutions will be further explored in the upcoming year to support and strengthen our research. A research experience and training opportunity of a graduate student will be performed at the other university/institution to explore the potential application of our extracted lignocellulosic components and professional development of the student. Therefore, collaboration in a potential area of further application with other University/Institution will be determined after the discussion with PI, Co-PI, and other partners.

Impacts
What was accomplished under these goals? During the 3rd year project, one graduate student received an M.S. Degree and one undergraduate student was hired by a packaging company. In total, ten undergraduate students were hired and involved in the research work of the project. The third year of the project was designed mainly to further explore the application of nanocellulose derived from potential biomasses as value-added products by using further optimization of various methods such as chemical, thermal, and TEMPO oxidation. Characterized nanocelluloses were used as a matrix to develop composites hybridized/incorporated with graphene oxide (GO) or other green polymers such as chitosan, poly lactic acid (PLA) and antimicrobial agents. During the project period, we formulated the sol-gel and filaments extrusion procedure by dissolution of cellulose incorporated with silver nanoparticles onto the matrix of polymer, and antimicrobial bio-polymer composite films and filaments hybridized with synthesized silver nanoparticles were developed. Newly fabricated films and filaments exhibited the antimicrobial activities against tested organisms both in solid and liquid culture medium. The characterization of developed materials was further confirmed by various analytic equipment such as XRD, Raman, TGA, TMA, FTIR and SEM. Further studies were carried out to determine the physical, thermal, barrier, and mechanical properties of the extracted nano-celluloses from biomass. Significant research progress & accomplishment highlights include the following: Optimization of isolation and separation procedures of lignocellulosic components: It was determined the weight percentage of each lignocellulosic component (hemicellulose, lignin, and cellulose) in each of the stages of treatment by a fiber analyzer using neutral and acid detergent fiber solutions. Weight percentage of hemicellulose (32.5%), lignin (15.5%) and cellulose (44.9%) from sugarcane bagasse were recovered in each stages of treatment. Extracted cellulose was further disintegrated into nano cellulose by using previously standardized ultrasonic methods. Chemical, thermal, and physical properties of the isolated nanocellulose by FTIR, TGA, Raman and SEM were also determined. Further study was also carried out to applied extracted cellulose as a composite material by incorporating it with other polymers to develop bio-plastic packaging film. Isolated nanocellulose fibrils were used as a composite material to develop the bio-plastic films. Tensile testing showed good mechanical strength which was increased by 20% elongation as compared to control films (PLA film). It also improved water vapor permeability (WVP) when isolated nanocellulose is incorporated with other polymers; however, increment in the percentage of nanocellulose in the films decreased the WVP. Preparation of active nano-ingredient using graphene oxide (GO) and chemical modification of nanocellulose using 2,2,6,6-tetramethylpiperidine-1-oxyl (TEMPO) oxidation: Preparation of nano-ingredient using GO: A modified Hummers method was used to prepare exfoliated graphene oxide from graphite. Ten grams of graphite powder was added to 250 mL of sulfuric acid in a flask at room temperature. The mixture was placed in an ice bath and followed by the addition of potassium permanganate, which was then allowed to react at 35°C for 12 h. The solution was cooled to < 5 °C in an ice bath again. Excess hydrogen peroxide was gradually added to the flask with stirring to reduce unreacted potassium permanganate. Once the mixture turned bright yellow and bubbles were observed, it was washed repeatedly with distilled water until a pH of 7 was achieved. The resulting mixture was transferred to a conical centrifuge tube and centrifuged until no more supernatant was observed. Lastly, liquid nitrogen was utilized to freeze the neutralized graphene oxide, which was subsequently obtained in powder form via freeze drying. The exfoliated graphene oxide was characterized by XRD. Chemical modification of nanocellulose using TEMPO oxidation: Twenty grams of cellulose was suspended in distilled water (2 L) using a domestic blender. 0.25 g of TEMPO and 2.5 g of sodium bromide (1X TEMPO) were added to a three-neck round bottom flask, and the mixture was agitated with an overhead stirrer at 300 rpm. Then, 46 mL of 13% sodium hypochlorite was gradually added to the cellulose slurry with a syringe pump at a rate of 1500 μL/min at room temperature. The pH of the solution was maintained to be 10±2 by the drop-wise addition of 0.5N sodium hydroxide. The oxidized cellulose was washed thoroughly with distilled water by centrifugation at 5000 rpm for 30 minutes at 0-5°C. This process was repeated several times until the pH of the cellulose sediment after the washes was adjusted to 7. The oxidized cellulose was stored at 4°C for further treatment. The TEMPO- oxidized cellulose nanocomposites prepared at different oxidation levels (0.5X, 1X, and 2X TEMPO) without GO were denoted as 0.5X, 1X, and 2X TOCN, respectively. Production of TOCN/GO nanocomposites: TEMPO-oxidized cellulose was mixed with graphene oxide (GO) with a high-pressure laboratory homogenizer. The TOCN/GO solution of the different concentrations were continuously agitated and homogenized. The TEMPO-oxidized cellulose nanocomposites (TOCN) were prepared with the addition of various graphene oxide percent loadings: 0.4, 1.2, and 2.0 wt % with respect to dried cellulose. The water content of the TEMPO-GO dispersions was evaluated in a moisture analyzer. Nanocomposite films were then cast from the cellulose/GO suspensions on a petri dish at 50% RH and room temperature. Further characterization of TOCN/GO nanocomposites: Fourier transform infrared spectroscopy (FT-IR): All chemical modification was confirmed by FT-IR and the spectrum clearly showed the successful surface modification; X-Ray Diffraction analysis: The level of crystallinity was evaluated by XRD test. It was confirmed that the crystallinity of cellulose was not affected due to the surface medication of nanocellulose. Dynamic mechanical analysis (DMA): Storage modulus and loss modulus was significantly affected by the level of surface modification and degree of active carbon material incorporation. Morphological analysis: The field emission scanning electron microscopy (FESEM) was carried out on a LEO (Zeiss) 1550 operated with an acceleration voltage of 2 kV. The cross-section of the sample was obtained by fracturing it in liquid nitrogen to assess the cross-sectional morphology. The TOCN/GO nanocomposite films were coated by sputtering with a thin layer of iridium. We were able to observe the well distribution of carbon-nano material into the matrix of nano-cellulose film. Oxygen permeation analysis: At 0.2% carbon material loading and 2X TEMPO treatment, oxygen barrier property was significantly improved.

Publications

  • Type: Conference Papers and Presentations Status: Published Year Published: 2017 Citation: Naresh Shahi, Byungjin Min, Desmond Mortley and Vijaya Rangari. Screening and Characterization of Nano-cellulose Isolated from Different Biomass. Professional Agriculture Workers Conference, Tuskegee, AL.
  • Type: Other Status: Published Year Published: 2018 Citation: Naresh Shahi and Byungjin Min. Characterization of Synthesized Nanocomposites Derived From Agricultural Biomass. The Second 1890 ARD & USDA-ARS Food Safety consortium Symposium, Beltsville, MD.
  • Type: Conference Papers and Presentations Status: Published Year Published: 2018 Citation: Naresh Shahi, Byungjin Min. Potential Antimicrobial Application of Silver Nanoparticles in Biopolymer Matrix. The Annual Meeting of American Society of Microbiology, Atlanta, GA
  • Type: Conference Papers and Presentations Status: Published Year Published: 2018 Citation: Naresh Shahi, Byungjin Min, Young Kim. Biopolymeric Nanocomposite Films Hybridized With Antimicrobials. The Annual Meeting of Institute of Food Technologist, Chicago, IL
  • Type: Journal Articles Status: Submitted Year Published: 2018 Citation: Yoojin Kim, Young Kim, Byungjin Min. TEMPO-oxidized Nanofibrillated Cellulose Film (NFC) incorporating Graphene Oxide (GO) Nanofillers, International Journal of biological macromolecules.
  • Type: Other Status: Other Year Published: 2018 Citation: Development of sustainable food packaging materials derived from renewable biomass. USDA/NIFA PI meeting, Washington DC


Progress 09/01/16 to 08/31/17

Outputs
Target Audience:The project at 2nd year was designed to drive continued efforts to screen out potential biomass for extraction of cellulose using melt compounding technology and to improve the process efficiency and explore to potential application in packaging system. Upon close discussion with the Tuskegee University research team, Virginia Tech research team and other project partner, BCI, we have selected agricultural wastes from Stevia and Sugarcane Bagasse due to the high demand from local industries and the significant potential of high value cellulose extraction. Also, nano-cellulose gel, which is commercially available and made from University of Maine, was used to compare the properties in analytic studies and to initiate application study as a control. Our research findings from the application study has been presented at the 2017 Annual ACS conference during April and August. Two Virginia Tech undergraduate students per semester have been hired and trained for continuation of the project. The new students have finished all safety training programs offered by Virginia Tech and have focused on doing project using biomass wastes. Changes/Problems: Nothing Reported What opportunities for training and professional development has the project provided?Two undergraduates successfully graduated during the second year period and two new undergraduates were hired for this project. All of them finished safety training programs and learned about lab protocols and experiment. How have the results been disseminated to communities of interest? Nothing Reported What do you plan to do during the next reporting period to accomplish the goals?Next year research will be more focused on the development of bio-plastic packaging films. Characterization of cellulose solution and films incorporated with antimicrobials will be determined using a variety of testing methods. It includes rheological behavior test, morphological changes, antimicrobial efficiency test, and other physical properties for applications in packaging system. We will also have diversified the application of nanocellulose in multi-disciplinary area such as in biomedicine as an antimicrobial wound gauges or other environmental testing kids such as rapid detection of water contamination etc. Application of cellulose in other area will be determined after the discussion with PI, Co-PI's and other partners. We did not determine the percentage of total hemicellulose loss and structural carbohydrate in each stages of the treatment procedures. Further optimization of the procedure will be carried out in the next year of the project. Also, further research is necessary to standardized and scale up the production of bio-plastic packaging films. A research experience and professional training of graduate students from Tuskegee University will be performed in the laboratory in the Department of sustainable biomaterials at Virginia Tech during the next year of project period. ?

Impacts
What was accomplished under these goals? During the 2nd year of research project period, Naresh Shahi (Graduate Student in Integrated Bioscience Ph.D. program at Tuskegee University) mainly worked on developing novel process to reduce or minimize harmful chemical use in multiple steps for cellulose extraction from biomass, and extracted cellulose was tested on their thermal and mechanical properties. The status of a former MS degree student on this project, Yoojin Kim (MS, Macromolecules Innovation Institute, Virginia Tech) was switched into the Ph.D degree program as of May 01, 2017. Based on her experience and skill in chemistry and macromolecules, she is currently focusing on the application of cellulose based packaging system in this project.Two former undergraduate researchers, Jacob Steven (Sustainable Biomaterials), Loc Pham (Sustainable Biomaterials) graduated at Dec.2016 and May 2017, respectively. Two new undergraduate students, Collin McGuire (Sophomore, Sustainable Biomaterials), Miguel Comparativo (Senior, Sustainable Biomaterials) were hired as of May 20, 2017. They both have finished laboratory training programs and have continued this project with Co-PI Dr. Kim. During this project period, we formulated the novel technique to isolate cellulose from biomass and optimized parameters for high purity and efficient isolation. We determined thermal, physical and mechanical properties of the isolated cellulose. Further study was also carried out to applied extracted cellulose as a composite material by incorporating with other polymers to develop active bio-plastic packaging film. Furthermore, our research findings during this project period, and abstracts were accepted to the national meeting of academic society such as American Chemical Society (ACS). To successfully accomplish objectives 1 and 2, sugarcane bagasse biomass wastes provided from Co-PI of Dr. Desmond Mortley (Plant Science at Tuskegee University) and stevia biomass wastes provided from US-Stevia (North Carolina) through collaboration with BCI were used to optimize the process during the project period. Significant research progress and accomplishment highlights include the followings: · Lab scale processing of Stevia stem and leaves in preparation for Glycerol Thermal Processing (GTP) using melt compounding process · CW Brabender Conical Twin Screw extruder (BCI) was used for continuous processing of stevia stem and leaves or mixtures · Change the critical treatment processes for GTP and improve the evaluation methods. · Based on our evaluation, there were around 90% of cellulose contents with minor impurities (lignin or other hemicellulose) · Production yield of preliminary lab scale process was around 33% comparing to the cellulose contents (45%) found at literature · Upon alpha cellulose content evaluation, stevia stem shows around 60% out of the crude cellulose fraction. · Lab scale extraction and purification of cellulose from sugarcane bagasse is developed. · Conditions for optimizing of extraction and purification of cellulose is formulated. · Lignin amount in crude sample of sugarcane bagasse was significantly reduced in purified sample. · Ultrasonic treatment was applied to avoid acid treatment and to apply less chemical treatment compared to traditional methods · Evaluation of alpha cellulose content of sugarcane bagasse is ongoing. Highlights of preliminary application study using commercially available nanocellulose as follows: Commercially available nano-cellulose gel was purchased from University of Maine as control and it was used for preliminary experiment for application in packaging system. To produce high end products in packaging, our team focused on surface modification with leveraged technology in our lab and fabricated nano-cellullose based composite film using carbon ased nano-material which was also leveraged in our previous projects. To achieve further individualization of cellulose nanofibrils, a promising chemical disintegration method called 2,2,6,6-tetramethylpiperidine-1-oxyl (TEMPO), was used. It is regioselective oxidation by converting primary alcohols to aldehydes and carboxylate groups. The surface modified cellulose becomes disintegrated by applying negative electrostatic repulsions and the cohesiveness of the fibrils with the introduction of appreciable amounts of carboxylate moieties. To improve typical properties of cellulose based film such as modulus, gas barrier properties and mechanical strengths, we explored to composite system with graphene oxide. It consists of carbon atoms in a 2-dimentional Honey-comb structure with oxygen-containing functionalities, such as hydroxyl, carboxyl, carboxyl, and epoxide. The sp2-hybridized carbon network exhibits excellent mechanical, thermal, optical, and electrical properties. Based on our preliminary experiments in this project period, cellulose based films reinforced by TEMPO treatment and carbon-based nanomaterial shows significant improvement in many properties such as storage modulus, tensile strength, and oxygen barrier properties. As a function of degree of oxidation by TEMPO treatment, 0.5X treatment showed highest young's modulus and tensile strength comparing to all other treatments including control. The highest tensile strength was observed at 1.2% of graphene oxide concentration while Young's modulus gradually increased from 0 % to 2.0%. Water barrier properties were not affected by both degree of oxidation and graphene oxide concertation. It resulted from the basic mechanism of water vapor transmission which is predominantly affected by the chemical composition of cellulose. During 2nd year of research project period, highly purified cellulose was extracted from stevia biomass wastes and sugarcane bagasse. Our team proved the potential of cellulose based compsite films for high end applications.

Publications

  • Type: Conference Papers and Presentations Status: Published Year Published: 2017 Citation: Yoojin Kim, Young Kim, Katia Rodriguez and Byungjin Min. 2017. TEMPO-oxidized Nanofibrillated Cellulose Film (NFC) incorporating Graphene Oxide (GO) Nanofillers. Annual Meeting of American Chemical Society (ACS) Conference, Poster presentation, San Francisco, California
  • Type: Conference Papers and Presentations Status: Published Year Published: 2017 Citation: Naresh Shahi, Byungjin Min, Desmond Mortley and Vijaya Rangari. 2017. Isolation and characterization of cellulose from biomass: applications in biomedical and food packaging. Annual Meeting of American Chemical Society (ACS) Conference, Oral and Poster presentation, Washington DC.
  • Type: Book Chapters Status: Published Year Published: 2017 Citation: Laszlo Horvath, Byungjin Min and Young Kim. 2017. Testing of Mechanical Properties for Plastic Packaging Materials: in Food Packaging Materials Testing and Quality Assurance by Preeti Singh et al. CRC press.
  • Type: Other Status: Other Year Published: 2017 Citation: Biopolymer and natural antimicrobials for novel food packaging applications. 2017. Guest Speaker in seminar class of Animal Science, Auburn University, AL.


Progress 09/01/15 to 08/31/16

Outputs
Target Audience:The 1st year of the project was designed to recruit undergraduate and graduate level research personnel to screen out potential biomass for extractable cellulose using melt compounding technology. During the first year of the project, the principal investigator at Tuskegee University has closely communicated with the Virginia Tech research team and other poroject partner, BCI, to select a few potentially useful biomassess. The target audience includes different agricultural industries that can provide biomass wastes, such as brewery spent grain (called BSG) from the industry, stevia stem from a stevia manufacturer and a few local farmers for peanut hulls, hemp stem and other agricultural biomass. Changes/Problems:We have found that many processing variations need to be optimized for better efficiency. During the 2nd year of the project, those processing parameters will be fine-tuned. What opportunities for training and professional development has the project provided? Nothing Reported How have the results been disseminated to communities of interest? Nothing Reported What do you plan to do during the next reporting period to accomplish the goals?To improve the production efficiency and quality of the cellulose product, we are planning to further screen out high cellulose contents biomass. During the 2nd yr. period, we will investigate a few different biomasses such as hemp stem and stevia stem and leaves because those are also very common agricultural wastes and those contain higher than 40% cellulose in biomass. Peanut hull or shell will be explored through collaboration with PI. During the next reporting period, both the Tuskegee University and the Virginia Tech research team will collaboratively work on two main objectives: Objective 2) to develop the sustainable food packaging systems using extracted fractions, and its evaluation of mechanical, barrier, and thermal as a novel green packaging material and objective 3) to develop multiple applications of new packaging films with selected natural antimicrobials for securing the safety and quality of agricultural food products.

Impacts
(N/A)

Publications