Source: UNIVERSITY OF MAINE submitted to NRP
DEVELOPING NANOSTRUCTURED BIOBASED NANOCELLULOSE POLYMER FILMS FOR IMPROVED FOOD PACKAGING
Sponsoring Institution
National Institute of Food and Agriculture
Project Status
COMPLETE
Funding Source
Reporting Frequency
Annual
Accession No.
1015191
Grant No.
2018-67010-27906
Cumulative Award Amt.
$471,661.00
Proposal No.
2017-07826
Multistate No.
(N/A)
Project Start Date
Apr 15, 2018
Project End Date
Apr 14, 2023
Grant Year
2018
Program Code
[A1511]- Agriculture Systems and Technology: Nanotechnology for Agricultural and Food Systems
Recipient Organization
UNIVERSITY OF MAINE
(N/A)
ORONO,ME 04469
Performing Department
Adv Struc & Comp Center
Non Technical Summary
The proposed research will generate adequate data to assess the feasibility of scale-up and demonstration of barrier packaging composites based on cellulose nanomaterials. The composites will comprise a thin layer of biodegradable nanocellulose in the polymers being examined for food packaging to prolong the shelf life of oxygen-sensitive dairy products, dehydrated foods, oily snacks, etc. Nanocellulose can be isolated from cellulose structures naturally occurring in wood cell walls. Occurring in the nano-sized length scale enables nanocellulose to form dense and transparent films with excellent barrier properties to oxygen permeation, however, it is a weak moisture barrier. We propose that the moisture sensitivity of nanocellulose can be improved by several material concepts including the following: developing synergistic means to enhance the barrier properties of nanocellulose films by controlling counterions and functional group charges on the nanocellulose; and screening additives to reinforce nanocellulose films for the improvement of mechanical properties. We will also design and fabricate polymer/nanocellulose multi-layer films with excellent barrier properties. Various processing strategies to manufacture multi-layer films will be explored. In this project, we will test these ideas and optimize processing and treatments to achieve optimum processing efficiency and barrier performance. The project is expected to deliver a body of knowledge of sustainably utilizing nanocellulose for high-performance biobased barrier materials for food packaging.
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
51106502000100%
Goals / Objectives
The long-term goal of the proposed work, led by the University of Maine, with expert contributions from the U.S. Forest Service Forest Products Laboratory (FPL), is to use nanocellulose, a generic name for several types of cellulose nanomaterials isolated from wood cell walls such as cellulose nanocrystals (CNCs) and cellulose nanofibrils (CNFs), as potential transparent barrier components in high-volume packaging materials to extend food shelf-life and quality. Supporting objectives:Develop synergistic means to improve the barrier properties of nanocellulose filmsImprove barrier performance of films through the control of counterions and functional group charges on the nanocelluloseFind additives to reinforce nanocellulose films for the improvement of barrier and mechanical propertiesDesign and fabricate polymer/nanocellulose multilayer films with excellent barrier properties under the guidance of sustainability principlesDesign film structures and select polymers to meet expected barrier specifications and sustainability requirementsDevelop processing strategies to manufacture multi-layer filmsDevelop nanocellulose/chitin nanofibril polyelectrolyte multilayer films using layer-by-layer assembly for the production of compostable barrier films
Project Methods
The project first optimizes the barrier properties of nanocellulose films followed by prototype production of the barrier structures and finally devises strategies for manufacturing the optimized barrier structures on a larger scale. This research will develop synergistic means to improve the barrier properties of nanocellulose films, two of which will be the control of nanocellulose surface functionalities and using additives to reinforce nanocellulose films for improvement of barrier and mechanical properties. Self-standing film fabrication will be developed in the lab. Letter-size self-standing nanocellulose films will be formed based on a coating of gel-type nanocellulose suspensions on a supporting substrate with controlled surface energy. We will design and fabricate multilayer polymer/nanocellulose films to achieve excellent barrier properties. Under the guidance of sustainability principles, we will design film structures and select polymers to meet expected barrier specifications and sustainability requirements. We will identify tie adhesives to render optimum bonding performance between cellulose and polymers cost-effectively.We will also develop processing strategies to manufacture multilayer films. Polymer and adhesive layers will be applied to nanocellulose films through extrusion, dispersion coating, or lamination. Multilayer films will also be formed through nanocellulose dispersion coating on polymer substrates.Processing and products will be characterized by a full suite of analytical instruments to inform the development and optimization. We will measure the values gained from researching, developing, and optimizing the processes and products by translating their mechanical, optical and barrier properties and characteristics to social-economic analysis, which identify the factors that may contribute to, or hinder, adoption of the technology during the course of the project.

Progress 04/15/18 to 04/14/23

Outputs
Target Audience:Forest landowners, pulp mills, paper and paperboard manufacturers and converters, packaging, plastic blenders Plastic packaging causes plastic contamination and pollution. These stakeholders look for alternative biobased packaging materials with compatible performance to plastics. Forest based stakeholders would expand the use of wood, increase the revenue to compensate forest management costs, and reduce fuels and wildfires. Changes/Problems: Nothing Reported What opportunities for training and professional development has the project provided?Cong Chen received a Ph.D. in Bioproducts Engineering from the University of Maine, School of Forest Resources. How have the results been disseminated to communities of interest?Conferences UV-light Protection Cellulose Nanocrystals Films Prepared through Trivalent Metal Ions, Cong Chen, Lu Wang, Jinwu Wang, Douglas Gardner, Proceedings of the 62nd International Convention of Society of Wood Science and Technology October 20-25, 2019 - Tenaya Lodge, Yosemite, California USA Cellulose Nanocrystals vs Cellulose Nanofibrils: Which One Performs Better in Flexible, Biodegradable and Multilayer Films for Food Packaging? Lu Wang, Proceedings of the 62nd International Convention of Society of Wood Science and Technology October 20-25, 2019 - Tenaya Lodge, Yosemite, California USA Barrier Properties of Multilayer Films of CNMs and Polymers Jinwu Wang, U.S. Forest Products Laboratory; Lu Wang, Cong Chen, Douglass Gardner, University of Maine, 2019 International Conference on Nanotechnology for Renewable Materials, Chiba, Japan June 3-7, 2019 Barrier Properties of Multilayer Films of CNMs and polymers - Jinwu Wang, Industrial Liaison Committee Meeting Alliance for Pulp and Paper Technology Innovation and Technical Association of the Pulp and Paper Industry, Madison, Wisconsin 53726, May 21-22, 2019 Cellulose Nanocrystals Coatings on Poly (lactic acid) Film for Food Packaging Applications, Cong Chen, Douglas Gardner, Jinwu Wang, Proceedings of the 64th International Convention of Society of Wood Science and Technology, August 1-6, 2021 - Flagstaff, Arizona, USA Developing Nanostructured Biobased Nanocellulose Polymer Films for Improved Food Packaging, Cong Chen, Lu Wang, Jinwu Wang, Douglass Gardner, Poster of 3 rd GRC Nanoscale Science and Engineering for Agriculture and Food Systems, June 19-24, 2022 - Manchester, New Hampshire, USA What do you plan to do during the next reporting period to accomplish the goals? Nothing Reported

Impacts
What was accomplished under these goals? Food packaging provides means to mitigate food spoilage caused by microbes and environmental exposure, as well as prolonging the shelf life of food products in a cost-effective manner that industry and consumers desire while minimizing environmental impact. However, conventional plastics are unsustainable, nonrenewable, and nondegradable, and coupled with single-use culture can cause serious environmental pollution and the loss of resources. Taking the above issues into consideration, bio-based materials with required properties are desirable to address the end-of-life issues for packaging. Cellulose nanomaterial (CNM) films were prepared by suspension casting. Cellulose nanocrystal (CNC) films were denser (~1.4 g/cm3) than cellulose nanofibril (CNF) films (1.1-1.3 g/cm3). The density of the CNM films increased with the basis weight. The CNC films were optically clearer than the CNF films. Moreover, the CNM films were laminated with polypropylene films (PP) using a polyurethane (PU) adhesive tie layer to form flexible multilayer packaging films with a structure of PP/PU/CNMs/PU/PP. The CNC and CNF laminates containing thicker CNM films had similar maximum tensile strength as control PP/PU laminates. The lamination significantly improved the barrier properties of the resulting laminates as compared with the neat films. For example, the water vapor transmission rate dropped from 540 to 1.0 g/(m2·day) and the oxygen transmission rate at 80% RH decreased from 109 to 5.3 cm3/(m2·day). In addition, laminating PU with CNF films improved the transparency of the CNF films. We have also designed film structures and selected polymers to meet expected barrier specifications and sustainability requirements as well as developed processing strategies to manufacture multilayer films. Cellulose nanomaterials (CNM)films were laminated with polypropylene (PP) film using a polyurethane (PU) adhesive tie layer to form flexible multilayer film packaging. The physical properties of the CNM films indicated that CNC films were denser (1.4 g/cm3) than CNF films (1.1-1.3 g/cm3). Casting weight affected the densities of the CNM films and this effect was material-type dependent. Optical property evaluation showed that the CNC films were clearer than the CNF films. Laminating CNF films with PU improved the transparency of the CNF films. Mechanical test results showed that CNC and CNF laminates containing thicker CNM films had similar maximum tensile strength as the control PP/PU laminates. Laminating CNM films with PP and PU significantly improved the barrier properties of the CNM films. For example, the water vapor transmission rate of CNC film dropped from 516 to 1.0 g/(m2·day). The oxygen transmission rate of CNC film at 80 % RH decreased from 126 to 6.1 cm3/(m2·day). The following four points have been highlighted 1. A CNF film is a better barrier material than a CNC film at 80 % RH, 2. CNMs maintain their high oxygen resistance at 80 % RH after being laminated with PP. 3. Adhesive layers should be used to retain a laminate's performance at 80 % RH. 4. An adhesive layer can increase the transparency of CNF films after lamination The results indicate that lamination structures of cellulose and polymers improve both oxygen and water vapor barrier properties and have potential to be used as barrier packaging materials. Cellulose nanocrystals (CNCs), as a major type of cellulose nanomaterials are directly extracted from renewable biomass resources and have tremendous potential in the packaging field as a natural material. However, CNC films are too brittle to use singly and extremely sensitive to moisture or water, which restricts the practical use of CNCs in food packaging applications. Environmentally friendly CNC films with high performance were fabricated as a promising substitute for plastic food packaging. We thoroughly studied the water vapor sorption behaviors and gas transport of the CNC films. CNC films adsorbed more moisture with increases in relative humidity (RH) and temperature, respectively. The oxygen permeability of CNC films exhibited an exponential increase above 50% RH. We successfully developed transparent CNC films with UV-light absorption, water and oxygen barrier properties, oil resistance, and fire self-extinguishment via trivalent metal ion exchange. We also prepared functional CNC films by incorporating different concentrations of sorbitol, polyvinyl alcohol, carrageenan, chitin nanofibers. The films exhibit good oxygen barrier, mechanical properties, and water durability. Additionally, we manufactured multilayer PLA-CNC-PLA films by mixing CNC suspensions with 15 wt.% polyvinyl alcohol or carrageenan CG coating on PLA substrate, followed by lamination without any petroleum-based tie layer or adhesive addition. These three-layer laminate films exhibited enhanced barrier properties and the PLA film protected the inner CNC film from water and mechanical damage. This research provides practical concepts for commercially eco-friendly, recyclable, high performance food packaging production. Besides the publications listed below, three additional publications will be submitted from Cong Chen's Ph.D. dissertation.

Publications

  • Type: Conference Papers and Presentations Status: Published Year Published: 2021 Citation: Wang, J., Bousfield, D.W., Cai, Z., Gardner, D.J., Hahmann, T., Shaler, S.M., Zwick, K., 2021a. Broadening cellulose-based packaging into plastic packaging markets, in: Proceedings of the 64th International Convention of Society of Wood Science and Technology. Presented at the 64th International Convention of Society of Wood Science and Technology, Little America Hotel, Flagstaff, Arizona, USA, pp. 117123.
  • Type: Journal Articles Status: Published Year Published: 2021 Citation: Wang, J., Wang, L., Gardner, D.J., Shaler, S.M., Cai, Z., 2021b. Towards a cellulose-based society: opportunities and challenges. Cellulose 28, 45114543. https://doi.org/10.1007/s10570-021-03771-4
  • Type: Theses/Dissertations Status: Published Year Published: 2023 Citation: Chen, C. 2023. DEVELOPMENT OF FOOD PACKAGING FILMS BASED ON CELLULOSE NANOCRYSTALS (CNCs), Ph.D. Dissertation, University of Maine, School of Forest Resources (Bioproducts Engineering), 140 p.
  • Type: Journal Articles Status: Published Year Published: 2022 Citation: Chen, C., Sun, W., Wang, L., Tajvidi, M., Wang, J., Gardner, D.J., 2022. Transparent Multifunctional Cellulose Nanocrystal Films Prepared Using Trivalent Metal Ion Exchange for Food Packaging. ACS Sustainable Chemistry & Engineering.
  • Type: Journal Articles Status: Published Year Published: 2021 Citation: Hasan, I., Wang, J., Tajvidi, M., 2021. Tuning physical, mechanical and barrier properties of cellulose nanofibril films through film drying techniques coupled with thermal compression. Cellulose 28, 1134511366.
  • Type: Journal Articles Status: Published Year Published: 2020 Citation: Wang, L., Chen, C., Wang, J., Gardner, D.J., Tajvidi, M., 2020. Cellulose nanofibrils versus cellulose nanocrystals: Comparison of performance in flexible multilayer films for packaging applications. Food Packaging and Shelf Life 23, 100464. https://doi.org/10.1016/j.fpsl.2020.100464
  • Type: Journal Articles Status: Published Year Published: 2022 Citation: Wang, L., Kelly, P.V., Ozveren, N., Zhang, X., Korey, M., Chen, C., Li, K., Bhandari, S., Tekinalp, H., Zhao, X., Wang, J., Seydibeyo?lu, M.�., Alyamac-Seydibeyoglu, E., Gramlich, W.M., Tajvidi, M., Webb, E., Ozcan, S., Gardner, D.J., 2022. Multifunctional polymer composite coatings and adhesives by incorporating cellulose nanomaterials. Matter. https://doi.org/10.1016/j.matt.2022.11.024


Progress 04/15/21 to 04/14/22

Outputs
Target Audience:Researchers in the profession through publication of a paper inACS Sustainable Chemistry & Engineering Changes/Problems:The project is set to finish in April 2023. We plan to complete the research project and the graduate student will prepare a dissertation from the work. It is envisioned that at least 2additional papers will be prepared from the results of the work. What opportunities for training and professional development has the project provided?The graduate student employed on this project completed candidacy requirements for the PhD degree in Forest Resources. How have the results been disseminated to communities of interest?One peer reviewed jounral article and two conference presentations. What do you plan to do during the next reporting period to accomplish the goals?Finding the reinforcement effect on barrier and mechanical properties of CNC films by different additives with various concentrations of the additivesD-sorbitol, PVA, chitin nanofibers, carrageenan.

Impacts
What was accomplished under these goals? During this reporting period, except for barrier properties, the morphology and properties of CNC coating systems and polylactic acid (PLA)/CNC laminated films were fully estimated. For examples, viscosity, surface tension, mechanical properties, morphology of surface and cross section film, etc. PLA film could protect inner fragile CNC layer under force and water destroying. On the other hand, CNC endow great oxygen barrier property to PLA film. The synergetic effort of laminated films showed much more potential for food packaging application. Additionally, the compatibility issue between CNC and PLA film during coating processing could be figured out by adding proper additives, such as poly vinyl alcohol (PVA) or carrageenan. We are analyzing data and preparing an article for a peer reviewed journal. The moisture-related behaviors of CNC films were measured and compared by dynamic vapor sorption (DVS), including adsorption and desorption isotherms, water vapor diffusion coefficients, and water vapor transmission rates, at different relative humidity levels (0-90%) and temperatures (5, 23 and 50 °C). Moreover, the oxygen barrier properties of the CNC films were investigated from 0 to 85% RH. A detailed analysis of water vapor sorption and barrier properties of the CNC films under different conditions will be addressed in this section.

Publications

  • Type: Journal Articles Status: Published Year Published: 2022 Citation: Chen C, Sun W, Wang L, Tajvidi M, Wang J, Gardner D. Transparent Multifunctional Cellulose Nanocrystal Films Prepared using Trivalent Metal Ion Exchange for Food Packaging. 2022. ACS Sustainable Chemistry & Engineering
  • Type: Conference Papers and Presentations Status: Published Year Published: 2021 Citation: Cellulose Nanocrystals Coatings on Poly (lactic acid) Film for Food Packaging Applications, Cong Chen, Douglas Gardner, Jinwu Wang, Proceedings of the 64th International Convention of Society of Wood Science and Technology, August 1-6, 2021  Flagstaff, Arizona, USA
  • Type: Conference Papers and Presentations Status: Published Year Published: 2022 Citation: Developing Nanostructured Biobased Nanocellulose Polymer Films for Improved Food Packaging Cong Chen, Lu Wang, Jinwu Wang, Douglass Gardner, Poster of 3rd GRC Nanoscale Science and Engineering for Agriculture and Food Systems, June 19-24, 2022  Manchester, New Hampshire, USA


Progress 04/15/20 to 04/14/21

Outputs
Target Audience:Researchers in the profession through publication of a paper in Cellulose. Changes/Problems:This project was delayed because of the COVID-19 pandemic. Personnel were kept from working in the lab during the past year for several months thus causing delays. We asked for and we were granted a one year no-cost extension on the project. What opportunities for training and professional development has the project provided?The graduate student employed on this project completed coursework requirements for the PhD degree in Forest Resources. How have the results been disseminated to communities of interest?One jounral article was published earlier this year. What do you plan to do during the next reporting period to accomplish the goals?The project is set to finish in April 2022. We plan to complete the research project and the graduate student will prepare a dissertation from the work. It is envisioned that at least 3 additional papers will be prepared from the results of the work.

Impacts
What was accomplished under these goals? Task 1 Cellulose nanocrystals (CNCs) obtained from sulfuric acid hydrolysis have sulfate half-ester groups on the surface with sodium ions as counterions. In this study, monovalent sodium ions were replaced with ferric and aluminum trivalent ions, which were observed to afford the CNCs in aqueous dispersion loosely agglomerated. Prepared ion-exchanged CNC films had the improved moisture barrier properties, water resistance, UV protection, and fire retardance. It is assumed that trivalent metal ions can cross-link the CNCs via sulfate half-ester groups and this accounts for the improvement. Additionally, ferric ions were demonstrated to improve the oxygen barrier property at high relative humidity (RH). The OTR of the CNC films treated by medium concentration ferric chloride was 41 cm3 m-2 day-1 on average, a significant decrease compared with the Na+-CNC films (88 cm3 m-2 day-1 on average). Task 2 Except for adhering the cast CNCs film to plastic polymer films by tie layer, coating CNCs suspensions on plastic films followed by lamination is another method. However, the compatibility between CNCs and plastic films is the most important issue that needs to be overcome. Based on this point, poly (vinyl alcohol) (PVA) and kappa-carrageenan (K-C) were added into 6% CNC suspensions, respectively, to prepare mixed CNCs composite formulations for PLA coating. Although there was a huge difference of viscosity between PVA and K-C mixed formulations, both of them could significantly improve the coating quality only at 15wt% addition based on the CNCs mass. After drying, another layer of PLA film was laminated onto the CNC coated side to obtain the final sandwich composite structure. All laminated samples showed excellent transparency by 80% transmittance. The laminated PLA/CNC films showed great barrier properties: water vapor transmission rates were around 24 g m-2 d-1 compared with pure CNC films (444 g m-2 d-1), and oxygen transmission rate was 2.26 cm3 m-2 day-1 compared with PLA films (162 cm3 m-2 day-1) at 50% RH and a half lower at 85% RH. Moreover, the laminated films could be separated by soaking in water for several hours, which means they are easy to be recycled after use. This kind of PLA/CNC laminated film has great potential for packaging application.

Publications

  • Type: Journal Articles Status: Published Year Published: 2021 Citation: Wang, J., Wang, L., Gardner, D. J., Shaler, S. M., & Cai, Z. (2021). Towards a cellulose-based society: opportunities and challenges. Cellulose. https://doi.org/10.1007/s10570-021-03771-4.


Progress 04/15/19 to 04/14/20

Outputs
Target Audience:Forest landowners, pulp mills, paper and paperboard manufacturers and converters, packaging producers, plastic blenders. Plastic packaging causes plastic contamination and pollution. These stakeholders look for alternative biobased packaging materials with compatible performance to plastics. Forest-based stakeholders would expand the use of wood, increase the revenue to compensate forest management costs, and reduce fuels and wildfires. Changes/Problems:The COVID-19 issue has impacted the laboratory work for this project. Our lab was closed from mid-March and recently re-opened on a limited basis in mid-June. We are somewhat behind and will be formally asking for a no cost extension on the project. What opportunities for training and professional development has the project provided?A graduate student and postdoctoral research associate have learned biobased barrier packaging materials concerning their requirements, specifications, design, processing, and performance evaluation. How have the results been disseminated to communities of interest?Conferences UV-light Protection Cellulose Nanocrystals Films Prepared through Trivalent Metal Ions, Cong Chen, Lu Wang, Jinwu Wang, Douglas Gardner, Proceedings of the 62nd International Convention of Society of Wood Science and Technology October 20-25, 2019 - Tenaya Lodge, Yosemite, California USA Cellulose Nanocrystals vs Cellulose Nanofibrils: Which One Performs Better in Flexible, Biodegradable and Multilayer Films for Food Packaging? Lu Wang, Proceedings of the 62nd International Convention of Society of Wood Science and Technology October 20-25, 2019 - Tenaya Lodge, Yosemite, California USA Barrier Properties of Multilayer Films of CNMs and Polymers Jinwu Wang, U.S. Forest Products Laboratory; Lu Wang, Cong Chen, Douglass Gardner, University of Maine, 2019 International Conference on Nanotechnology for Renewable Materials, Chiba, Japan June 3-7, 2019 Barrier Properties of Multilayer Films of CNMs and polymers - Jinwu Wang, Industrial Liaison Committee Meeting Alliance for Pulp and Paper Technology Innovation and Technical Association of the Pulp and Paper Industry, Madison, Wisconsin 53726, May 21-22, 2019 What do you plan to do during the next reporting period to accomplish the goals?Continue accomplishing the objectives Develop synergistic means to improve the barrier properties of nanocellulose films o Improve barrier performance of films through the control of counterions and functional group charges on the nanocellulose (80% done) o Find additives to reinforce nanocellulose films for the improvement of barrier and mechanical properties Design and fabricate polymer/nanocellulose multilayer films with excellent barrier properties under the guidance of sustainability principles Design film structures and select polymers to meet expected barrier specifications and sustainability requirements (60% done) Develop processing strategies to manufacture multilayer films (50% done) Develop nanocellulose/chitin nanofibril polyelectrolyte multilayer films using layer-by-layer assembly for the production of compostable barrier films (10% done)

Impacts
What was accomplished under these goals? During this reporting period, we have improved barrier performance of films through the control of counterions and functional group charges on the nanocellulose. To better preserve food from the effects of oxygen, moisture, and (light) UV radiation, typical polymer film packaging is opaque or metallized. There is increasing consumer demand for transparent packaging, or a transparent viewing window to allow viewing of food prior to consumer purchase. Cellulose nanocrystals (CNCs) show great potential for transparent food packaging, and can provide good oxygen permeation resistance, but CNCs are poor in preventing water vapor and UV light transmission. To overcome these disadvantages, CNC dispersions were treated with trivalent metal ions (Al3+, Fe3+) under different concentrations, respectively. It was observed that the trivalent ions rendered CNCs flocculated in the dispersions indicating they might crosslink CNCs through the coordination between them and sulfate half-ester groups of the CNCs. Homogeneous, transparent and flexible CNC films were prepared by solvent casting. CNC films exhibit high UV absorption properties. In addition, the water vapor transmission rate of the cross-linked films was decreased, and the water durability of the films was improved. We have also designed film structures and selected polymers to meet expected barrier specifications and sustainability requirements as well as developed processing strategies to manufacture multilayer films. Cellulose nanomaterials (CNM) films were laminated with polypropylene (PP) film using a polyurethane (PU) adhesive tie layer to form flexible multilayer film packaging. The physical properties of the CNM films indicated that CNC films were denser (∼1.4 g/cm3) than CNF films (1.1-1.3?g/cm3). Casting weight affected the densities of the CNM films and this effect was material-type dependent. Optical property evaluation showed that the CNC films were clearer than the CNF films. Laminating CNF films with PU improved the transparency of the CNF films. Mechanical test results showed that CNC and CNF laminates containing thicker CNM films had similar maximum tensile strength as the control PP/PU laminates. Laminating CNM films with PP and PU significantly improved the barrier properties of the CNM films. For example, the water vapor transmission rate of CNC film dropped from 516 to 1.0 g/(m2·day). The oxygen transmission rate of CNC film at 80 % RH decreased from 126 to 6.1 cm3/(m2·day). The following four points have been highlighted A CNF film is a better barrier material than a CNC film at 80 % RH, CNMs maintain their high oxygen resistance at 80 % RH after being laminated with PP. Adhesive layers should be used to retain a laminate's performance at 80 % RH. An adhesive layer can increase the transparency of CNF films after lamination The results indicate that lamination structures of cellulose and polymers improve both oxygen and water vapor barrier properties and have potential to be used as barrier packaging materials.

Publications

  • Type: Journal Articles Status: Published Year Published: 2020 Citation: Wang L, Chen C, Wang J, et al (2020) Cellulose nanofibrils versus cellulose nanocrystals: Comparison of performance in flexible multilayer films for packaging applications. Food Packaging and Shelf Life 23:100464


Progress 04/15/18 to 04/14/19

Outputs
Target Audience:Entrepreneurs of biobased materials, professionals from the pulp and paper industry and food packaging industry Changes/Problems: Nothing Reported What opportunities for training and professional development has the project provided?A graduate student and postdoctoral research associate have learned biobased barrier packaging materials concerning their requirements, specifications, design, processing, and performance evaluation. 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 complete Task 1.1 Improve barrier performance of films through the control of counterions and functional group charges on the nanocellulose, and Task 1.2 Find additives to reinforce nanocellulose films for the improvement of barrier and mechanical properties.Investigate different clays or polymers to further improve the barrier and mechanical properties of nanocellulose films.Investigate the effects of materials design and processing methods on film structure, morphology, and performance as well as new ways of incorporating cellulose nanomaterials in multilayer packaging, such as spray coating.

Impacts
What was accomplished under these goals? Task 1.1:Improved performance of CNC films through the control of counterions and surface charges of CNC. CNC films were modified with ion-exchanged by H+, Mg2+, Ca2+, Al3+, Fe3+ and their properties were tested. Task 1.2 .The effect of flexibility plasticizer (sorbitol) on CNC film preparation and WVTR was explored. Task 2.1:Designed film structures and select polymers to meet expected barrier specifications. Task 2.2: Develop processing strategies to manufacture multi-layer films. Cellulose nanomaterial (CNM) films were prepared by suspension casting. Cellulose nanocrystal (CNC) films were denser (~1.4 g/cm3) than cellulose nanofibril (CNF) films (1.1-1.3 g/cm3). The density of the CNM films increased with the basis weight. The CNC films were optically clearer than the CNF films. Moreover, the CNM films were laminated with polypropylene films (PP) using a polyurethane (PU) adhesive tie layer to form flexible multilayer packaging films with a structure of PP/PU/CNMs/PU/PP. The CNC and CNF laminates containing thicker CNM films had similar maximum tensile strength as control PP/PU laminates. The lamination significantly improved the barrier properties of the resulting laminates as compared with the neat films. For example, the water vapor transmission rate dropped from 540 to 1.0 g/(m2·day) and the oxygen transmission rate at 80% RH decreased from109 to 5.3 cm3/(m2·day). In addition, laminating PU with CNF films improved the transparency of the CNF films.

Publications