Title: Minimizing Oxygen Permeability in Chitin/Cellulose Nanomaterial Coatings by Tuning Chitin Deacetylation

Journal Article · · ACS Sustainable Chemistry & Engineering

The demand for packaging materials with low gas permeabilities is increasing, but commonly used petroleum-derived single-use plastics are not renewable, biodegradable, or easy to recycle. Nanomaterials composed of chitin and cellulose, which are abundant in nature, have high crystallinities and low oxygen permeabilities (OP), providing a viable alternative. In this work, we explore how deacetylation conditions of crab shell chitin can be used to tune the charge and size of resulting chitin nanowhiskers (ChNWs) and the resulting OP of layered film structures. Three deacetylation factors, the concentration of sodium hydroxide (%NaOH), temperature (T), and reaction time, were explored using a three-factor three-level Taguchi design with an orthogonal array. Furthermore, the resulting ChNW suspensions were sequentially spray-coated with suspensions of cellulose nanocrystals (CNCs) onto cellulose acetate (CA) films to form a multilayer structure. We show that ChNWs prepared under more aggressive deacetylation conditions inside the original orthogonal array (higher %NaOH, T, and time) had shorter lengths but the surface charge was significantly influenced only by more aggressive deacetylation outside of the original design conditions. With only ~10% decrease in the ultimate tensile strength and no significant loss in failure strain, the ChNW-CNC coating resulted in ~20% decrease in WVTR in comparison to uncoated CA films. The optimization of process conditions resulted in CA-ChNW-CNC films with a 91-99% decrease in OP (132-16.7 cm3∙μm/m2/day/kPa versus 1553 cm3∙μm/m2/day/kPa for uncoated CA).

Research Organization:
Georgia Tech Research Corporation, Atlanta, GA (United States)
Sponsoring Organization:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Transportation Office. Bioenergy Technologies Office
Grant/Contract Number:
AC36-08GO28308; EE0008494
OSTI ID:
1901790
Journal Information:
ACS Sustainable Chemistry & Engineering, Journal Name: ACS Sustainable Chemistry & Engineering Journal Issue: 1 Vol. 10; ISSN 2168-0485
Publisher:
American Chemical Society (ACS)Copyright Statement
Country of Publication:
United States
Language:
English

References (57)

Lateral thermal expansion of chitin crystals journal January 2000
The effect of reaction time and temperature during heterogenous alkali deacetylation on degree of deacetylation and molecular weight of resulting chitosan journal June 2003
Surface texture and barrier performance of poly(lactic acid)-cellulose nanocrystal extruded-cast films journal February 2019
Recent innovations in barrier technologies for plastic packaging?a review journal January 2003
SEM imaging of chiral nematic films cast from cellulose nanocrystal suspensions journal June 2012
Multi-functional coating of cellulose nanocrystals for flexible packaging applications journal August 2013
Highly transparent 100% cellulose nanofibril films with extremely high oxygen barriers in high relative humidity journal May 2018
Preparation of Cationic/Anionic Chitin Nanofiber Composite Materials journal April 2018
Preparation and application of chitin and its derivatives: a review journal February 2014
Chitin- and cellulose-based sustainable barrier materials: a review journal December 2020
Residual stresses and cracking in brittle solids bonded with a thin ductile layer journal August 1988
Oxygen and aroma barrier properties of edible films: A review journal July 1997
The crustacean exoskeleton as an example of a structurally and mechanically graded biological nanocomposite material journal September 2005
Individual chitin nano-whiskers prepared from partially deacetylated α-chitin by fibril surface cationization journal March 2010
Influence of TEMPO-oxidized cellulose nanofibril length on film properties journal March 2013
Microfibrillated cellulose – Its barrier properties and applications in cellulosic materials: A review journal October 2012
Tunable green oxygen barrier through layer-by-layer self-assembly of chitosan and cellulose nanocrystals journal February 2013
Nanocrystalline chitin thin films journal February 2014
Developing chitin nanocrystals for flexible packaging coatings journal December 2019
Biorenewable, transparent, and oxygen/moisture barrier nanocellulose/nanochitin-based coating on polypropylene for food packaging applications journal November 2021
Determination of the degree of deacetylation of chitin and chitosan by X-ray powder diffraction journal August 2005
The production of fully deacetylated chitosan by compression method journal March 2016
Permeability of polymer/clay nanocomposites: A review journal April 2009
Poly(lactic) acid (PLA) and starch bilayer films, containing cinnamaldehyde, obtained by compression moulding journal October 2017
Comparison of process technologies for chitosan production from shrimp shell waste: A techno-economic approach using Aspen Plus ® journal May 2017
Comparative characterization of aqueous dispersions and cast films of different chitin nanowhiskers/nanofibers journal January 2012
DLS and zeta potential – What they are and what they are not? journal August 2016
Thermal and Oxygen Barrier Properties of Chitosan Bionanocomposites by Reinforcement of Calcium Carbonate Nanopowder journal August 2014
Bio-nanocomposites for food packaging applications journal October 2013
Polymer film packaging for food: An environmental assessment journal September 2013
A comprehensive review on natural bioactive films with controlled release characteristics and their applications in foods and pharmaceuticals journal June 2021
Controlling Barrier and Mechanical Properties of Cellulose Nanocrystals by Blending with Chitin Nanofibers journal November 2019
High-Strength Nanostructured Films Based on Well-Preserved α-Chitin Nanofibrils Disintegrated from Insect Cuticles journal November 2019
Cellulose Nanocrystal (CNC) Coatings with Controlled Anisotropy as High-Performance Gas Barrier Films journal December 2018
Crab-on-a-Tree: All Biorenewable, Optical and Radio Frequency Transparent Barrier Nanocoating for Food Packaging journal March 2019
Moisture and Oxygen Barrier Properties of Cellulose Nanomaterial-Based Films journal November 2017
Spray-Coated Multilayer Cellulose Nanocrystal—Chitin Nanofiber Films for Barrier Applications journal July 2018
Optimization of Chitin Extraction from Shrimp Shells journal January 2003
Chitin Whiskers: An Overview journal December 2011
Facile Route to Produce Chitin Nanofibers as Precursors for Flexible and Transparent Gas Barrier Materials journal November 2014
Sustainability: Don't waste seafood waste journal August 2015
Relationship between aspect ratio and suspension viscosity of wood cellulose nanofibers journal July 2013
High strength films with gas-barrier fabricated from chitin solution dissolved at low temperature journal January 2013
Sustainable, self-cleaning, transparent, and moisture/oxygen-barrier coating films for food packaging journal January 2021
Cellulose nanomaterials review: structure, properties and nanocomposites journal January 2011
Chitin nanofibers: preparations, modifications, and applications journal January 2012
The hydrolysis of cellulose and its relation to structure journal January 1957
High-throughput mechanical characterization of free-standing polymer films journal June 2005
An Overview of Taguchi Method and Newly Developed Statistical Methods for Robust Design journal November 1992
Optimization of chitin extraction procedure from shrimp waste using Taguchi method and chitosan characterization journal December 2019
Accumulation and fragmentation of plastic debris in global environments
  • Barnes, David K. A.; Galgani, Francois; Thompson, Richard C.
  • Philosophical Transactions of the Royal Society B: Biological Sciences, Vol. 364, Issue 1526 https://doi.org/10.1098/rstb.2008.0205
journal July 2009
Plastics recycling: challenges and opportunities journal July 2009
Recent Advances on Edible Films Based on Fruits and Vegetables-A Review: Fruit and vegetable edible films… journal July 2017
A review of high performance polymer nanocomposites for packaging applications in electronics and food industries journal May 2019
Polymers book October 2008
Optimization of shrimp shell waste deacetylation for chitosan production journal October 2016
Chitin and Chitosan Preparation from Marine Sources. Structure, Properties and Applications journal March 2015