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New Generation of Functional Cellulose Fibre Based Packaging Materials for Sustainability

Final Report Summary - NEWGENPAK (New Generation of Functional Cellulose Fibre Based Packaging Materials for Sustainability)

NEW GENERATION OF FUNCTIONAL CELLULOSE FIBRE BASED PACKAGING MATERIALS FOR SUSTAINABILITY.

PITN-2011-GA-290098

www.NewGenPak.eu

CONTACT: Professor Chris Breen, Materials and Engineering Research Institute, Sheffield Hallam University, City Campus, Sheffield S1 1WB, United Kingdom. c.breen@shu.ac.uk

SUMMARY OF PROJECT OBJECTIVES

The NewGenPak ITN, which commenced in December 2011, established a multi-site network of ten early stage researchers (ESRs) and three experienced researchers (ERs) at ten partner institutions including three enterprises. The principle objective of NewGenPak was to deliver a joint multidisciplinary training programme designed to develop the researchers’ skills in scientific expertise, technological knowledge and professional aptitude. The key vehicle in this strategy was a supervised personal, original research project in a critical aspect of sustainable packaging for each of the 13 researchers.
The key scientific objectives of NewGenPak were:
(i) to conduct top-level research and devise innovative solutions for sustainable packaging,
(ii) to advance the state-of-the-art in sustainable packaging in three specific areas
(a) next generation packaging composites,
(b) cellulose-fibre based active packaging and
(c) environmental, economic and societal aspects of packaging production.
The key strategic aim was to further strengthen the long-term sustainable packaging research and training base in the EU.

WORK PERFORMED AND MAIN SCIENTIFIC RESULTS ACHIEVED

The ESR at Karlstad University in Sweden has demonstrated that rheological measurements of the structure in a suspension provides detailed information about the structure of particles in the resulting dry composite layer; confirming rheology as a useful tool to control the pigment/filler structure in coatings. It was shown that unmodified starch can be used to form the basis of an environmentally-friendly, responsive system which can be used to optimize coating processes because the viscosity, and other parameters, that determine the flow properties can be readily controlled by temperature.

The ESR at Sheffield Hallam University in the UK has developed structurally realistic, fully-atomistic models of montmorillonite (MMT) which, even though they only represent 2 nm x 2 nm, exhibited excellent agreement with the properties exhibited by real macroscopic samples. The ability of these simulations to distinguish between the same atom in different molecules provided key insights into the distribution of both starch and plasticiser molecules in MMT. This approach provided critical information concerning the interlayer composition that cannot be obtained experimentally.

The ESR at Denmark Technical University successfully extracted acetylated cellulose nanofibres (CNF) from sisal using a combination of easy-to-upscale alkali-acetylation treatments. The reinforcement of polylactic acid (PLA) with these fibres led to enhanced barrier and thermomechanical properties compared to PLA-nanoclay (Cloisite™ 30B). The combined addition of 5% of CNF and 5% of C30B reduced the
oxygen/water transmission rates by 90% and 76%, respectively. Careful control of the PLA crystallinity (using nanofillers/crystallisation procedures) prolonged the release of carvacrol from the composites.

The ESR at the University of Bologna in Italy analysed the water vapour solubility and diffusivity in carboxymethylated and enzymatically pre-treated microfibrillar cellulose (MFC) films over a wide range of experimental conditions. A water solubility increase with temperature was observed together with non Fickian diffusion behaviour at high temperature and high Relative Humidity (RH). Fully biodegradable PLA-MFC multilayer films were produced that reduced the oxygen permeability by a factor of 100 in dry conditions and maintained sufficient barrier properties up to 60% RH.

The ER working in UK industry studied the use of kaolin and synthetic binders to provide a barrier to mineral oils. New specifications for gravure cylinders (which allowed significantly higher coat weights to be delivered) were produced but process variables could not be optimised and the coatings require further development to outperform currently available solutions.

The ESR at INP Grenoble in France has demonstrated that cellulose nanofibers (CNF) can be grafted in water. Treatment with aminosilane enables CNF to mimic the antimicrobial properties of chitosan. Grafting CNF with cyclodextrins prolonged the release of active species, while Nisin-grafted CNF has shown promise for food packaging. Contact active materials produced by grafting benzylpenicillin onto CNF, show no leaching of penicillin and are active even when formulated in an industrial overprint varnish; extremely promising for medical packaging designed to prevent the spread of infection associated with multiple users accessing the same package.

The ESR at INNOVHUB-SSi in Milan explored the use of tittanium dioxide nanoparticles (NPs) as photoactive antibacterial agents on hydrophilic cellulose fibres and demonstrated that they were very effective against gram-positive and gram negative bacteria. Zinc oxide NPs were incorporated in a commercial overprint varnish and successfully applied on an industrial printing line during production of the NewGenPak demonstrator, SAFEBOX. Polyphenols extracted from waste tea, using water, proved completely effective against S. Aureus after seven hours contact. The polyphenols were added into standard formulations and coated onto paper.

The ESR working at ZUT in Poland confirmed that both Cinnamon oil and Argy wormwood oil exhibited a high, wide-spectrum antimicrobial activity and could be formulated into pre-emulsions. The stability and durability of the cinnamon oil based pre-emulsion can be further improved by the addition of typical triacylglycerols resulting in shelf lives of over ten weeks. Acceptable levels of antimicrobial activity were obtained when the appropriate modified coating formulation was identified.

The ESR at ITENE in Valencia, Spain, produced CNF grafted with increasing amounts of 3- aminopropyltriethoxysilane (g-CNF) and studied the redispersion of spray-dried samples in water. The extrusion of g-CNF into PLA led to modest improvements in elongation at break, Young's modulus and oxygen barrier. Single and multilayer coatings of PLA/g-CNF/natamycin clearly reduced the microbial growth of Penicillium roqueforti. CNF, modified using solvent free thiol-ene 'click' chemistry, exhibited useful activity against S. Aureus and E Coli.

The first ER at BUMAGA in The Netherlands completed a desk study of commercial thermochromic inks for printed intelligence elements for fruit and vegetable packaging before testing their printability on unmodified substrates. The second ER developed a lab-scale, biodegradable, three-layer packaging system in which paper is coated with poly(vinyl alcohol), PVOH, and polyhydroxyalkanoate, PHA. The resulting material exhibits a much improved barrier to water and oxygen compared to paper or PHA alone. A more bio-based and sustainable system in which PVOH was replaced by nanocrystalline cellulose was also evaluated.

The second ESR at ITENE in Valencia focussed on life cycle analysis (LCA) to establish the benefits of using essential oils in packaging to prolong the shelf life of packed beef, and as a tool to determine that a combination of silver and titanium dioxide NPs provided the best solution for active packaging using NPs. Subsequently, paper coated with a zinc oxide-PLA nanocomposite was produced and demonstrated good antimicrobial activity. This material's recyclability was assessed and the fate of the NPs was tracked.

THE SAFEBOX DEMONSTRATOR
Design Futures, at Sheffield Hallam University, provided the artwork for the NewGenPak demonstrator package which was produced in March 2015 at a partner's industrial printing line in Northern Ireland.

ITN TRAINING ACTIVITIES
All the recruited researchers developed and regularly updated their Personal Career Development Plans, which together with the seven mandatory NewGenPak workshops, and other formal courses, formed the backbone of the training and development which underpinned their personal project work. The workshops, held at 6-monthly intervals at different partner institutions, also included mandatory complementary training designed to develop and expand the researchers' transferable skills.

DISSEMINATION
The researchers have published six papers in international, peer-reviewed journals, there are two accepted and a further seven in review. Furthermore, there are another twenty-one manuscripts in preparation and these will be submitted by December 2016. Nine researchers will submit for a PhD with two already awarded, and one under review. The remaining six theses will be submitted during 2016. In addition to this permanent record of NewGenPak's output the researchers have presented a total of 58 oral contributions and 21 posters at regional, national and international meetings. Finally, nine ESRs and seven senior scientists described the results achieved and explained their wider relevance at the NewGenPak International Seminar held In Valencia in June 2015.

OUTREACH
Over 760 school students attended 26 events in five separate countries and 840 university students attended 11 events in seven different countries including India.
Five of the NewGenPak researchers contributed directly to the success of the project's stand at the EXPLORE Event held during the Sheffield Festival of Science and Engineering in March 2015 which was attended by almost 250 members of the general public.
115 members of the general public attended the Comieco Seminar in Milan where Joana Mendes, ESR at INNOVHUB-SSi in Milan, presented. The other two key elements of dissemination have been the NewGenPak external website (www.NewGenPak.eu) and the preparation and production of the NewGenPak Newsletters (July 2013 and Spring 2014).

WIDER RELEVANCE OF THE NEWGENPAK PROJECT.
NewGenPak addressed some of the key challenges, identified in EU strategy, including reduced energy consumption, sustainable consumption and production, as well as the conservation and management of natural resources. NewGenPak focused on the innovative development of barrier and active technologies so that the amount of wood pulp, paper and forest derived products used in the packaging chain can be increased. Cellulose fibre-based materials originate from the forest and are extensively reused through advanced materials recirculation methods so they are essentially CO2 neutral. This is very different to the large carbon footprint associated with petroleum-derived materials. Nonetheless, any packaging which helps to ensure that the enormous amount of embodied energy in food is not lost clearly represents a substantial and welcome benefit.

DELIVERABLES AND MILESTONES
All the deliverables and milestones of the project were achieved.