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Los últimos años han sido testigos de una tremenda expansión de los desarrollos de
investigación y tecnología en el campo de la nanotecnología, lo que ha resultado en
desarrollos significativos de aplicaciones en las áreas de alimentos y agricultura. Este es
particularmente el caso del campo del envasado de alimentos, donde los avances significativos
en la nanoreformación de materiales de origen biológico proporcionan un terreno más sólido
para aumentar la competitividad técnica y económica de los polímeros renovables para
diferentes aplicaciones. Sin embargo, aún queda un largo camino por recorrer, no solo en el
desarrollo de materiales y paquetes de minimización del consumo de energía, sino también en
la comercialización generalizada de estos nuevos biopolímeros nanoestructurados y la
caracterización completa de cualquier posible impacto toxicológico y ambiental. En este papel,
Introducción
En las últimas décadas ha habido un aumento significativo en la cantidad de plásticos que se
utilizan en diversos sectores, particularmente en aplicaciones de envasado de alimentos. De
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hecho, la mayor aplicación para plásticos en la actualidad es el envasado, y dentro del nicho
de envasado, el envasado de alimentos es la mayor aplicación de plásticos exigentes (
Lagaron & López-Rubio, 2010).) Esto es así, porque los plásticos aportan enormes ventajas,
como termoestabilidad, flexibilidad en propiedades térmicas y mecánicas, permiten procesos
integrados (es decir, pueden formarse, envasarse y sellarse los paquetes de plástico dentro de
la línea de producción), ligereza y bajo precio . Sin embargo, los polímeros también tienen una
serie de limitaciones para ciertas aplicaciones en comparación con materiales más
tradicionales como metales y aleaciones o cerámica. La principal limitación es su
permeabilidad inherente al transporte de componentes de bajo peso molecular que conduce a
problemas como la oxidación de alimentos por la penetración de oxígeno, la migración de
elementos tóxicos del plástico y el reventado de componentes alimenticios en el envase con
las consiguientes pérdidas en la calidad alimentaria y atributos de seguridad. Entre estos, la
migración potencial más allá de los límites legales de los constituyentes de polímeros y
aditivos es tal vez el problema más ampliamente reconocido con respecto a la seguridad de los
alimentos envasados. A pesar de esto, los materiales plásticos continúan expandiéndose y
reemplazando el uso convencional de cartón, latas de acero estañado y vidrio que, en el caso
de los dos últimos materiales, se han usado típicamente como sistemas monocapa en
aplicaciones alimentarias. Inicialmente, la mayoría de los embalajes de plástico estaban
hechos de materiales semirrígidos o flexibles monocapa, pero a medida que las ventajas de
los envases de plástico se establecían y desarrollaban, los requisitos cada vez más exigentes
de los productos alimentarios, junto con los avances significativos en formulaciones de
envases poliméricos más complejas. Esto dio como resultado estructuras multicomponente
complejas, tales como los denominados sistemas multicapa basados en envases ampliamente
utilizados en la actualidad, que en muchos casos pueden hacer uso de capas metalizadas.
Aún así, hay ventajas significativas en términos de costos, estrategias de empaquetado
ecológico (que consiste en reducir el consumo de materiales de embalaje por unidad de
envase) y otros problemas, como la facilidad de reciclado para el desarrollo de formulaciones
de envasado más sencillas y menos preocupadas por el medio ambiente. Como resultado,
durante las últimas décadas se han llevado a cabo grandes esfuerzos en el desarrollo de
materiales y en las estrategias de mezcla para reducir la complejidad de las estructuras de
envasado de alimentos al tiempo que se adapta el rendimiento. estrategias de empaquetado
ecológico (que consiste en reducir el consumo de materiales de embalaje por unidad de
envase) y otros problemas, como la facilidad de reciclaje en el desarrollo de formulaciones de
envasado más sencillas y menos preocupadas por el medio ambiente. Como resultado,
durante las últimas décadas se han llevado a cabo grandes esfuerzos en el desarrollo de
materiales y en las estrategias de mezcla para reducir la complejidad de las estructuras de
envasado de alimentos al tiempo que se adapta el rendimiento. estrategias de empaquetado
ecológico (que consiste en reducir el consumo de materiales de embalaje por unidad de
envase) y otros problemas, como la facilidad de reciclaje en el desarrollo de formulaciones de
envasado más sencillas y menos preocupadas por el medio ambiente. Como resultado,
https://www-sciencedirect-com.etechconricyt.idm.oclc.org/science/article/pii/S0924224411000082?_rdoc=1&_fmt=high&_origin=gateway&_docanchor=&md5=b84294
3/5/2018 Nanotecnología para bioplásticos: oportunidades, desafíos y estrategias - ScienceDirect
durante las últimas décadas se han llevado a cabo grandes esfuerzos en el desarrollo de
materiales y en las estrategias de mezcla para reducir la complejidad de las estructuras de
envasado de alimentos al tiempo que se adapta el rendimiento.
Although packaging can help reduce organic waste by preserving foods, the substantial
increase in the use of plastics has also raised a number of environmental concerns from a
waste management point of view. As a result, there has been a strong research interest,
pushed by authorities at national and international levels, and a concomitant industrial growing
activity in the development and use of biodegradable and/or biobased materials. The term
“biodegradable” refers to materials that can disintegrate or break down naturally into biogases
and biomass (mostly carbon dioxide and water) as a result of being exposed to a microbial
environment and humidity, such as the ones found in soil, hence reducing plastic waste,
whereas “biobased” sustainable materials, apart from being typically biodegradable albeit not
necessarily, consume carbon dioxide during their production, hence creating the potential for
the new concept of “carbon neutral materials” (Haugaard et al., 2001; Lagaron, Gimenez, &
Sanchez-Garcia, 2008; Petersen et al., 1999).
Amongst biobased materials, three families are usually considered: Polymers directly extracted
from biomass, such as the polysaccharides chitosan, starch, carrageenan and cellulose;
proteins such as gluten, soy and zein; and various lipids. A second family makes use of
biomass-derived monomers but uses classical chemical synthetic routes to obtain the final
biodegradable and/or renewable polymers, including thermoplastics and thermosets such as
those obtained derived from vegetable oils. In regard to thermoplastics, this is the case of
polylactic acid (PLA) and the non-biodegradable sugar cane ethanol-derived biopolyethylene
(Haugaard et al., 2001; Lagaron et al., 2008; Petersen et al., 1999). The third family makes use
of polymers produced by natural or genetically modified micro-organisms such as
polyhydroxyalkanoates (PHA) and polypeptides such as the elastin-like polymers (Reguera
et al., 2003). Amongst non-biobased materials, i.e. using either petroleum-based monomers or
mixtures of biobased- and petroleum-based monomers, there are also a number of
biodegradable resins such as polycaprolactones (PCL), polyvinyl-alcohol (PVOH) and its
copolymers with ethylene (EVOH) and some biopolyesters. Nevertheless, it seems clear that
although biodegradability can help reduce plastic waste, from a “green house” perspective,
biobased sustainable materials, the so-called bioplastics, are currently considered the way to
go and may be the only alternative in the future as fossil resources become exhausted.
Moreover, in order to reduce energy consumption during the production of bioplastics and
potential competition with agricultural resources for foods and also to provide additional raw
material sources, the exploitation of food by-products is also the current trend. Food processing
effluents or solid wastes are only partially exploited and are mostly disposed in landfill sites
where, since they are amenable to putrefaction, they have to be treated according to the
restrictions identified by, for instance, the international Landfill Directive (Awarenet, 2004).
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These by-products have rarely been used as a source of high added-value components such
as food ingredients, but they present great potential value for their use in the production of
bioplastics (Beccari et al., 2009).
Moreover, the high surface-to-volume ratio of many nanoscale structures which favours this
improved performance of composite materials, also becomes ideal for applications that involve
chemical reactions and drug delivery. Examples of their usefulness include the controlled
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and/or burst release of substances in active and functional food packaging technologies and
energy storage applications in, for instance, intelligent food packaging (Lopez-Rubio, Gavara, &
Lagaron, 2006; Shonaike & Advani, 2003).
Nanoclays
Amongst the various existing nanotechnologies available, the one that has attracted more
attention in the bioplastics field is the nanoclay-based nanocomposites. It has been broadly
reported in the scientific literature that the addition of low loadings of nanolayered clay particles,
i.e. nanoclays, with thickness in the nanometre scale and with high aspect ratios, to
biopolymers can have a profound enhancing effect over some material properties, such as
mechanical properties, thermal stability, UV–vis protection, conductivity, processability and gas
and vapour barrier properties (Cabedo, Giménez, Lagaron, Gavara, & Saura, 2004; Cyras,
Manfredi, Ton-That, & Vázquez, 2008; Lagaron et al., 2005, 2008; Park, Lee, Park, Cho, & Ha,
2003; Petersson & Oksman, 2006; Sanchez-Garcia, Hilliou, & Lagaron, 2010; Xu, Ren, &
Hanna, 2006; Yu, Lin, Yeh, & Lin, 2003). Moreover, the addition of low amounts of
nanoadditives does not alter to a significant extent, inherently good properties of polymeric
matrixes such as transparency and flexibility (Marras, Kladi, Tsivintzelis, Zuburtikudis, &
Panayiotou, 2008; Sanchez-Garcia, Hilliou, et al., 2010; Sanchez-Garcia, Lagaron, & Hoa,
2010; Wan, Qiao, Zhang, & Zhang, 2003). Important issues associated to the use of
bioplastics, such as the non-intended migration of plastic components to foods, can also be
potentially reduced by the use of these nanoclays and, since more recently, they also offer
great advantages in the formulation of active packaging technologies based on bioplastics such
as more efficient antioxidant, oxygen scavenging or antimicrobial biopackaging, which has
more direct implications in increasing packaged foods quality and safety (Busolo, Ocio, &
Lagaron, 2009; Lagaron, Gimenez, & Cabedo, 2007; Lopez-Rubio et al., 2006; Sanchez-
Garcia, Ocio, Gimenez, & Lagaron, 2008).
Fig. 1 shows, as an example, that the performance of biopolyesters, in terms of oxygen barrier,
is already significantly improved by melt compounding addition of food-contact complying
nanoclays (Sanchez-Garcia, Gimenez, & Lagaron, 2007). Although in comparison with PLA,
the PLA nanocomposite approaches more closely the barrier performance of the petroleum-
based polyester counterpart polyethylene terephthalate (PET), it does not yet outperform the
polyester oxygen barrier and further optimization work is required. On the other hand, the
nanoclay-based PHB does already outperform PET (Sanchez-Garcia et al., 2007) and, hence,
this microbial biopolymer has a good potential in food packaging applications.
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Fig. 1. Oxygen permeability of PLA, PHB and PET and of their nanocomposites (Sanchez-Garcia et al.,
2007).
As the worldwide production capacity of biopolyesters continues to grow, their cost will soon be
comparable to their petroleum-based counterparts. Currently, it is estimated that the
consumption of petroleum-based plastics amounts to ca. 52 million tons/year vs. only ca.
750,000 tons/year for bioplastics. Ideally, the biopolymers cost should be below 2 €/kg for mass
replacement of their petroleum-based counterparts. Food-contact complying nanoclays, on the
other hand, are currently mass produced. Depending on the grade, their cost can be below
10 €/kg (information provided by NanoBioMatters S.L., Spain), fact that together with the
recommended low dosages, i.e. typically below 5 wt.-%, convert these nanoadditives in truly
accessible commodities for food biopackaging applications.
Other nanofillers
Most applications of nanocomposites in bioplastics for packaging have made use of laminar
clays, but also, to some extent, of carbon nanotubes (Sanchez-Garcia, Lagaron, et al., 2010)
and nanoparticles of metals and oxides (Travan et al., 2009). However, there are other types of
reinforcing elements such as biodegradable cellulose nanowhiskers (CNW) and nanostructures
obtained by electrospinning, which are very promising in a number of application fields (Huang,
Zhang, Kotaki, & Ramakrishna, 2003; Lopez-Rubio et al., 2007; Olsson et al., 2010; Sanchez-
Garcia, Gimenez, & Lagaron, 2008; Torres-Giner, Gimenez, & Lagaron, 2008). The use of
biobased nanofillers to reinforce bioplastics has the additional value of generating fully
biobased formulations. These nanobiofillers (CNW and electrospun nanofibers) have a very
large surface to mass ratios (up to 103 higher than a microfiber), excellent mechanical strength
(this is true for the CNW and for some reinforced electrospun fibres), flexibility, lightness and, in
same cases, edibility since they can be made of food hydrocolloids (Capadona et al., 2009;
Helbert, Cavaillé, & Dufresne, 1996; Rojas, Montero, & Habibi, 2009). As previously
commented for the clay-based nanocomposites, the resulting properties of nanocomposites
with cellulose fibres are strongly related to the dimensions and aspect ratio of the fibres
(shifting from micro- to nanosized fibres improvements in optical and mechanical properties
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have been observed), as well as to the compatibility with the polymer matrix (Dubief, Samain, &
Dufresne, 1999; Hubbe, Rojas, Lucia, & Sain, 2008; Siaueira, Bras, & Dufresne, 2009). Aspect
ratios are mainly related to the origin of the cellulose used and to the nanowhisker preparation
conditions (Azizi Samir, Alloin, & Dufresne, 2005). The advantage of application of these
nanomaterials has already been considered in the controlled release of bioactive substances in
the pharmaceutical and biomedical fields and can also be applied as reinforcing fillers
(Sanchez-Garcia & Lagaron, 2010). Other uses include the controlled release of active and
bioactive compounds in food packaging applications, as well as for the nanoencapsulation of
functional added-value food additives (Fernandez, Torres-Giner, & Lagaron, 2009; Lopez-
Rubio, Sanchez, Sanz, & Lagaron, 2009).
As stated above most nanocomposite technologies in the market today make use of chemical
or otherwise modified commodity layered 2:1 or 1:1 phyllosilicates, the so-called nanoclays. A
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chemical and/or physical modification is needed to both compatibilize highly hydrophilic clays
with the more organic apolar chemical constitution of most thermoplastic biopolyesters and to
increase the clay intergallery space (basal space between adjacent layers), hence facilitating
both intercalation and exfoliation, i.e. nanodispersion, of the clay laminar components in the
matrix during compounding. In the food chain, special caution is needed because the
modifications should comply with the stringent migration regulations, i.e. functional barrier
status, and preferably make use of food-contact approved substances as valid modifiers.
Currently, many of the existing nanoadditives, such as those modified with some ammonium
salts which are commercially available, do not comply with, for instance, the current European
food-contact directive issued by the European Food Safety Authority (EFSA) (Commission
Directive 2007/19/CE, 2007).
Therefore, it is a very important concern that most of the nanocomposite formulations (first
generation nanocomposites, i.e. containing standard or general purpose organic-modified
nanoclays) in the market are currently making use of ammonium salts as organophilic chemical
modifiers, which have been devised to enhance the properties of engineering polymers in
structural applications. However, for food packaging applications, as mentioned above, only
food-contact approved materials and additives should be used, and should do so below their
corresponding threshold specific migration levels. Thus, second generation nanocomposites,
specifically designed to comply with current regulations and, at the same time, be cost effective
and specifically formulated to target particular materials (including biopolymers), materials
properties or production technologies are more suitable for the food biopackaging market. In
essence, second generation nanocomposites refer to materials with targeted specifications
rather than wide spectrum generic formulations.
In general, there is a lack of knowledge about the impact of nanomaterials when inserted into
bioplastics during service. For instance, very little is known about their stability during
processing and potential toxicity issues related to decomposition and/or migration and also as
to how they will affect the actual inherent bioplastic migration levels and the current
establishment of afterlife disposal channels such as incineration, composting or recycling.
However, and regarding this issue, the prospects for natural additives such as food-contact
complying nanoclays, essentially microparticles, and nanobiofibers due to edibility and/or
resorbability or biocompatibility may not be of so much concern in biopackaging. For instance,
regarding the afterlife disposal, we have found out in our research that nanoclays in
biodegradable matrices do not delay biodegradation during composting, since it is a process
that occurs from the outside towards the inside and that the nanoclays, due to their inherent
high surface energy, re-attach to each other to become microparticles of soil once the polymer
matrix disappears (Lagaron & Fendler, 2009). Similarly, several studies have demonstrated that
addition of nanoclays to various synthetic polymers led to enhanced or accelerated degradation
in comparison with the kinetics observed for the neat polymers (Kumanayaka, Parthasarathy, &
Jollands, 2010; Qin, Zhao, Zhang, Chen, & Yang, 2003; Tidjani & Wilkie, 2001). As a result,
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Regarding inherent nanoparticle hazard assessment, due to their small size, nanoparticles are
generally much more reactive than their corresponding macro-counterparts. But it is also true
that as a result of this, much smaller filler loadings are typically required, and hence added to
the matrix, to achieve the desired properties. The large surface area of nanoparticles allows a
greater contact with cellular membranes, as well as greater capacity for absorption and
migration (Li & Huang, 2008). Therefore, assessment of the effects of nanoparticles in food
packaging materials such as migration to foods, and potential bioaccumulation needs to be
considered in the expected dosages. Currently, data on toxicity and oral exposure of
nanoparticles are extremely limited and controversial when it comes to the studied dosages. In
addition, the small size of many nanoparticles causes them to take on unique chemical and
physical properties that are different from their macroscale chemical counterparts. This implies
that their toxicokinetic and toxicity profiles cannot be extrapolated from data on their equivalent
non-nanoforms. Thus, the risk assessment of nanoparticles has to be performed on a case-by-
case basis (Munro, Haighton, Lynch, & Tafazoli, 2009). However, it is also very important to
differentiate between three-dimensional nanoparticles (spherical or otherwise 3D nanoparticles
such as nanometals), which are capable of penetrating the cell membranes, bi-dimensional
nanoparticles (nanofibers, with only nanodimensions in the 2D cross-section), which are less
likely to penetrate cell walls and the least concerned, one dimensional nanoparticles (nanoclays
with only one nanodimension in the thickness direction). Thus, nanoclays should be considered
aside because in essence they are heat stable microparticles, which remain such all along the
process of production and commercialization and to a significant extent also as two-
dimensional microparticles within the biopolymer matrix during service. In any case, the general
risk assessment of migration products resulting from packaging materials has and continues to
pose a difficult challenge. As a general rule, nanocomposites within the European Union must
comply with the EFSA total migration limit of 10 mg/dm2, with the functional barrier stringent
migration level of 0.01 mg/kg of food or food simulant and/or with the specific migration levels
for their constituents in case they comprise food-contact components (Commission Directive
2007/19/CE that modifies Directive 2002/72/CE). Some studies have shown that upon melting
nanocomposite plastic films, some clay accumulation appears to occur at the surface of the
materials generating a clay-containing barrier (Hao, Lewin, Wilkie, & Wang, 2006; Lewin &
Tang, 2008). However, information about actual migration to food or food simulants is very
scarce. In a recent study, Schmidt et al. (2009) characterized the migration and size of migrated
particles from PLA nanocomposites in a fatty food stimulant (ethanol). The previous authors
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Finally, it is envisaged that the potential strategies to overcome the above and other pending
issues will come from focussing the research efforts and political strategies on the following
items:
- Boosting the creation of nanotechnology industry-based platforms with solid knowledge
of the problems to solve and of the legislation and commercialization barriers ahead.
Open innovation and collaborative action towards more rapid product development will
strongly benefit the area. Development and commercialization of commodity products
are a must. Thus, nanotechnology will only contribute to widespread the use of
bioplastics through the balancing of their properties if they become a commodity in terms
of pricing and volumes. This could significantly happen in developing countries since the
raw materials availability for bioderived products is vast and venture capital grows
interest.
- Focussing R&D efforts in order to provide real value for nanobiocomposites, i.e.
developing the underpinning science and technology to understand and control the
composition/properties/processing/aging relationship of nanobiocomposites.
- Developing new bioplastics and tailor-made reinforcing nanobioadditives that make use
of only biobased products and resources, particularly derived from valorization of food
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by-products.
- Deepening our understanding about the potential toxicity of current and under
development nanomaterials and of their nanobiocomposites. This should be carried out
through the characterization of the stability of nanobiocomposites during processing and
shelf-life, full migration studies and assessment of issues related to the various disposal
channels.
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