Abstract
For last 50 years plastics are widely used for manufacturing of packaging materials because of their performance and ease in production. With the advent of food processing industries there is a great demand for petroleum based packaging materials for food applications. However, increased use of plastics has created serious ecological problems to the environment because of their resistance to biodegradation. Biopolymers can be used as a solution to the problems posed by plastics as they easily degrade in the environment and also mimic the properties of conventional polymers. Biopolymers can be classified into three categories according to their origins of production. These are polymers extracted from biomass, synthesized from bio-derived monomers and produced from microorganisms. There are different film formation methods for biopolymers like solution casting method, melt mix method, electro spinning method, thermo pressing and casting, extrusion blown film method. The quality of polymers can be expressed as different properties like physical, thermal, mechanical and barrier properties. This review highlights the different kinds of biodegradable polymers, their characteristics with special emphasis on their market potential for food packaging applications. The review revels that presently starch based, PLA, PHA and different blends have been manufactured by industries, film properties compared with petrochemical based polymer for MAP and other food packaging applications. Since information on biopolymers is widely scattered over many sources and are very scarce compared to the conventional polymers, this article intends to give an overview of the state of the art on biodegradable polymer packages for food applications.
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Introduction
Today, polymers are an integral part of contemporary life because of their desirable properties including stability, resilience and ease in production. Worldwide production of plastics was approximately 322 million tons in 2015 which is a 3.5% increase as compared to 2014 [1]. In 2014–15, India produced 8.3 million tons of plastics [2]. At present, about 99% of all plastic materials are manufactured by the petrochemical industries, i.e., they are produced from petroleum based (non-renewable) resources [3,4,5]. In India, about 43% of annually produced synthetic polymers are utilized by packaging industry which is more than the world average of 39% [4]. Production and processing of plastics are energy exhaustive processes; those lead to increased emissions of greenhouse gases (GHGs) of enormous magnitude contributing to global warming. Moreover, plastics on burning release venomous emissions such as carbon monoxide, chlorine, hydrochloric acid, dioxin, furans, amines, nitrides, styrene, benzene, 1, 3-butadiene, and acetaldehyde which possess threat to environment as well as to public health [6]. Apart from degrading air quality, plastics generate lots of waste after use that has adverse effects on environment (leaching of chemical in aquifers, soil pollution) [7,8,9]. Waste generated from the plastics has been a pressing problem for many years because of their resistance to degradation [3, 10]. India produces about 5.6 million tons plastic waste every year. The environmental impact caused by excessive quantity of non-degradable waste materials is necessitating research and efforts to develop new alternate materials that can be manufactured with the utilization of environmentally friendly raw materials [3, 11, 12]. In recent years, bioplastics have emerged as an alternative to curb the menace caused by the plastics. The European Bioplastics Organization state that a plastic material is defined as a bioplastic if it is either biobased, biodegradable, or features both properties. The need of replacement for the petroleum based plastic with bio based polymers is impartial because producing conventional plastics consumes 65% more energy, unsustainable (due to environmental problems) and emits 30–80% higher greenhouse gases than bioplastics [13, 14]. Biodegradable polymers are produced from renewable sources, are complete biodegradable and mimic the properties of conventional polymers like polyethylene (PE), polypropylene (PP), polyethylene terephthalate (PET), etc. [15]. Thus, biopolymers in the form of packaging materials are key innovations that can help in reducing the environmental impact of plastic production and can have high value generation potential from the agriculture feed stocks [16].
Production and Application Statistics of Bioplastics
The global market for biodegradable polymers reached 206 million pounds at an average annual growth rate (AAGR) of 12.6% in 2010 and is expected to rise further by several folds in next 10 years [17]. According to a study by Institute of Bioplastics and Bio composites (2016), bioplastics production increased from 1.6 to 2.0 million tons during the period 2013–2015, biobased non-degradable polymers had the share of 0.9–1.3 tons and biodegradable plastics 0.6–0.7 million tons and it may attain 1.7 million tons by 2020. The shares of biobased non-degradable and biodegradable plastics were 63.7% and 36.3%, respectively. Majority of biodegradable plastics are made up of PLA (polylactic acid) (10.9%), biodegradable polyesters (10.8%), biodegradable starch blends (9.4%) and PHAs (polyhydroxyalkanoates) (3.6%). In bioplastics production, Asia contributes 63.1%, North America 13.5%, Europe 13.0% and South America 10.0%. Mostly biodegradable bioplastics are used for flexible packaging and non-degradable bioplastics are used for rigid packaging. The future of bioplastics focuses on the market for compostable, semi-durable and durable bio plastics used in consumer and industrial applications [18]. Biodegradable polymers can be used for modified atmospheric storage (MAP) of fruits and vegetables instead of conventional polymers. In MAP it is often desirable to generate an atmosphere low in O2 and/or high in CO2 to influence the metabolism of the product being packaged and the activity of decay-causing organisms to increase storability and/or shelf life. In addition to atmosphere modification, MAP vastly improves moisture retention, which can have a greater influence on preserving quality than O2 and CO2 levels [19,20,21,22,23,24,25,26,27,28,29,30]. Figure 1 represents the global scenario of bioplastics application in different sectors at present and a future estimation [18].
Biopolymers and Their Potential as a Packaging Material
Packaging is an integral component of the food processing sector. Food packaging is a combination of art, science and technology of enclosing a product for achieving safe transportation and distribution of the products in wholesome conditions to the users at least price [31]. Most of the conventional packaging materials are products of petro chemicals like PVC, PET, polystyrene (PS), polypropylene (PP), polyamide (PA) [23, 25, 29]. The properties which make them unique for packaging of food are low cost, excellent physical properties (density, molecular weight), mechanical properties (tensile strength), transmission properties (O2, CO2), which not only increase the shelf-life of the product, but also add functionality in terms of convenience and attractiveness to the consumers [32, 33]. The only problem with synthetic polymers is their resistance to degradation in the environment [34, 35]. According to ASTM standards D-5488-94d, biodegradable is defined as capable of undergoing decomposition into carbon dioxide, methane, water, inorganic compounds and biomass. With increased awareness on sustainability, the packaging industries around the globe are looking for biopolymers as the replacement of synthetic polymer. Biopolymers may be defined as the polymers that are biodegradable by the enzymatic action of microbes. In last two decades, a lot of research has been done on biopolymers for food packaging applications [36, 38].
Based on the researches biopolymer based packaging materials may be divided into three main groups based on their origin and production (Fig. 2) [36, 39,40,41].
Group 1 Thesis constitutes polymers which are directly extracted or removed from biomass. Certain polysaccharides such as starch, cellulose, and proteins (like casein and gluten) constitute represent this category. All these are, by nature, hydrophilic and somewhat crystalline and create problems while processing. Besides, Further, their performances are also poor especially in relation to packaging of moist food products. However, their excellent gas barrier properties make them suitable for their utilization in food packaging industry [36, 37, 40, 42,43,44,45].
Group 2 Thesis includes polymeric materials which are synthesized by a classical polymerization procedure such as aliphatic aromatic copolymers, aliphatic polyesters, poly-lactide, aliphatic copolymer (CPLA), using renewable bio-based monomers such as poly (lactic acid) and oil-based monomers like poly-caprolactones. A good example of polymer produced by classical chemical synthesis using renewable bio-based monomers is polylactic acid (PLA), a biopolyester polymerized from lactic acid monomers. The monomers themselves may be produced via fermentation of various carbohydrate feed stocks. PLA may be plasticized with its monomers or, alternatively, oligomeric lactic acid. PLA can be formed into blown film, injected mold objects and coating. Therefore, all together explaining why PLA is the first novel bio-based material produced at commercial scale [36, 37, 40, 42,43,44,45].
Group 3 Polymers which are produced by microorganisms or genetically modified bacteria constitute this group. Till date, this group of bio-based polymers consists mainly of the polyhydroxy-alkanoates, but developments with bacterial cellulose and other polysaccharides are also in progress. [39, 40, 42,43,44,45].
Starch Based Biopolymers
Starches are low cost polysaccharides, abundantly available and one of the cheapest groups of biodegradable polymers. It is also known hydrocolloid biopolymer. It is composed of amylose (poly-α-1, 4-d-glucopyranoside), a linear and crystalline polymer and amylopectin (poly-α-1, 4-d-glucopyranoside and α-1, 6-d-glucopyranoside), a branched and amorphous polymer. The amylose and amylopectin contents of starch ranges from about 10–20% and 80–90%, respectively, depending on the source [47]. Amylose is soluble in water and forms a helical structure [44]. Various kinds of starches like potato, cassava, rice, corn, and tapioca are used for the preparation of biopolymers [48,49,50]. Starch is usually used as a thermoplastic. It is plasticized through destructuration in presence of specific amounts of water or plasticizers and heat and then it is extruded. So thermoplastic starch has high sensitivity to humidity. Starches are poor resistance to moisture and their mechanical property restricts their uses. To improve these properties starches are blended with various biopolymers and certain additives. The list of research carried out on starch-based biopolymers is given in Table 1.
Protein Based Biopolymers
Many of the proteins like gelatin, keratin, and casein consisting very interesting features of polymers such as flexural, shear strength, tensile modulus, as well as exceptional material properties including toughness, strength and elasticity. Thus, these proteins are also useful for the creation of new biodegradable polymer for various commercial applications. Protein-based biodegradable polymers they have an expanding range of potential applications in formation of food and non-food packaging, and as biomaterials like reconstructive surgery, tissue engineering, etc. Therefore, the protein-based polymer can be used for the polymer reinforcement. The mechanical properties of protein polymer can be further enhanced by blending them with other protein and/or non-protein molecules. Blending technology gives us an opportunity to develop next generation biodegradable polymer/plastics which can replace the conventional plastics from the market. In food packaging industries films made by protein polymers (like Milk proteins, Whey protein, Gelatin, Wheat gluten, Corn, Zein, Soy protein, Egg white, etc.) are used as an edible film so that they can consume along with the food. Plant proteins from soybean, wheat, and corn are readily available and films from these proteins have been investigated extensively. The employment of protein-based film concepts to edible packaging materials promises to improve barrier and mechanical properties and facilitate the effective incorporation of bioactive ingredients and other functions such as tampering resistance, a barrier from oxygen, water vapor and dust, etc. In non-food packaging polymer of keratin, casein, zein, gelatin and soy-protein, etc., could play a crucial role in the development of various commercial products like shopping bags, mulch film, flushable sanitary product, etc. Blends of protein with non-protein, natural molecules such as chitosan, cellulose, and with synthetic polymer like polypropylene, polyethylene, polyvinyl chloride, etc., were prepared to improve the plastic properties of protein-based polymer which are suitable for food and non-food packaging [63].
Polylactic Acid (PLA)
PLA is one of the biopolymer that has gained lot of attention in recent years because of its economic and commercial viability during processing [62, 64]. Poly (lactic acid) (PLA) belongs to the family of aliphatic polyesters made up from alpha-hydroxyacids, including polyglycolic acid or polymandelic [63,64,65,–66]. The polylactic acid (PLA) is obtained from the controlled depolymerization of the lactic acid monomer obtained from the fermentation of sugar feedstock, corn, etc., which are readily biodegradable [65, 67]. PLA is a sustainable alternative to petrochemical-derived products, since the lactides are produced by the microbial fermentation of agricultural byproducts, mainly the carbohydrate rich substances [66, 68]. The yield of lactic acid from different microorganisms and different sources is shown in Table 2. PLA is becoming a growing alternative as a green food packaging material because it was found that in many circumstances its performance was better than synthetic plastic materials [17].
PLA is usually obtained from polycondensation of D- or L-lactic acid or from ring opening polymerization of lactide, a cyclic dimer of lactic acid [36, 44, 45, 68, 70]. Properties that make PLA a good food packaging material are their high molecular weight, water solubility resistance, good process ability, i.e., easy to process by thermoforming and biodegradability [36, 37, 44, 68, 70]. PLA has the tensile strength modulus, flavor and odor barrier of polyethylene and PET or flexible PVC; the temperature stability and process ability of polystyrene; and the printability and grease resistance of polyethylene. PLA can be processed by several approaches which include injection molding, sheet extrusion, blow molding, thermoforming and film forming. Processed PLA comes in the form of films, containers and coatings for paper and paper boards. PLA can be further recycled by chemical conversion back to lactic acid and then re-polymerized. Although PLA seems to be potential biodegradable polymer to be utilized in packaging of various food products, it exhibits certain limitations in unmodified form, viz. it is more brittle and degrades easily at substantial temperature rise. The list of patents on starch and PLA based biopolymers is shown in Table 3.
Polyhydroxyalkanoates (PHAs)
Polyhydroxyalkanoates (PHAs), a family of bacterial polyesters, are formed and accumulated by various bacterial species under unbalanced growth conditions. These polymers are produced in nature by bacterial fermentation of sugar and lipids. Structurally, PHAs comprise simple macromolecules composed of 3-hydroxy fatty acid monomers. PHA has a considerably low volume of the biopolymer market, somewhere around 453.59 tons per year. In 2008, approximately 55,115.57 tons of PHAs were commercially produced. PHAs have thermo-mechanical properties similar to synthetic polymers such as polypropylene [76, 78]. PHA polyesters are biodegradable, biocompatible and can be obtained from renewable resources [77, 79]. They have several desirable properties such as petroleum displacement and greenhouse gas minimization apart from their fully biodegradable nature [44]. Poly (3-hydroxybutyrate) (PHB) is one of the biodegradable PHA (polyhydroxyalkanoates) and is naturally occurring β-hydroxyacid linear polyester [78,79,80, 82]. The general structure of the repeating units of these polyesters is different depending on the type of bacteria and the feed, it is typically -(CH2)n-CH3 for most naturally occurring PHAs [81, 83]. Applications of PHA as a biodegradable packaging include bottles, containers, sheets, films, laminates, fibers and coatings. Over 100 monomers and copolymers can be developed from PHAs. Some of the polymers used are PHB, PHV, PHBV (Metabolix), PHBO, PHBH, PHBD. PHAs exhibit good tensile strength, printability, flavor and odor barrier properties, heat sealability, grease and oil resistance, temperature stability and are easy to dye, which boosts its application in food industry [44]. For example, Metabolix, a US-based company, produces “Metabolix PHA”, which is a blend of polyhydroxybutyrate (PHB) and poly (3-hydroxyoctanoate) that has been approved by the FDA for production of food additives and making packages that maintain all the performance characteristics of non-degradable plastics. Polyhydroxybutyrate (PHB), a lipid-like polymer of 3-hydroxybutyrate accumulate as a carbon and energy reserve under unbalanced (unfavorable) growth conditions, such as nutrient limitation. In general, PHB accumulation is favored by adequate availability of a suitable carbon source and a limiting supply of nitrogen, phosphate or dissolved oxygen or certain micro components like sulfur, potassium, tin, iron or magnesium [82, 84]. PHB exists in the cytoplasmic fluid in the form of crystalline granules having diameters of 0.2–0.7 μm and are surrounded by a membrane coat composed of lipid and protein about 2 nm thick and can be isolated as native granules or by solvent and enzymatic extraction [83,84,85,86].
Pathways for Synthesis of Biopolymers
Renewable sources like agriculture feed stocks (starches) act as a precursor for the synthesis of various biopolymers through enzymes and microbial fermentation. A schematic flow chart for the synthesis of biopolymers is shown in Fig. 3.
Application of Biofilm for MA Packaging
Modified atmosphere packaging is food preservation techniques in which the O2 concentration is reduced and CO2 concentration is increased to reduce the overall metabolic processes, there by extend the shelf life of the commodities. It is an economical and simple technique for extending the shelf life with preserving quality of fruits and vegetables. Researchers have successfully used petroleum based film for enhancing the storage life of various commodities [24,25,26,27]. In this study some relevant research work carried out on modified atmosphere packaging of fruits and vegetables using biodegradable polymers are listed and presented in Table 6.
Application of Biopolymers in Smart Food Packaging
Over the course of the last decade, significant interest in the use of biopolymers within the food industry as smart and active polymer systems has emerged. Such polymers have been successfully utilized to entrap micronutrients within microparticles and antioxidant packaging and have also been employed within food quality monitoring systems, such as active and intelligent packaging systems. The technologies that are associated with smart and active biopolymers have the potential to drive the development of a new generation of intelligent/active packaging systems that integrate food quality monitoring systems and microparticles in a manner that extends the shelf life of food products and their nutritional value [96].
Properties of Biopolymers
The shelf life of any product in a packaging depends primarily upon the barrier properties of the packaging material. Gas phase permeation through a nonporous material occurs through adsorption at the leading interface, diffusion through the material, and desorption at the trailing interface and is often measured with three parameters: transmission rate, permeance, and permeability. Transmission rate is the volume or weight of a permeant (e.g., oxygen or moisture) passing through a film per unit surface area and time under equilibrium with testing conditions. Permeance is the transmission rate divided by the partial pressure difference of the permeant across the film. Permeability is the permeance multiplied by the thickness. Barrier properties are not only determined by the nature of a material, but also a function of temperature, pressure, and relative humidity. Barrier properties are usually measured under equilibrium moisture conditions with a controlled environment [97, 98]. Oxygen, CO2 and water vapor are the main parameters studied in packaging applications. The change in product quality (weight loss, color change, change in pH and increase in microbial growth) occurs due to the movement of these gases and water vapor [45]. The properties of different biopolymers are listed in Table 7. The requirement of oxygen and carbon dioxide gas composition for optimum storage varies for different commodities. During the MAP of food, the gas composition changes due to different biological and chemical reactions, this results loss in product quality. The packaging material should have recommended level of permeability to gases and water vapor to maintain equilibrium atmosphere and thus to extend the shelf life of product.
If the oxygen permeability of film is high then the vapor pressure of oxygen inside the package increases and it leads to oxidation as well as respiration (fruits and vegetables) of the product. Water vapor barrier property of film is required for some products like bakery products, powders which need to be stored at very low moisture [45]. The oxygen, carbon dioxide and water vapor barrier properties of a film are quantified by the oxygen permeability coefficient (OPC), carbon dioxide permeability coefficient (CO2 PC) and water vapor permeability coefficient (WVPC), respectively, which indicate the amount of O2 oxygen or CO2 or water vapor that permeates per unit of area and time in a packaging material [(kg m m−2 s−1 Pa−1]) [103]. Transmission properties of different biopolymers and conventional polymers are listed in Table 8 [34, 45].
It is well- known that the polymer architecture plays an important role on the mechanical properties, and consequently on the process utilized to prepare the final product (i.e., injection molding, sheet extrusion, blow molding, thermoforming, and film forming). In addition, many packaging containers are commercially used below room temperature, so it is important to assess the mechanical performance under these conditions [17, 45]. The list of physical and mechanical properties of different bio and conventional polymers is shown in Table 9 [94, 99].
Thermal properties of film also play important role during the selection of packaging material, because most of the food products are stored at lower than the atmospheric temperature. The selection of packaging material mainly depends upon the processing, packaging and storage temperatures. Thermal properties can be characterized as glass transition temperature (Tg) and melting temperature (Tm); these can be calculated by differential scanning calorimeter (DSC). Thermal properties of different bio and conventional polymers are listed in Table 10 [39, 94, 99].
The advantage of biodegradable polymers over petroleum based polymers is its biodegradability. This can be quantified by emission of CO2 or CH4 or consumption of oxygen during the degradation process (Table 11).
Self-Healing Antimicrobial Biopolymer Film for Food Packaging
Antimicrobial properties are more essential to regulate unwanted microorganisms on food products by infusion of dynamic molecules, such as antimicrobial compounds. Antimicrobial compounds have also been incorporated into films for use in active packaging. These films are considered active because they rely on diffusion through the packaging medium as opposed to a triggered release of antimicrobials via responsive materials. Early research in this area utilized films incorporated with antibacterial/antifungal compounds like sodium benzoate and benomyl [104]. More recently, edible and inedible films have been explored that utilize natural antimicrobial ingredients like clove, pepper, cinnamon, coffee, and others [105,106,107,108]. Chitosan, another biologically derived material, has also been thoroughly researched due to its natural antimicrobial activities and its non-toxicity [109,110,111]. Rhim et al. [112] reported chitosan based Nano-silver and Ag-Ion incorporated nanocomposite films shows antimicrobial properties and enhance food quality and safety due to reducing the improvement of contaminant microorganisms after the post processing. Direct implementation of antimicrobial enzymes like lysozyme and other biocatalysts in active packaging has also been explored [113]. Very recently, bacteriophages have been embedded into acetate cellulose films for use against Salmonella Typhimurium [114]. Cinnamon oil-embedded polymer films have also been recently produced at the pilot-scale to repel larger pests and insect larvae [107]. Some other forms of antimicrobial packaging will enhance quality and safety of food products, like addition of sachets containing volatile antimicrobial agents into packages that are inherently antimicrobial due to immobilization of ions and covalent linkages [115].
Methods for Manufacturing Biodegradable Films
Manufacturing of biopolymers is a multi-step process that requires proper skill and thorough understanding of behavior of bio polymers during processing. Biopolymers can be processed into varieties of products (packaging films, laminated paper, films, trays, cups cutlery items) depending upon the processing route (cast films, blow molding, coextruded films). The fundamental step of processing of any biopolymer involves melting the biopolymer mix followed by casting, extrusion, blow molding, depending upon the material to be made. Different methods of processing of biodegradable materials are listed in Table 12.
Biodegradation of Biopolymers
During degradation, the polymer is first converted to its monomers and then these monomers are mineralized. Biodegradation is governed by different factors that include polymer characteristics, type of organism, and nature of pre-treatment. The list of factors affecting the rate of biodegradation of polymers is shown in Table 13. The polymer characteristics such as its mobility, tacticity, crystallinity, molecular weight, the type of functional groups and substitutes present in its structure, and plasticizers or additives added to the polymer all play an important role in its degradation [98, 99, 116, 117]. The reactions occurring during the biodegradation of polymers is shown below.
Tests for Biodegradation
To assess the biodegradability of a polymer there are mainly three methods, which include laboratory tests, simulation tests and field tests as shown in Fig. 4. The flow chart for soil burial test and enzymatic tests for biodegradation of biopolymers is shown in Figs. 5 and 6. The list of different standard methods to measure biodegradation of polymers is listed in Table 14.
Life Cycle Assessment of Biopolymers
LCA is an instrument to measure the sustainability and performance of a material with environment. Life cycle of biopolymer mimics the LCA of a biomass [105, 123]. Like biomass, biopolymers are degraded into carbon and water upon degradation by the action of enzymes and microbes. LCA of biopolymer is shown in Fig. 7. Biodegradation rate of different biopolymers is shown in Fig. 8. Biodegradation rate is calculated as the CO2 released during analysis, divided by the theoretical CO2 contained in the sample; EdK is a parameter used to quantitatively evaluate the potential biodegradability of biodegradable polymers in the natural environment. Natural soil samples are inoculated into bioreactors, and rates of biodegradation of reference materials are determined over a 2-week period. Starch and polyethylene are used as reference materials to define the EdK values of 100 and 0, respectively. Values are determined using the ISO 14852 method, detecting the evolved carbon dioxide as an analytical parameter.
Conclusions
Biopolymers help in reducing the environmental impact of plastic production, processing and in a way lead towards green economy. As biodegradable films are made from renewable feed stocks, agricultural waste, there is a great opportunity for research work in harnessing this economic opportunity. But still, the biodegradable polymer at present only replaces about 1% of the plastics. After three decade of researches, biopolymers are not at par with the conventional polymers because of the economics of scale in production, complicated downstream processing operations, and stability and durability issues as compared to plastics. Therefore, need of the hour is that basic and applied researches have to be more focused on improving the performance (physiochemical, thermal properties), reducing the cost and improving ease in production of biopolymers. The use of bio based polymers is increasing at a rapid pace for packaging of food and other applications. In context of food packaging the biodegradable packaging can be used for modified atmosphere packaging of high value products and niche merchandises like organic foods. However, before adopting any bio based packaging for food there has to be proper studies on the interaction between food components and biopolymers during processing and storage. Future researches have to be more focused on adding value to the packaging materials, i.e., use of nanotechnology, smart sensors, etc., which will not only maintain the integrity, but also communicate the information about the product to the consumers. Through biodegradable polymers there is a greater potential in better utilization of agricultural waste, addressing the problems of shortage of fossil fuel, health hazards, solid waste management and environmental issues as possessed by plastics. In nutshell, biopolymers driven innovations will contribute to a sustainable environment, economy and society.
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Mangaraj, S., Yadav, A., Bal, L.M. et al. Application of Biodegradable Polymers in Food Packaging Industry: A Comprehensive Review. J Package Technol Res 3, 77–96 (2019). https://doi.org/10.1007/s41783-018-0049-y
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DOI: https://doi.org/10.1007/s41783-018-0049-y