Properties of economical and eco-friendly polybutylene adipate terephthalate composites loaded with surface treated coffee husk

https://doi.org/10.1016/j.compositesa.2020.106154Get rights and content

Highlights

  • Biodegradable poly(butylene adipate terephthalate) (PBAT) was reinforced with coffee husk (CH).

  • The PBAT and/or CH were successfully treated with different techniques.

  • The composite filled with silane treated CH exhibited superior thermal and mechanical property.

  • The ductility of the composite showed 53.8% improvement with the %EB reaching up to 500%.

  • The composite is 32% less expensive than the neat PBAT.

Abstract

In this study, we have fabricated ecofriendly and economical polybutylene adipate terephthalate (PBAT) composites loaded with various concentrations of coffee husks (CH) to investigate the effects on the PBAT and CH interfaces as well as the physical properties of the composites. Contact angle (CA) measurements revealed that the silane-treated CH (T-CH) is more hydrophobic than the raw CH, which improved its compatibility with PBAT. Morphological analysis of the composites revealed that the matrix exhibited greater interfacial interactions with T-CH compared to other derivatized PBATs. The elongation at break revealed a unique increase from 325% (neat PBAT) to 500%. The tensile strength, and Young's and storage moduli of the 40 wt% T-CH is greater than that of neat PBAT, indicating its superiority. Furthermore, the addition of 40 wt% CH to PBAT reduced the cost of the composite by 32%, making it economically competitive with other commercial polymers.

Introduction

The generation huge amounts of non-recyclable and non-renewable plastic wastes associated with utilization of petrochemical based plastics are creating immense environmental concerns [1], [2], [3]. As a result, many countries are now forcing the inclusion of biodegradable polymers into plastic commodities to substitute for conventional neat polymers [4], [5]. Some of the most popular biodegradable polymers include polylactic acid (PLA), polybutylene adipate terephthalate (PBAT), polybutylene succinate (PBS), and polyhydroxy-alkanoates [6], [7], [8], [9]. However, the cost of these biodegradable polymers is about 2.5–7.5 times higher than conventional polymers like polyethylene, polypropylene [10], [11]. A widely accepted method to lower the cost of biodegradable polymers is to incorporate lignocellulose materials that do not significantly affect the properties of the biodegradable polymers [12], [13], [14].

Lignocellulose materials are any materials that contain a large amount of cellulose, hemicellulose, and lignin in their structure [15], [16]. Many forestry or agricultural wastes like rice straw, wheat straw, bamboo fibers, and coffee waste are considered as lignocellulose materials [17], [18], [19], [20], [21]. Coffee, as one of the most consumed commodities, its processing generates huge amount of waste material with more than 50% of it is disposed as waste. Consequently, many researchers have been incorporating various types of coffee waste to make ecofriendly biodegradable composites with improved mechanical properties [22], [23], [24], [25], [26]. PLA and PBS composites fabricated by Totaro et al. [27] containing up to 30 wt% coffee silver skin (CSS) show an increase in Young’s modulus without affecting the tensile strength. In another study, PLA composite with increased water resistance and biodegradability, compared to the neat PLA, was synthesized by incorporating surface treated coffee spent ground (CSG) [28]. In addition, other researchers stated that the right amounts of extracts have a positive effect on the antiaging properties of PLA without adversely affecting properties of the polymer [29], [30].

Among the biodegradable polymers, PBAT is getting attention because of its unique properties, including high flexibility, ductility, and toughness. However, its low stiffness limits its commercial applications [31], [32], [33], [34]. For almost two decades, PBAT has been widely used in the packaging industry, biomedical sector, and agriculture. However, its high production cost limits its large-scale production for use in alternative fields of applications [35], [36], [37], [38]. Many researches have incorporated lignocellulose materials into PBAT with the aim of lowering its cost by keeping useful properties of the polymer. An excellent enhancement of the thermomechanical properties of PBAT was obtained by incorporating torrified CSG for food packaging applications [39], [40]. A PBAT/poly(3-hydroxybutyrate-co-3-hydroxyvalerate) blend was reinforced with CSS to fabricate a composite with an increased Young’s modulus and degree of crystallinity without altering its tensile strength [41].

In this work, we fabricated ecofriendly PBAT composite loaded with micro-sized coffee husk (CH) fibers by using a melt extrusion technique. CHs are fibrous waste products obtained after dehulling the coffee cherries to get the beans [42], [43]. Like other lignocellulose materials, coffee husks exhibit a hydrophilic nature due to the presence of many hydroxyl groups within its cellulose and hemicellulose. Consequently, the CH material does not have high interfacial interactions and compatibility with the hydrophobic PBAT [44], [45]. We made two modifications to change the interactions of CH and PBAT: silane treatment of CH to increase its hydrophobicity and maleic anhydride (MA) compatibilization of PBAT to increase its hydrophilicity. The physical and thermomechanical properties of the PBAT/CH composites were investigated using a contact angle goniometer, a thermogravimeter, a universal testing machine, and a dynamic mechanical analyzer.

Section snippets

Materials

Polybutylene adipate terephthalate resins (PBAT, SolPol-1000) was obtained from Gio Soltech Co., Ltd., (Gangwon-do, Republic of Korea). Coffee husk (Coffee arabica sp.) was collected from a local coffee processing plant in Hararge, Ethiopia. Maleic anhydride (MA), benzoyl peroxide (BPO) and 3-Glycidoxypropyl trimethoxysilane (GPTMS) are used as a compatibilizer, initiator and coupling agent, respectively, and were purchased from Sigma Aldrich, Seoul, Republic of Korea. All the solvents and

Coffee husk characterization

FTIR results revealed the presence of different functional groups on the surface of the untreated and T-CH (Fig. 2a). The sharp and broad spectral peak at 3453 cm−1 was attributed to hydroxyl groups which demonstrates the presence of a large amount of cellulose in CH. Methyl and methylene (single bondCsingle bondH) stretching vibrations in cellulose and hemicellulose were indicated with a peak at 2926 cm−1. The peak at 1734 cm−1 was associated with single bondCdouble bondO stretching of the carbonyl groups of lignin. The Cdouble bondC stretching

Conclusion

The focus on the fabrication and development of biodegradable polymers has increased due to environmental concerns over the use of petrochemical chemical based conventional polymers. The fabrication of biopolymer composites reinforced with lignocellulose materials is an effective approach to reduce their cost. We fabricated economical and ecofriendly PBAT composites loaded with CH by melt extrusion. The surfaces of the components were treated to improve the interfacial interactions between the

CRediT authorship contribution statement

Zelalem Chernet Lule: Conceptualization, Methodology, Writing - original draft. Jooheon Kim: Writing - review & editing, Supervision, Funding acquisition.

Declaration of Competing Interest

The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper.

Acknowledgement

This research was supported by the MSIT(Ministry of Science and ICT), Korea, under the ITRC(Information Technology Research Center) support program (IITP-2020-2020-0-01655) supervised by the IITP(Institute of Information & Communications Technology Planning & Evaluation).

References (48)

  • H.N. Dhakal et al.

    Development of sustainable biodegradable lignocellulosic hemp fiber/polycaprolactone biocomposites for light weight applications

    Compos Part A Appl Sci Manuf

    (2018)
  • S. Negi et al.

    Biomethanation potential for co-digestion of municipal solid waste and rice straw: A batch study

    Bioresour Technol

    (2018)
  • M.A. Ahsan et al.

    Green synthesis of a highly efficient biosorbent for organic, pharmaceutical, and heavy metal pollutants removal: Engineering surface chemistry of polymeric biomass of spent coffee waste

    J Water Process Eng

    (2018)
  • C.S. Wu

    Renewable resource-based green composites of surface-treated spent coffee grounds and polylactide: Characterisation and biodegradability

    Polym Degrad Stab

    (2015)
  • M. Hernández-López et al.

    Bio-based composite fibers from pine essential oil and PLA/PBAT polymer blend. Morphological, physicochemical, thermal and mechanical characterization

    Mater Chem Phys

    (2019)
  • V. Gigante et al.

    Rubber toughening of polylactic acid (PLA) with poly(butylene adipate-co-terephthalate) (PBAT): mechanical properties, fracture mechanics and analysis of ductile-to-brittle behavior while varying temperature and test speed

    Eur Polym J

    (2019)
  • L.B. Tavares et al.

    PBAT/kraft lignin blend in flexible laminated food packaging: Peeling resistance and thermal degradability

    Polym Test

    (2018)
  • F. Sarasini et al.

    Recycling coffee silverskin in sustainable composites based on a poly(butylene adipate-co-terephthalate)/poly(3-hydroxybutyrate-co-3-hydroxyvalerate) matrix

    Ind Crops Prod

    (2018)
  • D. García-García et al.

    Green composites based on polypropylene matrix and hydrophobized spend coffee ground (SCG) powder

    Compos Part B Eng

    (2015)
  • K.G. Mansaray et al.

    Determination of kinetic parameters of rice husks in oxygen using thermogravimetric analysis

    Biomass Bioenergy

    (1999)
  • M. Kumar et al.

    Effect of glycidyl methacrylate (GMA) on the thermal, mechanical and morphological property of biodegradable PLA/PBAT blend and its nanocomposites

    Bioresour Technol

    (2010)
  • Z.C. Lule et al.

    Enhanced directional thermal conductivity of polylactic acid/polybutylene adipate terephthalate ternary composite filled with oriented and surface treated boron nitride

    Polym Test

    (2020)
  • J.P. Harrison et al.

    Biodegradability standards for carrier bags and plastic films in aquatic environments: A critical review

    R Soc Open Sci

    (2018)
  • C. Maraveas

    Production of sustainable and biodegradable polymers from agricultural waste

    Polymers (Basel)

    (2020)
  • Cited by (31)

    View all citing articles on Scopus
    View full text