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Mar Intetonl nual of Enea a Entonmentsl Communication 3.12021) 48.5, Maejo International Journal of Energy and Environmental Communication Journal homepage: htps:/ph02.tclthaljo.org/Iadex.php/MIJEEC Eco-friendly natural rubber latex and modified starch-based adhesive for wood-based panels application- A re Triveni Soubam', Arun Gupta” "Faculty of Chemical & Process Engineering Technology, Universiti Malaysia Pahang, 26300 Gambang, Pahang Malaysia, ARTICLEINFO ABSTRACT Arle histor Received 18 March 2021 Received in svied form, 12 apm 2001 Abvepied 28 April 2021 Resort NRL Rice starch Formaldetyde Syatbetie resin Sustainable bio-adbesive The we of formaldehye-based sythetic adhesives forthe development of wood-based panels thas increased rapidly inthe industry. Synthetic adhesives ae regarded aa threat to lean, ‘nenlth and a pollatant because they emis frmaldetyde's encinagenic gos. The breskahrengh lune prompted to sec: fora loug-enm solutiouto the formaldelyde zest with natural esourees There as been a significant rise in bio-based adhesive tehmology and development in the ‘wood-based panel indsty. The eurent review article i intended to present the potentials and the deowwhacs of the development of bio-adhesives fiom sustninable resourses sch as natural rubber latex (NRL) and starch. This review also discussed the chemical modification and crosslinkers of starch t9 improve water resistance and adhesion properties, Moreover, this anticle diseusses the compatibility of modified sice starch and NRL for their couclisive applicitioas as wood-hased panels aahesive. The findings aigaesed thet bio-based adhesives could replace more syutheti-based adhesives with comparable performance in the near future. 1. Introduction ‘Wood: based panels adhesives are synthetic polymers intended to interact physically, chemically, or both with the surface of the ‘wood i such a way that constaints are transmitted between bonded members, ideally without adhesive rupture or isconnection from the wood. Also, adhesives play a significant key role in determining the strength of the wood-based panels, Today, most of the adhesives used in the industries for bonding wood panels are synthetic adhesives, specifically phenol- fomaldehyde, wee-formaldehyde and melamine-formaldehyde, ‘hich pose a risk to human health and polluted air quality by emitting carcinogenic gas, formaldehyde, dusing the lndustal production aud usage of wood-based panels (Moubark et al 2013), Formaldehyde has been classified as the source of * Conesponiing auton Evra acres arin mp aba my (Ana Gp) 2673-0587 ©2019. Aleit reserved nasopharyngeal cancer by the Intemational Agency for Research, (on Cancer (IARC). Hence, California Air Resource Board (CARB) approved a regulation standard to lessen the formaldetyde emission from the wood-based panel's products, Therefore, renewable biopolymers such as starch (Li et al, 2014) and natural, rubber latex (Hemiati et al, 2006) are developing sustainable- based adhesives to fasten the composite wood panels. The application of NRL as a wood-based panel adhesive had reported many years ago due to its high strength, flexibility and elasticity (Weeramae ef al, 1972). However, natural eubber latex based adhesives’ physical aud mechanical strength is low compared to synthetic adhesives due to ther less heat resistance and moderate ‘water resistance (Marra, 1992) To promote the adhesion properties of NRL, the incorporation of the bio-based polymer as filler haé been found to 50 {improve the mechanical strength of NRL (Kim st al, 2016). As starch possess adhesion property naturally eiaforcing starch as an NRL filler bas davon concem on a lasge scale because of its abundance, inexpensiveness, and biodegradability (Liu et al., 2008). The starch can be found in rots, seeds and stalks of staple ‘rope such as wheat, ice, potato, corm ee. Though, the molecular structure of starch must be chemically modified or erosslinked with synthetic polymers to enhance its hydrophilicity nature before incorporation into NRL to generate an excellent efficiency of wood adhesive (Lei et al, 2014, Tan et al, 2011). The inclusion of ‘modified starch into NRL had improved the morphological and ‘mechanical properties ofthe overall adhesive system. The review focus on developing and applying the bio adhesive based on natural nubber latex incorporated with modified ce stare for wood-based panels bonding. 2. Natural rubber latex and starch bio-based. adhesive ‘Bio-based adhesives are natural adhesives derived from natural resources, such as starch, protein, lignin and tannin. Tt can provide ‘an environmentally fiendly and long-term substinte to the synthetic adhesives systems employed ia the wood-based panel industry. The natural adhesive can reduce the formaldehyde treat, ‘and indoor air quality issues caused by the wood-based panels ‘Simultaneously, bio-based adhesives can help accelerate the wood- based panel industry mose durable and reducing its seliance oa fossil fuels, However, the complete replacement of synthetic, adhesives with bio-based adhesives remains a. significant, challenge, owing to their relatively poor water resistance and large soatial varieties due to various growing consitions. There are ssuccessfil solutions to these drawbacks and diseuss them in the present review article, 2. Natural rubber latex as bio-adhesive ‘Natural rubber latex is a biopolymer of cis-4-polyisoprene. It is executed from the rubber tre scientifically named Hevea braziliensis. This biopolymer is well known for its impressive properties that even syuthetic subber latex could not win over as it is highly flexible at low temperature, high elasticity, resistant, against corrosion, impact and abrasion, provides greater adhesion, strength due tothe impermeability narute, good insulator and heat, lispersing agent (Rippel and Galembaek, 2000), Natural subber latex is mould and moisture resistant with no toxicity that boosts, ‘geen adhesive formulations’ application (Nasir et al, 2013). The partilebourd formed with NRL based adhesive had enhanced the ‘mechanical properties of the board (Nakanishi et al, 2018) However, Hermiati el. (2013) stated that the application of virgin, [NRL alone for the development of bio-adhesve is not advisable. ‘The biopolymer must be chemically modified or blend with ‘conventional adhesives to enhance the adhesion strength. Bras and Piccini (1951) were the frst to report the improvement in adhesion property when the lates is blended dizectly with syuthetic vesia ‘The petfoumance of NRL resin blend adhesive had beea studied on the different types of timber species and found that bond strength Mago ineraonlSural of ergy and Brooms! Conmanscaton of NRL based adhesives was increased significantly wien blended ‘with urea-formaldehyde aad phenol-formaldehyde resins. Whea NRL is a graft with diacetoue acrylamide (DAAM) using adipic acid diydrazide (ADH) as the crosslinking agen, te lap shear strength is improved considerably with the content of DAAM in the latex adhesives (Thongnuanchan, etal, 2007), Thus, uilization, ‘of natural mbber latex as an adhesive material is ouly practicable ‘upon chemical modification or incorporation with bio-polymer. ‘Table 1 Chemical composition of natueal subber latex (Baker and Fulton (1997). pecs = Day ibe content ooh coment Agaecas ses Mots wea 10510107 Hse. ‘c=cH i \ wwCH, —‘CHywwr Figure 1 Structure of cis-1 4-polyisoprene Hevea brasiliensis (Miller 2018), 2.2. Starch as bio-adhesive Starch is a white substance widely found in plant tissues, roots ‘and obtained from rice, cor, witeat, tapioca and potatoes, which ‘are insoluble in cold water or aleohol and one of the inexpensive biodegradable and sustainable polymers (Gaclhave et al.,2017a). It is a mixture of two polysaccharide ffactions- amylose and amylopectin both of distinct shapes and sizes, The proportion of these two polysaccharides differ on the genesis ofthe tare. Starch is a favourable material for the evolution of bio-adhesives due to its good adherence, inexpensive, easy accessibility and excellent film formation propeites (Tan etal, 2011 and Onssct, H. 1992), ‘A starch fiom ice, wheat, and potato has been used ia ‘manufacturing wood-based panels. However, the adhesive properties of starch vary with its genesis, andthe adhesion strength, of starch is not durable to fasten wooden products (Salleh et al., 2015), ‘Table 2 Amylose aud amylopectin content of starches (Gachave etal. 20178) ‘Wary com a a Tyce. v 3 De 2 o kitty 55-70) 30Gb) [Due to starc’s high viscosity, the entanglement of molecular weight macromolecules makes it hard to use them for industrial applications. The viscosity of starch ean be reduced by decreasing the aunber of entauglements per chain by adding molecules to swell the polymer network: Hence, starch needs to be chemically ‘modified or crosslinked to utilize in the wood industry (Movbacik et, 2010), Crepe fo Figure 2 Starch co-polymer with amylose and amylopectin ‘component (Masina et al.,2017). 2.3. Starch as filler for natural rubber atex-based adhesive EEarller, starch bas been utilized as a main component for adhesive development and as a bie-based filler for many elastomeric components, either for composites or adhesives development, From the mechanical point of view, the use of native starch as a reinforcing filler for mbber-based composites had been, investigated loag ago. Infision of native stach into mbber latex smatsix isthe reason behind the Weakening of mechanical steagth of composite wood due to incapable of homogeneous mixing With, the base component. This is due to the lyophilicity of starch agrauiles that led to the incompatibility of the non-polar hydrophobic nature ofthe rubber matrix. When (Kiing el 2013), employed native sago starch a5 filler to reinforce natural mibber latex; it eto the depletion of mechanical properties of composite panels, Progressively to overcome the incompatibility and impact, ‘caused by the incogporation of starch molecules in natural rubber particles, (Wu eta, 2004) employed a process to scieve uniform, starch in NRL matrix dispersion called the latex compounding method. The starch gragules were put for geltinization at temperature 90°C, and the gelatinized starch undergoes for compounding with NRL followed by immediate coagulation using calcium chloride. Based on the latex compounding theory, the size of starch particles was struak considerably, and this novel method enhanced the starch dispersion. The rubber starch based aduesives prepared through te latex compounding method exhibit optimized ‘performance compased to the syathetic adhesives. Consequestly to improve the reinforeing ability of starch on the NRL mati, ‘various surface weatment methods have been proposed and investigated by researchers 2.4, Chemical modification and crosslinking of starch-based adhesive ot (Chemical modification of hydrolysis is a chemical process in Which stare is added tothe aqueous solution of hydrochloric acid or sulphnsie aeid and in aqueous sodium hydroxide or potassium ‘hydroxide at a definite temperature (Okuulola and Akingbala, 2013). Ia an acid modification, starch's water resistance and adhesion properties are altered without disturbing its granular strutuze 10 enhance the solubility and gel strength. Generally starch is exposed to mineral acid below the gelatinization temperature (Pratiwi et al, 2018). The modification of starch increases the shor linear chain (amylose), which favour enhanced setcogradation (Dundar and Goemen, 2013). The process oF acidic ‘bydroiysis forms a erystallin structure of starch with an adequate Jength of amylose for the desirable formation of highly resistant and active starch molecules (Ferrin etal, 2008 and Ozturk etal 2011). Italso reduces the viscosity ofthe starch, whichis easier for ‘incorporation with other biopolymers (Ode etal, 2009), Similarly, the surface treatment of stach with sodium bhydeaxidsuecesfully removing the subsidiaries components found in starch granules that may affect its dispersion with other bio- polymers (Cihtmpom etl, 2012), Alkaline hydrolysis favours the ‘uncoiling, separation of double helices and obstruction of the crystalline stucture of starch. Thus, alkaline hydrolysis on starch expands stazch's amoyphous area and enhances the courespouding reaction with otter biopolymers. Also, the bonding strength and water resistance of starch-based adhesive can be synthesized via the graft copolymerization of oxidized starch with an olefin, ‘monomer and silane coupling agent (Zhang eal 2015). A nature- Iiendly starch adhesive with 2er0 foumaldehyde-emission was eveloped fom urea and oxidized stavch, where the adhesive shows an exceptional comprehensive performance and the stability of adhesive was enhanced by adding tianium dioxide nanoparticles (Zhso eta, 2018) ‘The starch crosslinked with sodium borate, epoxy chloropropane, hexamethoxymethylmelamine and isocyanstes, manifest high glueing properties and water resistance (Qiao et al 2015). Au epoxy sesin is a general commercial adhesive that can be used as a crosslinker of starch and other bio-based adhesives, (Nie et al, 2013). Af the same time, epoxy resins are mainly tested {or Veneer ghieing, imparting an adequate shear strength in arid and ‘wet cases. The starch modified with soevanate enhanced plyboare bonding properties and moisture resistance and can efficiently react with several finctioual groups, such as amino, carboxyl. and hhytroxyl groups with no formaldehyde emissions (Gu et al, 2010: Tan ef al, 2011), In Indonesia, the application of isocyanate adhesive for the bonding of composite wood has been expanded due to the formaldehyde cavcinogenle gas emission ftom the synthetic adhesive (Nuryawan and Alamsyah, 2017). A methyl methacrylate-grafied starch was modified with three different crosslinkers as dimethyloldihydroxyethyleneurea (DMDHEU), alutaraldehyde (G.A.) and N-methylol acrylamide (NMA) Tthas been found that DMDHEU crosslinked composite exhibits ‘minimum water absorption compared to GA. and NMA-based crosslinked composites. , the interaction between crosslinked polymer and wood is exceptional in DMDHEU crosslinked composites (Baishiya aud Maji 2014). When stach-based adhesive was prepated using- Methacryloxypropyl timethoxy silane (KHS70) as crosslinking agent, i improved the shear stwength an ‘promoted thermal stability. Furthermore, the KHS70 enbanced the 2 sltear-thinning property and weakened the pseudoplastic behaviour of the adhesive (Chen ef al, 2017), Therefore, to improve the incompatibiliy of stareh on the NAL matix, the starch must be chemically modified or blend with conventional, adbesivelcrossliakers to overcome its limitation upon blending with NRE, 2.5. Natural rubber latex fuse modified starch-based adhesive ‘for wood-based panels Starch is widely used in binders, sizing materials, glues and paste. It also played a significant role a5 a bio-based filer for elastomeric components for composite wood adhesives. The ability (of star as filer for abber-based adhesive ad bees looking over ong ago from the mechanical point of study. However, the hhy

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