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- ItemA New Route to Highly Stretchable and Soft Inorganic–Organic Hybrid Elastomers Using Polydimethylsiloxane as Crosslinker of Epoxidized Natural Rubber(New York, NY [u.a.] : Wiley InterScience, 2021) Banerjee, Shib Shankar; Banerjee, Susanta; Wießner, Sven; Janke, Andreas; Heinrich, Gert; Das, AmitSulfur or peroxide crosslinking is the most common and conventional method to develop elastomeric materials. A new approach to crosslink epoxidized natural rubber (ENR) by aminopropyl terminated polydimethylsiloxane (AT-PDMS) is described, intending to develop a new kind of hybrid organic–inorganic elastomers. The curing reaction is accelerated by using hydroquinone as a catalyst. The formation of the hybrid structure is evident from the appearance of two glass transition temperatures, at −1 and −120 °C, for the ENR and PDMS phases, respectively. The curing reaction is found to be of first order with respect to amine concentration with the estimated activation energy of ≈62 kJ mol−1. Comparing the mechanical properties to a typical ENR-sulfur system leads to the conclusion that the ENR/AT-PDMS hybrid structure is highly stretchable and soft, as demonstrated by its relatively higher strain at failure (up to ≈630%), and lower hardness and modulus values. The higher stretchability and soft nature of the material are achieved by introducing flexible PDMS chains during the curing process resulting to a hybrid elastomer networks. This kind of soft but robust materials can find several applications in diverse fields, such as soft robotics, flexible, and stretchable electronics.
- ItemInfluence of Controlled Epoxidation of an Asymmetric Styrene/Butadiene Star Block Copolymer on Structural and Mechanical Properties(Basel : MDPI, 2020) Khatiwada, Shankar P.; Staudinger, Ulrike; Jehnichen, Dieter; Heinrich, Gert; Adhikari, RameshwarThe chemical modification (namely the epoxidation) of a star shaped block copolymer (BCP) based on polystyrene (PS) and polybutadiene (PB) and its effect on structural and mechanical properties of the polymer were investigated. Epoxidation degrees of 37 mol%, 58 mol%, and 82 mol% were achieved by the reaction of the copolymer with meta-chloroperoxy benzoic acid (m-CPBA) under controlled conditions. The BCP structure was found to change from lamellae-like to mixed-type morphologies for intermediate epoxidation level while leading to quite ordered cylindrical structures for the higher level of chemical modification. As a consequence, the glass transition temperature (Tg) of the soft PB component of the BCP shifted towards significantly higher temperature. A clear increase in tensile modulus and tensile strength with a moderate decrease in elongation at break was observed. The epoxidized BCPs are suitable as reactive templates for the fabrication of nanostructured thermosetting resins.
- ItemPoly(acrylonitrile-co-butadiene) as polymeric crosslinking accelerator for sulphur network formation(London [u.a.] : Elsevier, 2020) Hait, Sakrit; Valentín, Juan López; Jiménez, Antonio González; Ortega, Pilar Bernal; Ghosh, Anik Kumar; Stöckelhuber, Klaus Werner; Wießner, Sven; Heinrich, Gert; Das, AmitThe major controlling factors that determine the various mechanical properties of an elastomer system are type of chemical crosslinking and crosslink density of the polymer network. In this study, a catalytic amount of acrylonitrile butadiene copolymer (NBR) was used as a co-accelerator for the curing of polybutadiene (BR) elastomer. After the addition of this copolymer along with other conventional sulphur ingredients in polybutadiene compounds, a clear and distinct effect on the curing and other physical characteristics was noticed. The crosslinking density of BR was increased, as evidenced by rheometric properties, solid-state NMR and swelling studies. The vulcanization kinetics study revealed a substantial lowering of the activation energy of the sulphur crosslinking process when acrylonitrile butadiene copolymer was used in the formulation. The compounds were also prepared in the presence of carbon black and silica, and it was found that in the carbon black filled system the catalytic effect of the NBR was eminent. The effect was not only reflected in the mechanical performance but also the low-temperature crystallization behavior of BR systems was altered. © 2020 The AuthorsMaterials science; Materials chemistry; Crosslinking accelerator; Sulphur network; Solid state NMR; Curing kinetics; Activation energy; Acrylonitrile butadiene; Polybutadiene; Low-temperature; Crystallization. © 2020 The Authors
- ItemA nonequilibrium model for particle networking/jamming and time-dependent dynamic rheology of filled polymers(Basel : MDPI, 2020) Robertson, Christopher G.; Vaikuntam, Sankar Raman; Heinrich, GertWe describe an approach for modeling the filler network formation kinetics of particle-reinforced rubbery polymers—commonly called filler flocculation—that was developed by employing parallels between deformation effects in jammed particle systems and the influence of temperature on glass-forming materials. Experimental dynamic viscosity results were obtained concerning the strain-induced particle network breakdown and subsequent time-dependent reformation behavior for uncross-linked elastomers reinforced with carbon black and silica nanoparticles. Using a relaxation time function that depends on both actual dynamic strain amplitude and fictive (structural) strain, the model effectively represented the experimental data for three different levels of dynamic strain down-jump with a single set of parameters. This fictive strain model for filler networking is analogous to the established Tool–Narayanaswamy–Moynihan model for structural relaxation (physical aging) of nonequilibrium glasses. Compared to carbon black, precipitated silica particles without silane surface modification exhibited a greater overall extent of filler networking and showed more self-limiting behavior in terms of network formation kinetics in filled ethylene-propylene-diene rubber (EPDM). The EPDM compounds with silica or carbon black filler were stable during the dynamic shearing and recovery experiments at 160 °C, whereas irreversible dynamic modulus increases were noted when the polymer matrix was styrene-butadiene rubber (SBR), presumably due to branching/cross-linking of SBR in the rheometer. Care must be taken when measuring and interpreting the time-dependent filler networking in unsaturated elastomers at high temperatures.
- ItemEffect of prestrain on the actuation characteristics of dielectric elastomers(Basel : MDPI, 2020) Kumar, Mayank; Sharma, Anutsek; Hait, Sakrit; Wießner, Sven; Heinrich, Gert; Arief, Injamamul; Naskar, Kinsuk; Stöckelhuber, Klaus Werner; Das, AmitDielectric elastomers (DEs) represent a class of electroactive polymers that deform due to electrostatic attraction between oppositely charged electrodes under a varying electric field. Over the last couple of decades, DEs have garnered considerable attention due to their much-coveted actuation properties. As far as the precise measurement systems are concerned, however, there is no standard instrument or interface to quantify various related parameters, e.g., actuation stress, strain, voltage and creeping etc. In this communication, we present an in-depth study of dielectric actuation behavior of dielectric rubbers by the state-of-the-art “Dresden Smart Rubber Analyzer” (DSRA), designed and developed in-house. The instrument allowed us to elucidate various factors that could influence the output efficiency of the DEs. Herein, several non-conventional DEs such as hydrogenated nitrile rubber, nitrile rubber with different acrylonitrile contents, were employed as an electro-active matrix. The effect of viscoelastic creeping on the prestrain, molecular architecture of the matrices, e.g., nitrile content of nitrile-butadiene rubber (NBR) etc., are also discussed in detail.