Rubber nanocomposites experiencing dynamic shears at large strain amplitudes (γ) exhibit the nonlinear Payne effect featured by decays of storage and loss moduli (G′ and G″) or by G′ decay accompanied with G″ overshoot near a critical strain amplitude. The occurrence of the Payne effect has been assigned to damages of “filler network” and rubber-filler interfacial interactions for a long time and to Rouse dynamics of rubber chains recently. To solve the dispute, influences of extraction, crosslinking, and paraffin swelling on the Payne effect of carbon black filled natural rubber nanocomposites are investigated systematically. Master curves of G′ as a function of γ could be always created, and overshoot of G″ in the filled vulcanizates weakens with increasing filler content and intensifies by dilution via paraffin swelling, suggesting that the Payne effect is not mainly rooted in the “filler network” and rubber-filler interfacial interactions. The filler reduces the onset strain amplitude of the Payne effect by amplifying microscopic strain amplitude of the rubber phase, irrespective of whether the matrix is crosslinked or not and whether the crosslinked matrix is swollen or not. Partial removal of bound rubber by compounding the paraffin swollen compounds could lower modulus and eliminate G″ overshoot of the deswollen vulcanizates without influence on the mechanism of G′ decay accompanying Payne effect. The overshoot is found to be closely related to the overall viscous characteristic of the vulcanizates in the linear viscoelastic regime. Provided herein are new insights for recognizing the important roles of the viscoelastic rubber phase on the Payne effect of the nanocomposites.

中文翻译：

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炭黑填充天然橡胶纳米复合材料的佩恩效应：萃取、交联和溶胀的影响

橡胶纳米复合材料在大应变振幅 ( γ ) 下经历动态剪切，表现出非线性佩恩效应，其特征是存储和损耗模量 ( G'和G" )的衰减或G'衰减伴随着临界应变振幅附近的G"过冲。佩恩效应的出现长期以来被归结为“填料网络”和橡胶-填料界面相互作用的破坏以及最近橡胶链的劳斯动力学。为解决这一争议，系统研究了萃取、交联和石蜡溶胀对炭黑填充天然橡胶纳米复合材料佩恩效应的影响。G' 的主曲线作为γ的函数总是会产生，并且填充硫化胶中G" 的过冲随着填料含量的增加而减弱，并通过石蜡溶胀稀释而加剧，这表明 Payne 效应并非主要源于“填料网络”和橡胶-填料界面相互作用。填料通过放大橡胶相的微观应变幅度来降低佩恩效应的起始应变幅度，而不管基体是否交联以及交联的基体是否溶胀。通过混合部分去除结合橡胶的石蜡溶胀化合物可以降低模量和消除G“上的机构的deswollen硫化橡胶的过冲，而不影响G'伴随佩恩效应的衰减。发现超调量与线性粘弹性状态下硫化胶的整体粘性特性密切相关。本文提供了用于识别粘弹性橡胶相对纳米复合材料佩恩效应的重要作用的新见解。