Investigation of filler network percolation in carbon black (CB) filled hydrogenated butadiene-acrylonitrile rubber (HNB

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Investigation of filler network percolation in carbon black (CB) filled hydrogenated butadiene‑acrylonitrile rubber (HNBR) Jiwen Liu1 · Benxin Li1 · Yehua Jiang1 · Xiaojuan Zhang1 · Guangshui Yu1 · Chong Sun1 · Shugao Zhao1 Received: 28 July 2020 / Revised: 22 October 2020 / Accepted: 1 November 2020 © Springer-Verlag GmbH Germany, part of Springer Nature 2020

Abstract The filler network is one of the most important concepts in filled rubber nanocomposites. It ensures the rubber matrix some properties, such as electrical conductivity, heat conductivity, reinforcement property, and so on. The more or the less the filler content, the worse the combination properties. Therefore, the filler network percolation threshold is very significant to be controlled. In this work, the filler network percolation in CB filled HNBR was investigated, combining dielectric with dynamic and quasi-static mechanical measurement. The results showed there are two sudden increases in the platform value of the conductivity by 1–3 orders of magnitude by means of dielectric measurement. They are defined as the (α) process and the (α′) process, respectively. The (α) process that the CB content is between 25 vol.% and 26.5 vol.% is classified to the electric percolation threshold, according to the percolation theory prediction. Meanwhile, the (α′) process that the CB content is between 21.7 vol.% and 23.4 vol.% corresponds to the mechanical percolation threshold, according to the result of mechanical measurement. Keywords  Filler network · Percolation · Dielectric property · Mechanical property

Introduction It is well known that the incorporation of nanoscopic fillers as carbon black, silica, or polymeric microgels can markedly improve the mechanical, electrical, and other properties of elastomeric polymers. The effect of fillers on reinforcement of a rubber is of scientific and commercial importance [1].

* Chong Sun [email protected] 1



Key Laboratory of Rubber and Plastics, Ministry of Education, Qingdao University of Science and Technology, Qingdao 266042, China

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Polymer Bulletin

There are some reports of the percolation behavior of filler networks. Sumita et  al. [2] investigated polymer dynamics in highly filled composites and proposed that dynamic percolation measurements may provide an incisive method to study the influence of particle–polymer interactions on the relaxation and viscoelastic properties of a polymer matrix. Mujtaba et  al. [3] drew the percolation threshold at a silica volume fraction of about 15 (vol.%) for silica-filled solution styrene–butadiene rubbers by means of nuclear magnetic resonance (NMR) and mechanical measurements. In addition, Meier et al. [4] had investigated the CB network in elastomers by dielectric spectroscopy. Reinforcement is one of the most important concepts for filled systems [5]. Guth and Gold [6] were the first authors to point out that the static modulus E and Ef of unfilled and filled rubber material obeys the law Ef = A(𝜑) ∗ E , in which the coefficient A(𝜑