Critical Role of Rubber Functionalities on the Mechanical and Electrical Responses of Carbon Nanotube-Based Electroactive Rubber Composites

Abstract

Carbon nanomaterials, particularly carbon nanotubes (CNTs), are widely used as reinforcing fillers in rubber composites for advanced mechanical and electrical applications. However, the influence of rubber functionality and its interactions with CNTs remains underexplored. This study investigates electroactive elastomeric composites fabricated with CNTs in two common diene rubbers: natural rubber (NR) and acrylonitrile-butadiene rubber (NBR), each with distinct functionalities. For NR-based composites containing 2 vol% CNTs, mechanical properties, such as elastic modulus (2.24 MPa), tensile strength (12.48 MPa), and fracture toughness (26.92 MJ/m3), show significant improvements of 125%, 215%, and 164%, respectively, compared to unfilled rubber. Similarly, for NBR-based composites, the elastic modulus (5.46 MPa), tensile strength (13.47 MPa), and fracture toughness (82.89 MJ/m3) increase by 94%, 22%, and 65%, respectively, over the unfilled system. Although NBR-based composites exhibit higher mechanical properties, NR systems show more significant improvements, suggesting stronger chemical bonding between NR chains and CNTs, as evidenced by dynamic mechanical, X-ray diffraction, thermogravimetric, and thermodynamic analyses. The NBR-based composite at 1 vol% CNT content exhibits 261% higher piezoresistive strain sensitivity (GF = 65 at 0% ≤ Δε ≤ 200%) compared to the NR-based composite (GF = 18 at 0% ≤ Δε ≤ 200%). The highest gauge factor of 39,125 (1000% ≤ Δε ≤ 1220) was achieved in NBR-based composites with 1 vol% CNT content. However, 1.5 vol% CNT content in NBR provides better strain sensitivity and linearity than other composites. Additionally, NBR demonstrates superior electromechanical actuation properties, with 1317% higher actuation displacement and 276% higher electromechanical pressure compared to NR at an applied electric field of 12 kV. Due to the stronger chemical bonding between the rubber and CNT, NR-based composites are more suitable for dynamic mechanical applications. In contrast, NBR-based CNT composites are ideal for stretchable electromechanical sensors and actuators, owing to the high dielectric constant and polarizable functional groups in NBR.