Carbon nanotube (CNT) bundles/fibers possess promising applications in broad fields, such as artificial muscles and flexible electronics, due to their excellent mechanical properties. The as-prepared CNT bundles contain complex structural features (e.g., different alignments and components), which makes it challenging to predict their mechanical performance. Through in silico studies, this work assessed the torsional performance of CNT bundles with randomly packed CNTs. It is found that CNT bundles with varying constituent CNTs in terms of chirality and diameter exhibit remarkably different torsional properties. Specifically, CNT bundles consisting of CNTs with a relatively large diameter ratio possess lower gravimetric energy density and elastic limit than their counterpart with a small diameter ratio. More importantly, CNT bundles with the same constituent CNTs but different packing morphologies can yield strong variation in their torsional properties, e.g., up to 30%, 16% and 19% difference in terms of gravimetric energy density, elastic limit and elastic constants, respectively. In addition, the separate fracture of the inner and outer walls of double-walled CNTs is found to suppress the gravimetric energy density and elastic limit of their corresponding bundles. These findings partially explain why the experimentally measured mechanical properties of CNT bundles vary from each other, which could benefit the design and fabrication of high-performance CNT bundles.
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