The formation of highly ordered graphitic interphase around embedded CNTs controls the mechanics of ultra-strong carbonized nanofibers

Abstract Templating graphitization, i.e., the transformation of certain polymers to highly-ordered graphitic (HOG) domains upon pyrolysis in the vicinity of graphitic nanomaterials, such as carbon nanotubes (CNTs), is known to be an effective approach to modify the microstructure of carbon nanofibers (CNFs). In this work, the microstructure of CNFs subjected to the templating effect of functionalized single-walled CNTs (f-SWNTs) and the effect of templating on mechanical properties of CNF/f-SWNTs hybrid nanofiber are studied. The CNF/f-SWNTs were fabricated via pyrolysis of electrospun polyacrylonitrile precursors with CNT inclusions. Prior to pyrolysis, the precursors were subjected to thermomechanical treatments, known as hot-drawing, to enhance chain and CNT alignment and packing. The study of the microstructure of the precursor and CNFs indicates the crucial role of precursor hot-drawing in enhancing the microstructure of the precursor and CNFs, leading to drastically enhanced templating effect, as evidenced from the thickness of the HOG that forms around CNTs. Mechanical tests on single nanofibers using custom-designed microdevices led to the realization that the templating effect of CNTs on CNFs, when properly implemented via precursor hot-drawing, can considerably increase the strength of CNFs. The average tensile strength and modulus of CNF/f-SWNTs in which HOG domains had clearly formed were measured to be 7.6 and 268 GPa, respectively, which are the highest value reported to date among similar types of materials. The existence and evolution of the HOG around CNTs inside CNFs and mechanical reinforcing of HOG were thoroughly discussed in conjunction with finite element models of building blocks of CNFs, alluding to the stress fields around HOG and CNTs in the CNF. The high-performance 1-D hybrid graphitic nanostructure developed here, CNF/f-SWNTs, can serve as an outstanding reinforcement material for weight sensitive applications.