Coal to Carbon Fiber (C2CF) Continuous Processing for High Value Composites (Final Report)

Abstract

Coal tar is a condensed and recovered by-product of the coking of metallurgical coal for steel production. The heaviest fraction of distilled coal tar is an isotropic pitch largely used as a binder in the manufacturing of carbonaceous electrodes for primary aluminum smelting and in electric arc furnaces. Coal tar pitch offers high carbon yield upon carbonization. In this project, a process to convert the domestically sourced isotropic coal tar pitch, containing very low particulates (QI = 0.32 wt.%), to form flow-domain mesophase pitch amenable for melt spinning into precursor (green) fibers for carbon fiber, was developed and optimized. The final reproducible processing developed is reviewed in this report, along with several characterizations of the mesophase pitch. A final definition of the characteristics of a ‘spinnable’ mesophase pitch is presented. With this mesophase pitch, reproducible and stable multifilament melt spinning was developed, producing green fiber tows with filament diameters of approximately 20 m. The multifilament melt spinning was the most challenging aspect of the project and required the most effort. The best practices learned from this project for melt spinning are reviewed in this report. Once spun, the green fibers were oxidatively stabilized, carbonized and graphitized under inert gas atmosphere to form the final carbon fibers. Given the relatively high softening point of the mesophase pitch, no issues of interfilament fusion were observed during batch oxidation, and subsequent batch carbonization and graphitization went smoothly in all cases. An ~ 80 wt.% conversion of the green fiber mass to final carbon fiber was achieved. After graphitization, the carbon fibers showed high tensile moduli (most were ~ 600 GPa, or 87 Msi) consistent with commercially-available high-performance pitch-based carbon fiber. However, tensile strength and strain to failure were comparatively low. Further work to reduce defects in and on the fiber surfaces would increase these properties. SEM imaging of the graphitic fiber textures is presented herein. Rudimentary composites were fabricated from the carbon fibers and characterized showing similar modulus to baseline composites fabricated with commercial carbon fiber. Finally, a basic economic analysis was done showing the potential to increase the value of the isotropic coal tar pitch by up to 13.6 to 136 times based on a carbon fiber value of $\$$5/lb to $\$$50/lb, respectively. Moreover, the site case study suggests that the coal tar from the single integrated steel mill could supply production of up to 16 kt/yr of carbon fiber. Finally, a technological gap analysis was done which shed light on remaining technical challenges. These challenges included: recovery and utilization of condensates from the mesophase pitch processing, further advancing and increasing stability of the multifilament melt spinning processing, optimization of the oxidation processing, defect reduction for increased carbon fiber strength, and the development of a weaving process towards carbon fiber fabrics. To maximize the coal value chain, the primary objectives of this project were to (a) develop and scale efficient processing technology for producing melt-spinnable mesophase pitch from isotropic coal tar pitch, (b) clarify and simplify tedious continuous fiber processing technologies (particularly multifilament melt spinning of mesophase pitch) towards the efficient production of high performance carbon fiber, and (c) demonstrate and characterize representative composite parts derived from the final carbon fiber. Immense progress was made on all 3 objectives and is detailed in this report.