Harnessing High-Density-Polyethylene-Derived Liquid as a Model Solvent for the Co-Liquefaction of Low-Rank Coals: Toward Sustainable Mesophase Pitch for Making High-Quality Carbon Fibers from Waste Plastics

The accumulation of polyolefin waste, particularly high-density polyethylene (HDPE), presents a growing environmental challenge due to limited recycling options and poor end-of-life recovery. This study explores a strategy to convert HDPE into mesophase pitch (MP), a valuable carbon precursor, by integrating polyolefin recycling with the mild solvolysis liquefaction (MSL) of low-rank coals. HDPE was first hydrogenolyzed into a hydrogen-rich aromatic liquid (HDPE-liquid), which was then used as the liquefaction solvent. Under identical conditions (400 °C, 60 min), Utah Sufco coal co-liquefied with HDPE-liquid produced tar that formed mesophase pitch with a higher mesophase content (84.5% vs. 78.6%) and a lower softening point (~302 °C vs. >350 °C) compared to pitch from conventional tetralin (THN). The approach was extended to Illinois #6 and Powder River Basin coals, increasing the mesophase content from 12.4% to 32.6% and 17.8% to 62.1%, respectively. These improvements are attributed to differences in tar composition: HDPE-derived tars had lower terminal methyl (Hγ) contents, reducing cross-linking during thermal upgrading. This work demonstrates that HDPE-derived liquids can act as functional solvents for coal liquefaction, enabling an effective route to recycle polyolefin waste into durable carbon products, while also reducing reliance on fossil-based solvents for mesophase pitch production.