Polyethylene Upcycling to Fuels: Narrowing the Carbon Number Distribution in N-Alkanes by Tandem Hydropyrolysis/Hydrocracking

• Upcycling PE plastic wastes via a tandem hydropyrolysis/hydrocracking was conducted. • The yields of gasoline and jet-fuel n-alkanes were maximized at 86.0 wt% and 68.1 wt%. • The effect of Co/Al molar ratio in CoAl 2 O 4 spinel on n-alkanes production was investigated. • The CoAl 2 O 4 spinel catalysts illustrated high activity in degrading realistic PE plastics. • A ∼73.1 wt% gasoline and a ∼54.7 wt% jet-fuel were retained after 3 cycles in-situ regeneration. The extensive use of plastics in modern life has resulted in a global waste crisis to the environment. Polyethylene (PE) is one of the most popular and hardest plastics to recycle because of its strong C(sp 3 )-C(sp 3 ) bonds. In this report, a tandem conversion process, i.e., hydropyrolysis and subsequent vapor-phase hydrocracking of primary intermediates (C n>5 alkenes and long-chain alkanes), was conducted via a two-step pressurized flow-through fixed-bed reactor over a CoAl 2 O 4 spinel-derived catalyst. The product distribution could be flexibly tuned by regulating operating parameters in the cascade fixed-bed reactor and Co/Al molar ratio in CoAl 2 O 4 spinel catalysts. Under optimal reaction conditions (0.2 MPa H 2 , 550 °C for hydropyrolysis in the 1st reactor, 300–325 °C for hydrocracking in the 2nd reactor, 20 s −1 of gas hourly space velocity), the maximum single-pass yields of gasoline (C 5 -C 12 ) and jet-fuel (C 8 -C 16 ) range n -alkanes reached 86.0 wt% and 68.1 wt%, respectively. The CoAl 2 O 4 spinel catalysts also gained high activity in degrading realistic post-consumer plastics such as linear low-, low-, and high-density PE, and a ∼ 73.1 wt% gasoline yield and a ∼ 54.7 wt% C 8 -C 16 yield were retained even after 3 cycles in-situ regeneration of deactivated CoAl 2 O 4 catalysts. This work provides an efficient and tunable approach to upcycle PE wastes into liquid fuels with an ideal carbon length.