Bridging Catalyst Design and Process- Level Analysis for Sustainable Polyethylene Recycling via Hydrogenolysis

Abstract

Aligning catalyst development with process-level sustainability metrics is crucial for advancing the chemical recycling of plastics. We bridge both elements to study hydrogenolysis of high-density polyethylene and report Ru–Ni alloy nanoparticles supported on titania that yield up to 55% liquid alkane products (C₆–C₄₅) under optimized conditions. Operando spectroscopy reveals Ru–Ni alloy sites formed in situ, and temperature-programmed experiments suggest an enhanced preference for internal instead of terminal scission over the bimetallic catalysts. By integrating these experimental insights with life cycle and techno-economic analyses, we identify a minimum average-chain-length threshold of C₁₁ for product distributions as a catalyst design guideline to reconcile environmental and economic objectives, illustrating the value of bridging catalyst design and process-level analyses.