Upcycled polymer waste-derived N-doped carbon supports enabling durable PtCo catalysts for PEM fuel cells

초록

Upcycling plastic waste into functional electrocatalyst supports enables a sustainable pathway for advancing fuel cell technologies. Herein, we develop nitrogen-doped carbon supports via a one-pot Friedel-Crafts reaction between waste polystyrene and pyrrole, enabling simultaneous hyper-crosslinking and nitrogen (N) incorporation without post-treatment. Upon carbonization, the resulting framework exhibits tunable N content and hierarchical porosity, providing a robust platform for proton exchange membrane fuel cell catalysts. N doping regulates ionomer distribution and strengthens Co-N coordination, promoting the formation of uniformly dispersed intermetallic PtCo nanoparticles with enhanced structural stability. Density functional theory calculations reveal that subsurface Co induces a downshift of the Pt d-band center, weakening *O adsorption and accelerating oxygen reduction reaction kinetics. As a result, the catalysts deliver a mass activity of 0.84 A mgPt- 1 at 0.9 V, approaching twice the U.S. DOE 2025 target. In full-cell tests, a peak power density of 1180 mW cm- 2 is achieved and retained at 1024 mW cm- 2 after 30,000 potential cycles, demonstrating excellent durability. This work presents a scalable and cost-effective strategy that integrates plastic waste upcycling with rational catalyst design, offering a viable route toward high-performance PEMFC systems.

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