Laser-Stabilized Atomically Dispersed Ru on Co3O4 Nanosheets for C1/C2 Selectivity in PET Electro-Upcycling

초록

Herein, we present a rapid and one-step CO2 laser irradiation strategy that stabilizes Ru single atoms (RuSAs) on two-dimensional Co3O4 nanosheets (RuSA/Co3O4) within 3 min under ambient conditions. The Co3O4 substrate was derived from microwave-synthesized alpha-Co(OH)2 (2.45 GHz, 1 min) followed by thermal oxidation at 350 degrees C for 1 h, affording a spinel oxide with ordered Co2+/Co3+ sites. Distinct from carbon-supported single-atom catalysts (SACs) systems, the oxide support functions as both an anchoring matrix and active redox component during the ethylene glycol oxidation reaction (EGOR). Combined experimental and theoretical analyses reveal that alpha-Co(OH)2 promotes C2-selective C & horbar;H bond oxidation to glycolate, Co3O4 favors C & horbar;C bond cleavage toward C1 products (formate), and RuSA/Co3O4 enables tunable and balanced C1/C2 product formation during the EGOR, highlighting the role of RuSA sites in regulating EGOR pathways with excellent stability over 100 h. Beyond the EGOR, practical polyethylene terephthalate (PET) waste upcycling was demonstrated using PET hydrolysate feedstock; the RuSA/Co3O4 catalyst achieves high recovery yields of terephthalic acid (88.0%), formate as potassium diformate (90.6%), and glycolate as potassium glycolate glycolic acid (91.3%). This study elucidates laser-induced defect-SA interactions for rapid SAC fabrication and establishes an integrated platform coupling SA engineering with plastic waste upcycling.

키워드