Dissolution-Mediated Synthesis of Atomically Thin High-Entropy Hydroxides for Efficient Polyester Glycolysis

Area of Science:

• Materials Science
• Catalysis
• Nanotechnology

Background:

• Atomically thin high-entropy hydroxides (HEHs) show promise in catalysis.
• Controlled synthesis of HEHs faces challenges like thermodynamic incompatibility and thickness control.

Purpose of the Study:

• To develop a novel synthesis strategy for atomically thin HEHs.
• To overcome limitations in multication coprecipitation and layered crystallization.
• To explore HEHs for sustainable polymer upcycling.

Main Methods:

• Dissolution-mediated growth strategy with controlled metal cation flux.
• Ultrafast NaBH4-driven coreduction of mixed metal precursors to form high-entropy boride (HEB) intermediates.
• Atmospheric oxidation of HEB intermediates followed by in situ reaction with hydroxide ions.

Main Results:

• Successfully synthesized atomically thin HEHs with defect-rich atomic architecture.
• Demonstrated 100% glycolytic recycling of poly(ethylene terephthalate) (PET) using FeCoNiCuZn-HEH-derived catalysts.
• Achieved superior catalytic performance compared to low-entropy and medium-entropy materials.

Conclusions:

• The developed synthesis approach effectively overcomes HEH fabrication challenges.
• High-entropy materials exhibit significant potential for sustainable polymer upcycling.
• This work advances the synthesis of high-entropy materials for catalytic applications.