Covalent-Organic Framework-Manipulated Multi-Reactant Activation Enables Polystyrene Electrodegradation in Tandem With Over-Oxidation Product Upgrading.

Authors

Yu Chen, Xiao-Hong Chen, Qian-Qian Huang, Si-Ying Huang, Run-Han Li, Ya-Fang Guan, Jiang Liu, Ning Li, Ya-Qian Lan

Published in

Angewandte Chemie (International ed. in English). Pages e5012045. Sep 14, 2026. Epub Sep 14, 2026.

Abstract

Polystyrene (PS) waste is exceptionally difficult to chemically degrade under environmental conditions, and the high-value utilization of low-value C₁ products generated during the process has never been achieved. Herein, we constructed a metalloporphyrin-anthracene sp² covalent-organic framework (COF) electrocatalyst, TAPP-Fe^III-An, which displays high structural stability and outstanding capability in activating O₂ and multi-reactants. This enables it to effectively electro-degrade PS into high-value benzoyl products (yield, 23.2%, M_w residue 0.3%) and re-convert 20% of C₁ products into high-value 1-formyl-1,2,3,4-tetrahydroquinoline (anticancer drug intermediate) with 9.4% yield, through a tandem quinoline carbonylation reaction. This breaks the traditional dilemma where PS degradation produces low-value byproducts that are difficult to re-utilize. Electrochemical experiments combined with theoretical calculations reveal that the valence tautomerism (Fe^II-Fe^III-Fe^IV) of metal center and active An ligand endow TAPP-Fe^III-An catalyst with the ability to activate O₂ (generating ¹O₂, •O₂ ^-, and •OH) and multi-reactants (PS and CO), thus enabling efficient PS electrodegradation (to benzoyl products) in tandem with low-value C₁ products carbonylation (to anticancer drug intermediate). In this process, the generated C₁ products (HCOOH, CO) were re-activated by TAPP-Fe^III centers, and then react with 1,2,3,4-tetrahydroquinoline for high-value conversion. This work pioneers a tandem conversion strategy for PS waste degradation and low-value C₁ products upgrading.

PMID:
42733956
Bibliographic data and abstract were imported from PubMed on 14 Sep 2026.

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