Metal-free redox active covalent organic frameworks for electrocatalytic oxygen reduction reaction.

Authors

Bikash Mishra, Surajit Samui, Sourav Ghosh, Supriti Dutta, Chowdhury Ismat Nurani, Monojit Roy, Debashis Adhikari, Ranjit Thapa, Ramendra Sundar Dey, Pradip Pachfule

Published in

Science advances. Volume 12. Issue 35. Pages eaee3092. Aug 28, 2026. Epub Aug 26, 2026.

Abstract

Designing efficient, metal-free covalent organic framework (COF) electrocatalysts is a promising strategy for the oxygen reduction reaction (ORR) due to their structural tunability and stability. Herein, we report two redox-active donor-acceptor COFs, TAPA-DHTD and TTT-DHTD, incorporating a thiophene-based dithiophenedione (DHTD) unit. Among them, TTT-DHTD exhibits superior ORR performance with a half-wave potential (E_1/2) of 0.82 V vs RHE, approaching that of 20% Pt/C (0.85 V) and surpassing most reported metal-free COFs. It also demonstrates excellent methanol tolerance and long-term durability, maintaining activity over 120 hours. Density functional theory (DFT) calculations reveal that the donor-acceptor framework optimizes the p-band center, enhances charge separation, and improves adsorption of oxygenated intermediates, thereby accelerating ORR kinetics. This work provides a rational strategy for designing durable, high-performance metal-free electrocatalysts for sustainable energy applications.

PMID:
42647637
Bibliographic data and abstract were imported from PubMed on 27 Aug 2026.

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