Graphene Framework Pillared by Co-Metalated Porphyrin Linker as CO₂ Reduction Electrocatalyst.

Authors

Faruk Ahamed Rahimi, Soumitra Barman, Tamagna Mandal, Rohan Jena, Anupam Dey, Adrija Ghosh, Debabrata Samanta, Ritu Dahiya, Ravi Kumar, Sourav Maji, Surendra Kumar Makineni, Dibyendu Bhattacharyya, Tapas Kumar Maji

Published in

Small (Weinheim an der Bergstrasse, Germany). Pages e75653. Sep 10, 2026. Epub Sep 10, 2026.

Abstract

Developing low-cost, efficient, and durable electrocatalysts for CO₂ conversion remains a significant challenge. Herein, we report a Co-metalated porphyrinic pillared graphene framework (Co-P-PGF) that functions as a single-atom catalyst (SAC) for efficient electrochemical CO₂ reduction. The framework was synthesized via Sonogashira-Hagihara coupling between Co-porphyrin linkers and iodobenzene-functionalized reduced graphene oxide (rGO), alongside a metal-free analogue (P-PGF). The atomically dispersed Co(II) centers serve as active sites for CO₂ binding and activation, while the conductive rGO sheets facilitate rapid electron transport and efficient charge transfer at the electrode-electrolyte interface. Owing to the integrated conductive graphene architecture, Co-P-PGF exhibits excellent intrinsic electrocatalytic activity without requiring additional conductive carbon additives. The catalyst achieves a remarkable Faradaic efficiency for CO production (FE_CO = 94.07%) in aqueous electrolyte in an H-cell configuration. Furthermore, operation in a flow cell results in a six-fold enhancement in current density compared to the H-cell. Operando DRIFTS, Raman spectroscopy, and X-ray absorption spectroscopy, complemented by density functional theory calculations, reveal the nature of the active sites and reaction intermediates during CO₂ reduction. These results highlight the promise of graphene-based SACs as cost-effective, sustainable, and high-performance catalysts for electrochemical CO₂ reduction reaction (CO₂RR).

PMID:
42723410
Bibliographic data and abstract were imported from PubMed on 11 Sep 2026.

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