Sustainable Synthesis of Edge-Dominant Pyridinic Nitrogen-Doped Carbon from Tannic Acid for High-Performance Vanadium Redox Flow Batteries

Abstract

A novel carbon material with edge-dominant pyridinic nitrogen doping is synthesized from tannic acid (TA), an agricultural byproduct, using a quick and straightforward two-step microwave irradiation technique. Tris(2-aminoethyl)amine (TAEA) plays a dual role in this process, acting as a condensing agent for TA in the initial step and providing nitrogen for the pyridinic structure in the second step. This approach results in a distinctive carbon structure (C–TA/TAEA) characterized by enhanced graphitic features, fewer imperfections, and similar hydrophilicity. The edge pyridinic configuration lowers the desorption energy of V³⁺ complexes and the deprotonation energy of VO²⁺ complexes, thereby boosting the catalytic activity for vanadium ion redox reactions (VIRR) by influencing the rate-limiting steps of both positive and negative side VIRRs. When applied to commercial thermal-treated graphite felt (T-GF/[C-TA/TAEA]), the material demonstrates stable performance during vanadium redox flow battery (VRFB) single cell testing, even at 500 mA cm⁻², showing improved energy efficiency (EE) and discharge capacity compared to T-GF. Furthermore, when applied to pristine graphite felt (GF/[C–TA/TAEA]), the material maintains a 94.12% discharge capacity retention rate over 1000 cycles at 400 mA cm⁻², underscoring its potential as an eco-friendly, energy-efficient treatment method for producing VRFB electrodes.

Keywords

graphitic carbon / microwave / tannic acid / tris(2-aminoethyl)amine / vanadium redox flow battery

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