Boosting the Performance of Pt/C Catalysts via Nitrogen‐Doped Carbon Support: Insights from Structural and Electrochemical Characterization
Yulia Bayan, E. R. Beskopylny, E. Yu. Gerasimov, Egor E. Aydakov, K.K. Volik, Ilya Pankov, Ilya V. Chepkasov, Mikhail M. Lukanov, Alexander G. Kvashnin, А. А. Алексеенко
Abstract
Nitrogen-doped carbon supports enhance platinum electrocatalysts for proton exchange membrane fuel cells (PEMFCs). This study demonstrates a rapid melamine-assisted N-doping method for conductive carbon black (Ketjenblack EC600JD), producing a high-loading (≈40 wt.% Pt) catalyst with exceptional activity and durability. X-ray photoelectron spectroscopy confirms successful N-incorporation. Microscopy reveals uniform Pt nanoparticles (2.5-3 nm) and atomic Pt clusters on the N-doped support, attributed to strong Pt-N interactions. Density functional theory (DFT) calculations highlight the critical role of pyridinic-N defects in stabilizing atomic Pt, enhancing activity via charge transfer, and improving stability via strong Pt anchoring. Electrochemically, Pt/KB-600-N achieves twice the mass activity of commercial HiSPEC4000. After accelerated stress testing, it shows only a 15% electrochemical surface area (ESA) loss versus 35% for undoped Pt/KB-600. Enhanced stability correlates with pyridinic/graphitic N species mitigating carbon corrosion and Pt detachment. Binding energy analysis and cluster models quantify the Pt-support interaction, revealing N-doping increases Pt adhesion energy by 20-30% compared to pristine carbon. This work establishes a rational design strategy for high-performance Pt-based electrocatalysts by leveraging nitrogen-doped carbon supports, offering fundamental insights into the critical role of Pt-N interactions in enhancing both activity and durability for PEMFC applications.