The Synergistic Effect of Pyrrolic-N and Pyridinic-N with Pt Under Strong Metal-Support Interaction to Achieve High-Performance Alkaline Hydrogen Evolution

Developing high-performance Pt-based catalysts with strong metal-support interaction (SMSI) is significant for hydrogen production by water electrolysis working at high current density conditions, but still challenging. Herein, Pt/X-NCNT (X = 4, 8, 12, 16) with SMSI is designed and developed by combining the advantages of Platinum-based catalysts and nitrogen-doped carbon material. In-situ and ex-situ experiments and density functional theory simulations illustrate that the Gibbs free energies (Delta G) of reaction intermediates (H2O*, OH*, H*) are optimized by the synergistic effect of various N functional groups and Pt under SMSI. The Pt/8-NCNT only needs overpotentials of 17, 107, and 153 mV to reach current densities of 10, 500, and 1000 mA cm(-2). Concurrently, the Pt/8-NCNT exhibits brilliant stability after 100 h current-time (i-t) tests at 500 mA cm(-2). More importantly, this work demonstrates the function of pyrrolic-N and pyridinic-N in the reaction, and provides new ideas for the design of advanced SMSI electrocatalysts for various electrochemical and catalytic applications.

Automated summary

This study successfully develops Pt/X-NCNT (X = 4, 8, 12, 16) catalysts with strong metal-support interaction (SMSI), which shows significant potential for hydrogen production by water electrolysis at high current density conditions. In-situ and ex-situ experiments and density functional theory simulations reveal the synergistic effect of various nitrogen functional groups and Pt under SMSI, optimizing the Gibbs free energies of reaction intermediates.