LAUSR

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 (ΔG) 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.