Nitrided Rhodium Nanoclusters with Optimized Water Bonding and Splitting Effects for pH‐Universal H₂‐Production

Abstract The nitridation of noble metals‐based catalysts to further enhance their hydrogen evolution reaction (HER) kinetics in neutral and alkaline conditions would be an effective strategy for developing high‐performance wide pH HER catalysts. Herein, a facile molten urea method is employed to construct the nitrided Rh nanoclusters (Rh_xN) supported on N‐doped carbon (Rh_xN‐NC). The uniformly distributed Rh_xN clusters exhibited optimized water bonding and splitting effects, therefore resulting in excellent pH‐universal HER performance. The optimized Rh_xN‐NC catalyst only requires 8, 12, and 109 mV overpotentials to reach the current density of 10 mA cm⁻² in 0.5 M H₂SO₄, 1.0 M KOH, and 1.0 M PBS electrolytes, respectively. The spectroscopic characterizations and theoretical calculation further confirm the vital role of Rh‐N moieties in Rh_xN clusters in improving the transfer of electrons and facilitating the generation of H₂. This work not only provides a suitable nitridation method for noble metal species in mild conditions but also makes a breakthrough in synthesizing noble metal nitrides‐based electrocatalysts to achieve an exceptional wide‐pH HER performance and other catalysis.