Ordered Intermetallic PdFe 3 N with Interstitial N Atoms on Porous Carbons for Efficient and Durable Hydrogen Production

Abstract Pd‐based dual‐metal site catalysts are active for the electrochemical water splitting for hydrogen production, while the slow hydrogen‐binding ability and sluggish hydrolysis‐dissociation kinetics of Pd‐based catalysts limit their practical application. Assisting with the Gel‐sol method, a complexation‐gel strategy is proposed to synthesize ordered PdFe 3 N transition metal nitrides on porous carbons (PdFe 3 N TMNs/C) with the long‐range ordered atomic arrangement, which accelerates water activation and dissociation. Moreover, interstitial N atoms in PdFe 3 N TMNs/C induce charge dilution and redistribution at the dual‐metal site, resulting in the optimization of the d‐band centers and enhancing the bonding strength, which is efficient and durable for the hydrogen evolution reaction (HER). As a result, the prepared coating achieves overpotentials of only 45 mV for the HER at 10 mA cm −2 in alkaline seawater electrolytes and exhibits excellent anion exchange membrane (AEM) performance and operates stably at a current density of 500 mA cm −2 at 1.76 V for 100 h. This work presents a new perspective for synthesizing TMNs nanocrystals and promotes their application in bifunctional electrocatalysts.