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Selective and Long-Term Stable Ammonia Electrolysis Using Pt-WOx Catalysts with Suppressed NOx Formation and Enhanced
Changhyun Lim1,2, Hyogyun Roh1,2, Hyeon Kim3
1Surface Chemistry Laboratory of Electronic Materials (SCHEMA), Department of Chemical Engineering, Pohang University of Science and Technology (POSTECH), Pohang, 37673, Republic of Korea.
Abstract:
Ammonia electrolysis presents a promising strategy for low-voltage hydrogen production; however, its advancement is impeded by limitations in electrocatalyst performance due to sluggish reaction kinetics and deactivation caused by strongly adsorbed nitrogen-containing intermediates. In this study, a photodeposited Pt on tungsten suboxide (WOx) nanowires (Pt-WOx (P)) is introduced as a bifunctional electrocatalyst for ammonia electrolysis. The photodeposition induces strong metal-support interaction, resulting in robust interfacial bonding between Pt and WOx and facilitating electron transfer from WOx to Pt. ATR-SEIRAS (attenuated total reflection-surface enhanced infrared absorption spectroscopy) identifies the Gerischer-Mauerer (G-M) mechanism through absorbance peaks corresponding to NH2 and NxHy (x = 1-2) and reveals effective suppression of NOx poisoning on Pt-WOx (P). DFT confirms the electronic modulation of Pt significantly lowers the energy barrier of the rate-determining step (RDS) for the conversion of *NH2 to *NH by enhancing hydrogen bonding of *NH and *OH. As a result, Pt-WOx (P) exhibits outstanding AOR activity, achieving a high peak current density of 49.69 mA cm-2. Furthermore, it demonstrates remarkable stability for over 120 h during ammonia electrolysis. In an MEA-based flow cell, Pt-WOx (P) delivers current densities exceeding 500 mA cm-2, underscoring its potential as a bifunctional catalyst for ammonia electrolysis applications.
