Congratulations to Yue Mao for his paper accepted by Applied Catalysis B: Environment and Energy!
The development of efficient and durable electrocatalysts for the ammonia oxidation reaction (AOR) is critical for practical hydrogen production via anion exchange membrane ammonia electrolysis (AEMAE). Herein, we show that a simple sulfur (S)-doping strategy triggers the gradient surface reconstruction for Ni–Cu layered double hydroxide (Ni0.8Cu0.2 LDH) to enhance the performance of AOR. In situ Raman spectroscopy and various ex situ characterizations further reveal that after electrochemical activation, the S-Ni0.8Cu0.2 LDH accumulates more high-valence species on the surface, which lowers the formation potential of S-Ni0.8Cu0.2OOH as active centers, thereby accelerating AOR kinetics. Density functional theory calculations elucidate that S-doping catalyst reduces the energy barriers of both dehydrogenation and rate-determining step (*NH3 → *NH2). In particular, the S-Ni0.8Cu0.2 LDH can serve as self-standing catalytic electrode for AEMAE, achieving the industrial current density of 500 mA cm–2 at a cell voltage of no more than 2.0 V, and operating stably for 100 h. This study offers valuable insights into the dynamic surface reconstruction, thereby providing a guideline for developing advanced AOR catalysts with superior performance.
