In-situ reconstructed Ru atom array on α-MnO2 with enhanced performance for acidic water oxidation
Chao Lin, Ji-Li Li, Xiaopeng Li, Shuai Yang, Wei Luo, Yaojia Zhang, Sung-Hae Kim, Dong-Hyung Kim, Sambhaji S. Shinde, Ye-Fei Li, Zhi-Pan Liu, Zheng Jiang & Jung-Ho Lee
Abstract
The development of acid-stable oxygen evolution reaction electrocatalysts is essential for high-performance water splitting. Here, we report an electrocatalyst with Ru-atom-array patches supported on α-MnO2 (Ru/MnO2) for the oxygen evolution reaction following a mechanism that involves only *O and *OH species as intermediates. This mechanism allows direct O–O radical coupling for O2 evolution. Ru/MnO2 shows high activity (161 mV at 10 mA cm−2) and outstanding stability with small degradation after 200 h operation, making it one of the best-performing acid-stable oxygen evolution reaction catalysts. Operando vibrational and mass spectroscopy measurements were performed to probe the reaction intermediates and gaseous products for validating the oxygen evolution reaction pathway. First-principles calculations confirmed the cooperative catalysis mechanism with a reduced energy barrier. Time-dependent elemental analysis demonstrated the occurrence of the in-situ dynamic cation exchange reaction during the oxygen evolution reaction, which is the key for triggering the reconstruction of Ru atoms into the ordered array with high durability.
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Time-dependent ICP-MS of the electrolyte is the control I’d add: 161 mV at 10 mA cm−2 and 200 h are not enough if Mn dissolution or Ru loss isn’t tracked, especially when the in-situ dynamic cation exchange is claimed as the key reconstruction step. Even a best-of AI tool list might help plot those traces, but it can’t replace 18O labeling to test the O–O radical coupling route.
Calling the O–O radical coupling the decisive step is too tidy. The 161 mV at 10 mA cm−2 and 200 h stability are strong, but operando mass spectroscopy only confirms gaseous products; it cannot rule out Mn dissolution or electrolyte impurities driving the in-situ cation exchange. Acid OER needs a value list for growing a garden of failure modes, not just one elegant pathway.