posted on 2025-05-08, 03:43authored byCi Lin, Tsung-Yi Chen, Tao Zhou, Yingqiang Wu, Ching Kit Tommy Wun, Weicheng Chen, Han-Yi Chen, Vincent Tung, Zhengxiao Guo, Tsz Woon Benedict Lo, Liang Cai, Yida Deng, Philip C. Y. Chow
Regulating the oxygen evolution reaction (OER) mechanism
presents
a promising yet challenging approach to address the performance-stability
trade-off of acidic water oxidation catalysts. Here we demonstrate
the regulation of the OER mechanism through in situ surface reconstruction
of manganese oxybromides (MOB) catalysts modified with single-atom
ruthenium (Ru-MOB). In situ Raman spectroscopy reveals that Ru incorporation
intensifies the inherent, reversible surface reconstruction of MOB,
resulting in the formation of a γ-MnO2 layer with
an onset potential approximately 100 mV lower. Various operando/in
situ characterizations and theoretical calculations show that the
reconstructed Ru-MOB significantly suppresses the lattice oxygen mechanism
while simultaneously enhancing the adsorbate evolution mechanism.
In an electrochemical cell, the reconstructed Ru-MOB drives acidic
OER with an overpotential about 90 mV lower at 10 mA cm–2 compared to pure MOB, and it shows negligible performance degradation
for over 1400 h. Our work offers a design strategy for the future
development of acidic OER catalysts.