<p>Designing highly efficient acidic oxygen evolution reaction (OER) electrocatalysts that combine high activity, long-term stability, and low cost has become crucial for proton exchange membrane water electrolyzers. RuO<sub>2</sub> catalysts, following a kinetically favorable lattice oxygen mechanism, exhibit superior intrinsic activity but suffer from inferior stability for acidic OER. Current research predominantly focuses on sacrificing the intrinsic activity of RuO<sub>2</sub> to enhance stability. The activity-stability trade-off in RuO<sub>2</sub>-based catalysts remains a central research focus. Here, we propose a grain boundary engineering strategy to boost the OER activity and stability of RuO<sub>2</sub> in acidic media. Grain boundaries in RuO<sub>2</sub> catalysts do not alter the Ru valence state and Ru–O covalency, thus enabling grain boundary-rich RuO<sub>2</sub> catalysts (GB-RuO<sub>2</sub>) to follow the lattice oxygen mechanism pathway. We discover that grain boundaries can increase the content of coordinatively unsaturated Ru<sup>6+</sup> species and promote the deprotonation kinetics of adsorbed oxygen species, thus balancing acidic OER activity and stability. The optimal GB-RuO<sub>2</sub> catalysts achieve an exceptionally low acidic OER overpotential of 159 mV at 10 mA cm<sup>−2</sup> and a minor potential increase of 44 mV after 24 h at 50 mA cm<sup>−2</sup>, significantly surpassing RuO<sub>2</sub> catalysts with a low grain boundary.</p>

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Grain boundary in RuO2 to boost acidic oxygen evolution activity and stability

  • Qian Lu,
  • Xiaohong Zou,
  • Weixing Wu,
  • Ying Wang

摘要

Designing highly efficient acidic oxygen evolution reaction (OER) electrocatalysts that combine high activity, long-term stability, and low cost has become crucial for proton exchange membrane water electrolyzers. RuO2 catalysts, following a kinetically favorable lattice oxygen mechanism, exhibit superior intrinsic activity but suffer from inferior stability for acidic OER. Current research predominantly focuses on sacrificing the intrinsic activity of RuO2 to enhance stability. The activity-stability trade-off in RuO2-based catalysts remains a central research focus. Here, we propose a grain boundary engineering strategy to boost the OER activity and stability of RuO2 in acidic media. Grain boundaries in RuO2 catalysts do not alter the Ru valence state and Ru–O covalency, thus enabling grain boundary-rich RuO2 catalysts (GB-RuO2) to follow the lattice oxygen mechanism pathway. We discover that grain boundaries can increase the content of coordinatively unsaturated Ru6+ species and promote the deprotonation kinetics of adsorbed oxygen species, thus balancing acidic OER activity and stability. The optimal GB-RuO2 catalysts achieve an exceptionally low acidic OER overpotential of 159 mV at 10 mA cm−2 and a minor potential increase of 44 mV after 24 h at 50 mA cm−2, significantly surpassing RuO2 catalysts with a low grain boundary.