Effectiveness of strain and dopants on breaking the activity-stability trade-off of RuO(2) acidic oxygen evolution electrocatalysts

应变和掺杂剂对打破RuO(2)酸性析氧电催化剂活性-稳定性权衡的有效性

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Abstract

Ruthenium dioxide electrocatalysts for acidic oxygen evolution reaction suffer from mediocre activity and rather instability induced by high ruthenium-oxygen covalency. Here, the tensile strained strontium and tantalum codoped ruthenium dioxide nanocatalysts are synthesized via a molten salt-assisted quenching strategy. The tensile strained spacially elongates the ruthenium-oxygen bond and reduces covalency, thereby inhibiting the lattice oxygen participation and structural decomposition. The synergistic electronic modulations among strontium-tantalum-ruthenium groups both optimize deprotonation on oxygen sites and intermediates absorption on ruthenium sites, lowering the reaction energy barrier. Those result in a well-balanced activity-stability profile, confirmed by comprehensive experimental and theoretical analyses. Our strained electrode demonstrates an overpotential of 166 mV at 10 mA cm(-2) in 0.5 M H(2)SO(4) and an order of magnitude higher S-number, indicating comparable stability compared to bare catalyst. It exhibits negligible degradation rates within the long-term operation of single cell and PEM electrolyzer. This study elucidates the effectiveness of tensile strain and strategic doping in enhancing the activity and stability of ruthenium-based catalysts for acidic oxygen evolution reactions.

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