The electronic structure modulation through heterogeneous single-atom doping is an effective strategy to improve electrocatalysis performance of catalysts. Here, Ir single-atom doped RuO₂ (Ir_SA/RuO₂) is constructed by substituting Ru sites with mono-disperse Ir atoms in RuO₂ crystals. The Ir_SA/RuO₂-850 catalyst shows excellent activity for the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) in alkaline media, with overpotentials of only 37 and 234 mV respectively, at a current density of 10 mA cm⁻², lower than that of commercial Pt/C (39 mV-HER) and RuO₂ (295 mV-OER). Notably, no significant degradation occurs during the 1000 h HER stability test at 500 mA cm⁻². Furthermore, Ir_SA/RuO₂-850 also demonstrates superior catalytic activity and stability in acidic media. Theoretical calculations show that the interaction between Ir and RuO₂ modulates the electronic structure of both Ru and Ir sites, resulting in the lowest reaction energy barriers of Ru and Ir sites for the HER and OER, respectively, which thermodynamically explains the enhancement of the catalytic activity. Besides, the introduction of Ir atoms also enhances the demetallation energy of Ru atoms and strengthens the structural stability of the crystal, leading to the improved stability of the catalyst. This work provides an effective strategy for construction of high-performing catalysts by precisely controlling the electronic structure and active sites of polymetal atoms.

中文翻译：

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双活性位点介导的 Ir 单原子掺杂 RuO2 催化剂，用于高效稳定的水分解


通过非均相单原子掺杂进行电子结构调制是提高催化剂电催化性能的有效策略。这里，Ir单原子掺杂RuO ₂ (Ir _SA /RuO ₂ )是通过用RuO ₂晶体中的单分散Ir原子取代Ru位点而构建的。 Ir _SA /RuO ₂ -850催化剂在碱性介质中对析氢反应（HER）和析氧反应（OER）表现出优异的活性，在电流密度为10 mA cm时，过电势分别仅为37和234 mV ^-如图2所示，低于商业Pt/C(39mV-HER)和RuO ₂ (295mV-OER)。值得注意的是，在500 mA cm ^-2下进行1000小时HER稳定性测试期间没有发生明显的降解。此外，Ir _SA /RuO ₂ -850在酸性介质中也表现出优异的催化活性和稳定性。理论计算表明，Ir和RuO ₂之间的相互作用调节了Ru和Ir位点的电子结构，导致Ru和Ir位点分别对于HER和OER具有最低的反应能垒，这从热力学上解释了催化活性的增强。活动。此外，Ir原子的引入还增强了Ru原子的脱金属能，增强了晶体的结构稳定性，从而提高了催化剂的稳定性。 这项工作通过精确控制多金属原子的电子结构和活性位点，为构建高性能催化剂提供了有效的策略。