For acid–water oxidation, pyrochloric ruthenates are thought to be extremely effective electrocatalysts. In this work, through partial B-site replacement with larger M²⁺ cations, the electronic states of Y₂Ru₂O₇ with strong electron correlations are reasonably managed, by which the inherent performance is tremendously promoted. Based on this, the improved Y₂Ru_1.9Sr_0.1O₇ electrocatalyst exhibits an outstanding durability and presents a highly inherent mass activity of 1915.1 A g_Ru^–1 (at 1.53 V vs RHE). The enhanced oxygen-evolving reaction (OER) activity by ionic dopant in YRO pyrochlore can be attributed to two aspects, i.e., the lattice distortion induced inhibition of the grain coarsening, which results in a large surface area for YRO-M and increases the OER active sites, and the weakening of electron correlation via broadening of the Ru 4d bandwidths due to the increase of the average radius of B-site ions, which gives rise to an enhancement of conductivity and a strengthened hybridization between Ru 4d and O 2p orbitals and improves the reaction kinetics. The synergistic effects of lattice distortion and orbital hybridization promote the enhanced OER activity. The results would provide fresh concepts for the design of improved electrocatalysts and underscore the significance of managing the intrinsic performance through the dual modification of microstructure morphology and electronic structure.

中文翻译：

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烧绿石 Y2Ru2O7 中离子掺杂剂诱导的晶格畸变和轨道杂化促进酸水氧化

对于酸水氧化，烧氯钌酸盐被认为是极其有效的电催化剂。本工作通过用较大的M ^{2+阳离子取代部分B位，合理地管理了具有强电子相关性的Y} ₂ Ru ₂ O ₇的电子态，从而极大地提升了其固有性能。基于此，改进的Y ₂ Ru _1.9 Sr _0.1 O _{7电催化剂表现出出色的耐久性，并呈现出1915.1 A g Ru} ^–1的高度固有质量活性（在1.53 V vs RHE下）。 YRO烧绿石中离子掺杂剂增强的析氧反应（OER）活性可归因于两个方面，即晶格畸变诱导抑制晶粒粗化，这导致YRO-M具有较大的表面积并增加了OER由于 B 位离子平均半径的增加，Ru 4d 带宽变宽，从而削弱了电子相关性，从而增强了电导率，并增强了 Ru 4d 和 O 2p 轨道之间的杂化改善反应动力学。晶格畸变和轨道杂化的协同效应促进了OER活性的增强。研究结果将为改进的电催化剂的设计提供新的概念，并强调通过微观结构形态和电子结构的双重修饰来管理内在性能的重要性。