用第一性原理法揭示Ru基高熵氧化物在析氧反应中的稳定性机制

IF 2.9 4区工程技术 Q1 MULTIDISCIPLINARY SCIENCES

Advanced Theory and Simulations Pub Date : 2025-05-15 DOI:10.1002/adts.202500218

Zhizhao Zhang, Jice Li, Hui Liu, Jiaxing Wang, Limin Liang, Ying Li

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引用次数: 0

摘要

实验报道，钌基高熵氧化物（Ru - HEO）在酸性析氧反应（OER）中表现出比RuO2更高的稳定性和耐久性。然而，潜在的稳定机制仍不清楚。本文首先研究了Ru - HEO和RuO2的表面状态作为外加电位和pH的函数，以阐明在OER电催化条件下Ru活性位点的中毒或氧化。随后，计算了各种Ru - HEO表面态上氧空位的形成能，这些空位通常与晶格氧氧化机制导致的结构不稳定性有关。结果表明，金属原子在Ru - HEO中的存在加强了Ru─O键，可能有助于Ru - HEO OER催化剂的长期稳定性。这项工作通过与RuO2的比较，为Ru - HEO稳定性的起源提供了见解。

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Unraveling the Stability Mechanism of Ru‐Based High‐Entropy Oxides for Oxygen Evolution Reactions by the First‐Principles Method

It has been experimentally reported that Ru‐based high‐entropy oxides (Ru‐HEO) exhibit higher stability and durability in acidic oxygen evolution reaction (OER) compared to RuO2. However, the underlying stability mechanism remains unclear. Herein, the surface states of Ru‐HEO and RuO2 are first studied as a function of applied potential and pH to elucidate the poisoning or oxidation of Ru active sites under OER electrocatalytic conditions. Subsequently, the formation energies of oxygen vacancies on various Ru‐HEO surface states are calculated, which are typically associated with structural instability due to the lattice oxygen oxidation mechanism. The results indicate that the presence of metal atoms in Ru‐HEO strengthens the Ru─O bond, possibly contributing to the long‐term stability of Ru‐HEO OER catalysts. This work provides insights into the origin of Ru‐HEO stability by comparison with RuO2.

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来源期刊

Advanced Theory and Simulations Multidisciplinary-Multidisciplinary

CiteScore

5.50

自引率

3.00%

发文量

221

期刊介绍： Advanced Theory and Simulations is an interdisciplinary, international, English-language journal that publishes high-quality scientific results focusing on the development and application of theoretical methods, modeling and simulation approaches in all natural science and medicine areas, including: materials, chemistry, condensed matter physics engineering, energy life science, biology, medicine atmospheric/environmental science, climate science planetary science, astronomy, cosmology method development, numerical methods, statistics