RhRu3Ox对酸性水氧化的温度依赖机理演化。

IF 15.7 1区综合性期刊 Q1 MULTIDISCIPLINARY SCIENCES

Nature Communications Pub Date : 2025-10-20 DOI:10.1038/s41467-025-64286-1

Ming-Rong Qu,Heng Liu,Si-Hua Feng,Xiao-Zhi Su,Jie Xu,Heng-Li Duan,Rui-Qi Liu,You-Yi Qin,Wen-Sheng Yan,Sheng Zhu,Rui Wu,Hao Li,Shu-Hong Yu

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引用次数: 0

摘要

析氧反应作为许多电化学器件的阳极反应，在能量转换中起着至关重要的作用。然而，非铱基材料在析氧反应中的稳定性不足严重限制了该类器件的大规模应用。本文利用自制的operando微分电化学质谱系统，揭示了RhRu3Ox在析氧过程中具有温度依赖性的机制演化效应，突出了温度在触发机制演化中的作用。这一效应丰富了通路操作的策略。由于不同的动力学途径可以影响催化剂的稳定性，这一发现表明，温度依赖的途径调节可以作为优化稳定性的方法。为了评估RhRu3Ox在实际应用中的潜力，我们将其组装到质子交换膜电解槽中，并在200 mA cm-2的电流密度下证明其在室温下超过1000小时的稳定性。密度泛函理论研究表明，与晶格氧活化相关的动力学屏障的存在可能是RhRu3Ox在高温下观察到的温度依赖行为的原因。

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Temperature-dependent mechanism evolution on RhRu3Ox for acidic water oxidation.

The oxygen evolution reaction, as the anodic reaction of many electrochemical devices, plays a crucial role in energy conversion. However, the insufficient stability of non-iridium-based materials during the oxygen evolution reaction has severely limited the large-scale application of such devices. Here, using a home-made operando differential electrochemical mass spectrometry system, we show a temperature dependent mechanism evolution effect of RhRu3Ox in the oxygen evolution process, which highlights the role of temperature in triggering mechanism evolution. This effect enriches the strategies for pathway manipulation. Since different kinetic pathways can influence catalyst stability, this finding suggests that temperature-dependent pathway regulation may serve as an approach to optimize stability. To evaluate the potential of RhRu3Ox for practical applications, we assemble it into a proton exchange membrane electrolyzer and demonstrate its stability at room temperature for over 1000 hours at a current density of 200 mA cm-2. Density functional theory studies suggest that the existence of a kinetic barrier related to lattice oxygen activation might be the reason for the observed temperature dependent behavior of RhRu3Ox at elevated temperatures.

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来源期刊

Nature Communications Biological Science Disciplines-

CiteScore

24.90

自引率

2.40%

发文量

6928

审稿时长

3.7 months

期刊介绍： Nature Communications, an open-access journal, publishes high-quality research spanning all areas of the natural sciences. Papers featured in the journal showcase significant advances relevant to specialists in each respective field. With a 2-year impact factor of 16.6 (2022) and a median time of 8 days from submission to the first editorial decision, Nature Communications is committed to rapid dissemination of research findings. As a multidisciplinary journal, it welcomes contributions from biological, health, physical, chemical, Earth, social, mathematical, applied, and engineering sciences, aiming to highlight important breakthroughs within each domain.