Fan Bai , Jonas Schulwitz , Tatiana Priamushko , Ulrich Hagemann , Aleksander Kostka , Markus Heidelmann , Serhiy Cherevko , Martin Muhler , Tong Li
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引用次数: 0
摘要
开发高效的氧进化反应（OER）电催化剂需要深入了解结构-活性-稳定性关系，最好是在原子尺度上。在此，我们采用原子探针断层扫描和透射电子显微镜揭示了在 OER 过程中 LaCoO3 和掺钙 LaCoO3 表面的组成和结构变化。我们发现原始包晶的最顶端表面由 A 位元素（La）终止。在 OER 之后，LaCoO3 表面会形成无定形的 La(OH)3，从而导致活性显著下降。对于掺 Ca 的 LaCoO3，观察到氢氧根离子的插层和渗透增强，同时出现了 Co3+/4+ 氧化还原对，这有助于增强其 OER 活性和稳定性。我们的研究证明了电催化剂表面原子尺度的组成和结构细节如何加深我们对其活性和稳定性的理解。
Correlating atomic-scale structural and compositional details of Ca-doped LaCO3 perovskite nanoparticles with activity and stability towards the oxygen evolution reaction
Developing efficient oxygen evolution reaction (OER) electrocatalysts requires a thorough understanding of structure–activity-stability relationships, ideally at the atomic scale. Herein, we employed atom probe tomography and transmission electron microscopy to reveal compositional and structural changes on LaCoO3 and Ca-doped LaCoO3 surfaces during OER. We reveal that the topmost surfaces of pristine perovskite are terminated by the A-site element (La). After OER, amorphous La(OH)3 is formed on the surfaces of LaCoO3, which leads to significant activity deterioration. For Ca-doped LaCoO3, enhanced intercalation and penetration of hydroxide ions, along with the appearance of Co3+/4+ redox couple, are observed, contributing to its enhanced OER activity and stability. Our study demonstrates how atomic-scale compositional and structural details of electrocatalyst surfaces deepen our understanding of their activity and stability.
期刊介绍：
The Journal of Catalysis publishes scholarly articles on both heterogeneous and homogeneous catalysis, covering a wide range of chemical transformations. These include various types of catalysis, such as those mediated by photons, plasmons, and electrons. The focus of the studies is to understand the relationship between catalytic function and the underlying chemical properties of surfaces and metal complexes.
The articles in the journal offer innovative concepts and explore the synthesis and kinetics of inorganic solids and homogeneous complexes. Furthermore, they discuss spectroscopic techniques for characterizing catalysts, investigate the interaction of probes and reacting species with catalysts, and employ theoretical methods.
The research presented in the journal should have direct relevance to the field of catalytic processes, addressing either fundamental aspects or applications of catalysis.
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