Baiutti F, Chiabrera F, Acosta M, Diercks D, Parfitt D, Santiso J, Wang X, Cavallaro A, Morata A, Wang H, Chroneos A, MacManus-Driscoll J, Tarancon A
Catalonia Institute for Energy Research (IREC), Jardins de Les Dones de Negre 1, Sant Adrià del Besòs, Barcelona, Spain.
Department of Materials Science and Metallurgy, University of Cambridge, Cambridge, UK.
Nat Commun. 2021 May 11;12(1):2660. doi: 10.1038/s41467-021-22916-4.
The implementation of nano-engineered composite oxides opens up the way towards the development of a novel class of functional materials with enhanced electrochemical properties. Here we report on the realization of vertically aligned nanocomposites of lanthanum strontium manganite and doped ceria with straight applicability as functional layers in high-temperature energy conversion devices. By a detailed analysis using complementary state-of-the-art techniques, which include atom-probe tomography combined with oxygen isotopic exchange, we assess the local structural and electrochemical functionalities and we allow direct observation of local fast oxygen diffusion pathways. The resulting ordered mesostructure, which is characterized by a coherent, dense array of vertical interfaces, shows high electrochemically activity and suppressed dopant segregation. The latter is ascribed to spontaneous cationic intermixing enabling lattice stabilization, according to density functional theory calculations. This work highlights the relevance of local disorder and long-range arrangements for functional oxides nano-engineering and introduces an advanced method for the local analysis of mass transport phenomena.
纳米工程复合氧化物的实现为开发一类具有增强电化学性能的新型功能材料开辟了道路。在此,我们报告了镧锶锰氧化物和掺杂二氧化铈垂直排列的纳米复合材料的实现,该材料可直接用作高温能量转换装置中的功能层。通过使用包括原子探针断层扫描结合氧同位素交换在内的互补先进技术进行详细分析,我们评估了局部结构和电化学功能,并直接观察了局部快速氧扩散途径。所得的有序介观结构以连贯、密集的垂直界面阵列表征,具有高电化学活性且抑制了掺杂剂偏析。根据密度泛函理论计算,后者归因于自发的阳离子混合实现了晶格稳定。这项工作突出了局部无序和长程排列对功能氧化物纳米工程的相关性,并引入了一种用于质量传输现象局部分析的先进方法。