Structural properties and surface chemistry of nano structured electroactive materials

纳米结构的过渡金属氧化物体系，如金属尖晶石氧化物，由于其在广泛的电化学反应中的有用性和最近作为电池中的电极材料和燃料电池中的氧还原催化剂的应用，以及作为有趣的磁性材料、传感器和电容器的应用，已经重新受到关注。在这项研究计划中，我们将利用我们在电化学，表面科学和材料表征方面的专业知识来识别，量化和理解过渡金属氧化物（如AxB 3-xO 4，AxByCzOq）表面活性位点的作用，并研究这些金属阳离子的氧化还原性质在电化学反应中的作用，以建立可用于预测其性能的趋势和指导方针。我们计划的短期目标是识别，量化和理解过渡金属（M）-钴氧化物尖晶石（MxCo 3-xO 4）薄膜中活性位点的作用，M = Cu，Ni和Fe，x值范围从0到1，以及制备方法，退火和电极历史对材料结构，表面化学和相关性能的影响。这些材料将用于进行我们的第一个原位X射线吸收光谱（XAS）研究，更具体地说，原位X射线吸收近边结构（XANES）。使用这些材料，我们将确定它们的本体结构，包括阳离子类型及其化学环境，以及材料表面可能的相分离，确定它们如何形成和影响电化学反应。一旦获得了清楚的理解，将使用我们的方法以系统的方式研究附加掺杂剂在这些材料中的作用，以形成具有例如M，M' = Cu，Ni，Mn，Fe的（M）（M'）CoO 4尖晶石。基于它们的组成和结构，这些氧化物材料在多相催化、电极、气体和葡萄糖传感器、燃料电池和与H2燃料生产相关的光驱动水电解等领域中找到应用。

Nanostructured transition metal oxide systems such as metal spinel oxides have received renewed attention due to their demonstrated usefulness for a wide range of electrochemical reactions and recent applications as electrode materials in batteries and as oxygen reduction catalysts in fuel cells, but also as interesting magnetic materials, sensors, and capacitors. In this research program, we will use our expertise in electrochemistry, surface science and materials characterization to identify, quantify and understand the role of active sites at the surface of transition metal oxides (such as AxB3-xO4, AxByCzOq) and study the role that the redox properties of these metal cations have in electrochemical reactions to establish trends and guidelines that can be employed to predict their performance. The short terms objectives of our program are to identify, quantify and understand the role of active sites in transition metal (M)-cobalt oxide spinel (MxCo3-xO4) thin films with M = Cu, Ni and Fe and x values ranging from 0 to 1, as well as the effects of the preparation method, annealing and electrode history on the material's structure, surface chemistry and relevant properties. These materials will be used to perform our first in situ X-ray absorption spectroscopy (XAS) studies, more specifically in situ X-ray absorption near-edge structure (XANES). Using these materials, we will identify their bulk structures including types of cations and their chemical environments, as well as possible phase segregation at the surface of the materials, identifying how they form and affect electrochemical reactions. Once, a clear understanding is obtained the role of additional dopants in these materials will be investigated using our methodology to form (M)(M')CoO4 spinels with, for example, M, M' = Cu, Ni, Mn, Fe, in a systematic way. Based on their composition and structure, these oxide materials find applications in areas such as heterogeneous catalysis, electrode, gas and glucose sensors, fuel cells and photo driven electrolysis of water relevant to the production of H2 fuel.