非化学计量过渡金属氧化物及其衍生物的制备及催化性能研究

Transition metal oxides and their derivatives have attracted extensive attention due to their potential application in the fields of electrocatalysis and energy storage. Especially, the non-stoichiometric transition metal oxides often present excellent catalytic activity because of its special structure and have a more important research value. Based on the previous research, this project aims to fabricate non-stoichiometric transition metal oxides and its derivatives through spray pyrolysis as main method and transition metal salt as raw material. Non-stoichiometric transition metal oxides and their derivatives will be obtained by means of element doping, atmosphere control and calcining process. In this project, we will systematically study the influence of pyrolysis temperature, atmosphere, calcining temperature and the ratio of raw material on the composition of material and active element oxidation state, so as to accomplish the regulation of the oxidation state on active element. Based on the preparation, the project will conduct the basic research on electrochemical performance of the obtained materials to explain the relationship between oxidation state of active elements and catalytic performance from the level of electron, and then get the connection among components, electronic structure and properties. In addition, based on the high yield of the preparation method, the obtained materials will be manufactured into corresponding electrochemical devices for performance estimation and some excellent electrode materials will be filtered out. Therefore, the research of this project is significant both in theory and practice.

过渡金属氧化物及其衍生物在电催化以及能量存储领域具有广阔的应用前景，已经引起了广泛关注，尤其是非化学计量过渡金属氧化物因其特殊的结构经常表现出优异的催化活性，具有更为重要的研究价值。在前期研究基础上，本项目拟采用喷雾热解法为制备方法，以过渡金属盐为原料，通过元素掺杂、气氛控制和煅烧工艺等手段获得非化学计量过渡金属氧化物及其衍生物。项目将系统研究热解温度、气氛、煅烧温度以及原料配比等工艺条件对材料组分和活性元素氧化态的影响，实现对活性元素平均氧化态的调控。在材料制备基础上，开展过渡金属氧化物及其衍生物电化学性能基础研究，从电子层面研究并解释活性元素氧化态与催化活性的关系，获得组分-电子结构-性质之间的关联性认识。此外，结合制备方法本身易量产的特点，将所得的材料加工成相应的电化学器件进行性能评价，筛选出一些性能优异的电极材料。因此，本项目的研究具有重要的理论意义和潜在应价值。

过渡金属氧化物及其衍生物在电催化以及能量存储领域具有广阔的应用前景，非化学计量过渡金属氧化物因其特殊的结构经常表现出优异的催化活性，具有更为重要的研究价值。项目围绕非化学计量过渡金属氧化物及其衍生物的制备及催化性能研究展开了系列研究。主要研究内容包括：.1.采用喷雾热解法制备了一系列过渡金属氧化物及其衍生物。系统探索了材料制备条件，对喷雾热解过程中混合氧化态的形成机理进行了探究，实现了材料的组分和元素氧化态的调控。.2.研究了工艺参数对材料形貌、元素氧化态的影响。实现了前驱物氧化深度的调控，并对产物的微观形貌进行优化，探索了组分变化对化合态的影响。.3.进行了材料的性能研究和应用探索。研究了产品催化性能，筛选出一批性能优异的催化材料。.4.研究了组分-电子态-性质关系。结合电子态的表征和理论模拟从氧化态调控、轨道能量等微观层面认识金属氧化物的组分-电子态-性能之间的关系。.在该项目经费的资助下，课题组在电催化以及能源材料领域取得了一系列研究成果，共发表学术论文24篇，申请发明专利4项，授权专利6项，并培养了一批研究生和本科生。

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