磁场调控Ni-Mn基铁磁形状记忆合金电子结构对催化析氧性能影响的研究

理解催化剂电子结构与催化活性之间的关联，是澄清电催化机制和提高能源转换存储效率的关键。Ni-Mn基铁磁形状记忆合金是一类优良的电催化析氧材料，在磁场作用下可驱动其逆马氏体相变，改变自旋态和轨道电子占据态。这就为开展磁场原位调控电子结构对电催化性能影响的研究提供了一个理想的平台。本项目中，我们将以Co掺杂的Ni-Mn-X（X=Ti、In、Sn）为研究对象，研究磁场原位驱动对其OER性能的影响。在理论计算马氏体相和奥氏体相的电子结构基础上，结合理论模拟电催化过程的热力学信息，确定电子结构变化对催化界面化学吸附作用的影响，澄清电子结构与催化活性间的关联，揭示磁场调控催化活性的物理机制，为获得高性能的过渡金属基电催化剂提供实验与理论依据。

Understanding the relationship between electronic structure and electrocatalytic activity is crucial to clarify electrocatalytic mechanism and improve energy conversion and storage efficiency. Ni-Mn based ferromagnetic shape memory alloys have been considered as one efficient electrocatalysts for oxygen evolution reaction. And their electronic structure such as spin state and electron occupancy of orbitals would be altered during magnetic-field-induced reverse martensitic transformation. Therefore, they can provide an ideal platform for the investigation of the influence of the in situ magnetic-field-manipulated electronic structure on oxygen electrocatalytic activity. Herein, we will select Co-doped Ni-Mn-X (X=Ti, In, and Sn) as the research object, and carry out the study of how oxygen electrocatalytic activity is affected by in situ applied magnetic field. On the basis of the electronic structures calculated theoretically for martensite and austenite, and the thermodynamic information simulated theoretically in their electrocatalytic process, the effect of the electronic structure change on the chemisorption in catalytic interface can be revealed. Further, we can clarify the internal relationship between electronic structure and electrocatalytic activity, and expound the physical mechanism of the magnetic field control of oxygen electrocatalytic activity, thus providing experimental and theoretical reference for the acquirement of transition-metal-based electrocatalyst with excellent activity.