XIn2S4(X=Co, Fe, Ni)纳米材料“多维度”构筑及外场调控析氢动力学研究

设计价格低廉、性能优异的新型催化剂，理解水分子在催化剂表面反应动力学过程，用于实现水分子高效裂解一直是氢能源获取领域的核心研究任务。当前催化剂设计主要基于“电子层面”考虑，即：忽略自旋相关电荷转移及轨道相互作用。如果“独辟蹊径”，理解并利用自旋态和电子态耦合作用协同优化析氢限速步骤，就可以为催化剂提供更多设计空间。基于此考虑，本项目从“自旋维度”出发利用可控原子杂化策略构筑一系列具有不同磁结构特性XIn2S4 (X=Co, Fe, Ni)纳米材料，利用光、电、磁等外场对材料自旋量子态进行可逆操控，结合原位光谱技术追踪并厘清电子态、自旋态及其耦合态对水分子反应动力学的调控机制，精确无误确立自旋态量子调控与析氢效率之间的普适规律，为新型“自旋”催化剂设计和“去耦合”析氢动力学研究提供理论依据。

Designing new types of catalysts with low cost and excellent performance and understanding the reaction kinetics process of water molecules on the catalyst surface has been the major researching task for exploiting hydrogen energy. However, current researches mainly focus on microstructure strategies based on electronic regulation but ignore the contribution of spin-related charge transfer and orbital interaction to the performance of catalysts. If we can find a new strategy that we can understand and use the coupling effect of spin state and electronic state to accelerate the hydrogen evolution reaction, which will provide more designs for the catalyst. Based on “spin dimension” consideration, we will construct XIn2S4 (X=Co, Fe, Ni) nanostructures with different magnetic configuration and regulate the distribution of spin carrier via external light field, electric field and magnetic field. Associated with in-situ spectral technology, we will disclose the contribution of electronic states and spin sates to hydrogen evolution reaction, respectively. Finally, the universal law between the quantum control of spin states and the efficiency of hydrogen evolution is accurately established, which can be used as a useful guide for designing new spin catalysts and understanding kinetics of decoupled hydrogen evolution reaction.