镍基硫化物的制备、结构调控与电催化水分解性能研究

Nickel sulfide is considered to be a low-cost nonprecious catalysts for the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) in the field of water splitting. However, significant challenges remain on the structure design, controllable preparation, revealing structure-activity relationship, and promotion of the catalytic activity. This project is going to explore the influence of the composition, crystal phase, and structure of nickel sulfides (NiS, Ni3S2, Ni3S4, etc.) on the electrocatalytic properties for HER and OER, and then obtain the orders of electrocatalytic activities and the relative rules between the structure and performance. Based on this, in order to promote the electrocatalytic performance and stability of nickel sulfides that have a better activity, morphological control (nano-laminated structure assembly) and the local electronic structure control (introduction of foreign metal element Zn or non-metal element Se) are proposed. The effects of the microstructure control and electronic structure regulation on the electrocatalytic activity are further invesigited. Then further elucidate the relationship between modified structure and activity to construct and prepare high active nickel sulfide based bifunctional electrocatalysts for HER and OER.

镍硫化合物可作为低成本非贵金属析氢、析氧双功能催化剂用于电解水，如何实现结构设计和可控制备以及揭示构效关系、提升催化性能仍然是重要课题。本项目拟通过可控合成一系列镍硫化物（NiS、Ni3S2、Ni3S4等），系统性探索镍硫化物组成、晶相、结构对催化氧析出和氢析出性能的影响，揭示结构与性能的关联规律和催化活性顺序；在此基础上，针对活性较优镍硫化物进行微结构形貌调控（多孔纳米叠片结构组装）和电子结构调控（引入第二金属元素Zn或非金属元素Se）来进一步提升其活性和稳定性。通过研究微结构调控和表面电子结构调控对电催化活性的影响机制，进一步阐明结构与性能之间的构效关系，实现高活性非贵金属镍硫基双功能催化剂的设计制备。

镍基硫属化合物由于其成本低廉、环境友好、导电性高可作为非贵金属析氢、析氧双功能催化剂用于电解水制氢。瞄准镍基硫属化合物在结构设计和可控制备方面欠缺、构效关系不明确、催化活性有待提高等重要问题，申请人通过结构设计，可控制备了一系列镍基硫属化物，系统性探索了镍基硫属化物结构对催化氧析出和氢析出性能的影响，揭示了结构与性能的关联规律和催化活性顺序；在此基础上，进一步针对活性较优的镍硒化物进行形貌微结构和电子结构调控，制备第二金属元素掺杂的多孔纳米叠片结构催化剂，从而提升了其催化活性和稳定性。通过研究这种形貌微结构调控和电子结构调控对电催化活性的影响机制，从而阐明了镍基硫属化物结构与性能之间的构效关系，为设计制备其他非贵金属电催化剂提供了理论指导。