原子层沉积制备钴镍硫化物薄膜的方法学研究及其在电催化方面的应用

硫化钴镍是一类重要的热点电催化材料，但目前并不清楚哪种晶相组成的硫化钴镍比性能最好。原子层沉积（ALD）技术是一种受到广泛看好的新型可控薄膜制备技术，它能够对薄膜的成分实现精确可控，并可将薄膜均匀包覆在复杂多孔结构上。本项目将利用ALD技术来系统地制备各种晶相组成的硫化钴镍薄膜，深入研究晶相组成对其电催化性能的影响并进行优化。因目前尚未有硫化钴镍的ALD方法报道，所以本项目的重点是研发一系列硫化钴镍的ALD可控制备方法。为此我们拟从前驱体的设计与合成开始，研发ALD工艺，并通过原位在线手段，深入探究ALD过程中的表面化学反应机理，实现对硫化钴镍制备方法的高度可控与可调性。最后，我们将优化后的ALD硫化钴镍薄膜均匀包覆在高表面积电极骨架结构上，从整体上提高电极的电催化性能。本研究不仅在ALD的基础方法学研究方面有重要的意义，而且这种分立优化骨架几何结构与表面性能的思路具有广泛的应用借鉴意义。

Cobalt nickel sulfides are an important hot-spot materials category for electrocatalysis, but it is still unknown which phase and stoichiometry of cobalt nickel sulfides is the best for electrocatalysis. Atomic layer deposition (ALD) technology has been widely regarded as a highly-promising, novel, and highly-controllable thin film deposition technology, as it can realize the precise control of film composition and thickness, and it can also be employed to uniformly coat complex porous structures. In this project, we will use ALD to systematically fabricate cobalt nickel sulfide films with various phases and compositions, and investigate and optimize the effect of phase and composition for their electrocatalytic performance. Since there is no currently existing ALD processes reported for cobalt nickel sulfides, the most important goal is to study and develop an ALD process for a series of cobalt nickel sulfides with high controllability. Therefore, we would like to first design and synthesize the precursors for cobalt and nickel, and then carefully develop the ALD process and study the surface chemistry reaction mechanisms by in-situ methods in the associated ALD process. These studies would help us to achieve the high controllability and adjustability for the ALD process. Finally, we will coat the optimized ALD cobalt nickel sulfide films uniformly on electrode frameworks with high surface areas, and thus the total electrocatalytic performance will be maximized. This study is not only meaningful from the fundamental ALD methodology point of view, but the idea of separately optimizing the geometry for the frameworks and the materials on the surface can also be widely applied to various other similar situations.