单原子掺杂二硫化钼量子点的可控制备及析氢机制研究

在化石能源日渐枯竭、全球气候变暖等多重能源和环境问题的压力下，优化能源结构、发展清洁能源是当今化学工程及环境学科迫切需要解决的重大任务之一。氢能由于具有经济、高效和环境友好等优点，被认为是最具发展前景的清洁能源之一。但由于析氢催化剂主要依赖于资源稀缺的贵金属铂，严重阻碍了其商业化进程。为此，本项目拟采用“超重力+水热”法合成二硫化钼量子点载体 ，并创新性地采用超重力耦合等离子体技术原位制备金属单原子掺杂二硫化钼量子点催化剂，通过同时提高载体边缘和基面内活性S原子数来增强其催化活性，研究耦合的过程强化技术对反应环境均一性及载体表面负载机制的影响，实现均匀、稳定和高效析氢催化剂的可控制备；采用量子化学方法研究载体和金属原子的配位与分散规律，及其协同催化机制等，建立催化剂的结构特性和局域环境与电催化性能之间的本征构效关系，实现析氢催化剂的非铂金属替代，为加速氢能的商业化应用提供示范和科学基础。

With the fast depletion of fossil energy and the exacerbation of greenhouse effect, developing clean energy is an urgent task in chemical engineering and environment fields. It is believed that hydrogen energy is one of the promising clean energies, due to its high efficiency, stability and friendly environment. However, the hydrogen evolution reaction (HER) still strictly depends on precious Pt, which hinders the commercialization of hydrogen energy significantly. Therefore, in this project, we use the high-gravity technology coupled with plasma to synthesize metal single-atom doped MoS2 quantum dots catalysts, which have a large number of active sites not only on the edge also on the center of MoS2 carrier, contributing to the improvement of electrocatalytic activity. The effect of process intensification on the uniformity of reaction environment and loading mechanism is investigated. On the basis of these researches, the controllable preparation of homogeneous, stable and highly efficient electrocatalyst will be achieved. We also use the density functional theory (DFT) to systematically investigate the coordination, distribution pattern and synergistic catalytic mechanism of metal atom and its carrier, and further explore the effects of local bonding environments of non-precious metal single-atom catalysts and the intrinsic properties of substrates on the HER catalytic activity and stability，achieving the non-precious metal replacement to Pt in HER, which will speed up the development of hydrogen energy.