基于单层磷掺杂二硫化钼高效析氢催化剂的可控合成及其构效关系研究

Hydrogen as an energy carrier has advantages such as clean, renewable, high energy density and abundant sources, which has made it the most important parts of the national energy system. To develop a distributed hydrogen production strategy, electrocatalysis using non-precious metal to substitute the expensive and scarce platinum-based catalysts provides a cost-effective approach. Taking advantage of the unique electronic properties of monolayer molybdenum disulfide and the perturbation of energy level through heteroatom doping, here we propose developing a new approach for the synthesis of monolayer phosphorous-doped molybdenum disulfide with controllable properties, including the size, edge abundance, and elemental compositions. By using techniques such as scanning transmission electron microscopy and density functional theory, we aim to quantify the hydrogen evolution activity at the basal plane and edge sites and elucidate the correlation between catalyst structure and electron transport kinetics. The structure-activity relationship will then be used for the rational design of phosphorous-doped molybdenum disulfide/graphene hybrid materials for the cost-effective production of hydrogen. The project will be an important advancement of non-precious-metal-based hydrogen evolution catalysts that could inspire the rational design and optimization of two-dimensional catalysts.

氢能是一种清洁的可再生能源，具有高热值、来源广等优势，是国家能源体系的重要组成部分。降低电化学制氢成本，包括对非贵金属析氢催化剂的研发，以取代昂贵、低丰度的金属铂催化剂，是推广其分布式产氢的可行性方案之一。基于单层二硫化钼的独特电子结构和异元素掺杂的轨道干扰效应，本项目拟开发一种磷掺杂单层二硫化钼的可控性合成方法，包括对尺寸大小、边界丰度、元素成分等性质的准确调控。通过利用扫描透射电子显微镜、密度泛函理论等表征、分析手段，量化磷掺杂二硫化钼的基平面、边界的不同催化位点的析氢活性，探索催化剂结构与电子传输的动力学关系；通过构建构效关系，合理设计磷掺杂二硫化钼/石墨烯复合材料，实现低廉、高效制氢。本项目是非贵金属析氢催化剂的重要研究进展，为二维材料催化剂的合理设计和性能优化提供了技术支撑。

氢能是一种清洁的可再生能源，具有高热值、来源广等优势，是国家能源体系的重要组成部分。降低电化学制氢成本，包括对非贵金属析氢催化剂的研发，以取代昂贵、低丰度的金属铂催化剂，是推广其分布式产氢的可行性方案之一。基于单层二硫化钼的独特电子结构和异元素参杂的轨道干扰效应，本项目开发一种少层磷参杂二硫化钼的可控性合成方法，包括对尺寸大小、元素成分等性质的准确调控。通过利用扫描透射电子显微镜、密度泛函理论等表征、分析手段，量化磷参杂二硫化钼的基平面、边界的不同催化位点的析氢活性，探索催化剂结构与电子传输的动力学关系；通过构建构效关系，合理设计磷参杂二硫化钼/石墨烯复合材料，实现低廉、高效制氢。本项目是非贵金属析氢催化剂的重要研究进展，为二维材料催化剂的合理设计和性能优化提供了技术支撑。