Two-dimensional (2D) transition metal dichalcogenides (TMDCs) have attracted tremendous interest as functional materials due to their exceptionally diverse and tunable properties, especially in their edges. In addition to the conventional armchair and zigzag edges common to hexagonal 2D materials, more complex edge reconstructions can be realized through careful control over the synthesis conditions. However, the whole family of synthesizable, reconstructed edges remains poorly studied. Here, we develop a computational approach integrating ensemble-generation, force-relaxation, and electronic-structure calculations to systematically and efficiently discover additional reconstructed edges and screen their functional properties. Using MoS₂ as a model system, we screened hundreds of edge-reconstruction to discover over 160 reconstructed edges to be more stable than the conventional ones. More excitingly, we discovered nine new synthesizable reconstructred edges with record thermodynamic stability, in addition to successfully reproducing three recently synthesized edges. We also find our predicted reconstructed edges to have multi-functional properties—they show near optimal hydrogen evolution activity over the conventional edges, ideal for catalyzing hydrogen-evolution reaction (HER) and also exhibit half-metallicity with a broad variation in magnetic moments, making them uniquely suitable for nanospintronic applications. Our work reveals the existence of a wide family of synthesizable, reconstructed edges in 2D TMDCs and opens a new materials-by-design paradigm of ‘intrinsic’ edge engineering multifunctionality in 2D materials.

二维（2D）过渡金属二硫化碳（TMDC）由于其特别多样化和可调节的特性（尤其是在其边缘）而作为功能材料引起了极大的兴趣。除了六角形2D材料常用的常规扶手椅和锯齿形边缘外，可以通过仔细控制合成条件来实现更复杂的边缘重建。但是，整个可合成的，重建的边缘家族仍然研究不足。在这里，我们开发了一种集成集合生成，力松弛和电子结构计算的计算方法，以系统有效地发现其他重建边缘并筛选其功能特性。使用MoS ₂作为模型系统，我们筛选了数百个边缘重建，以发现160多个重建边缘比传统边缘更稳定。更令人兴奋的是，除了成功地复制了三个最近合成的边缘外，我们还发现了九个具有可记录的热力学稳定性的可合成的新重建边缘。我们还发现预测的重构边缘具有多功能特性-与常规边缘相比，它们具有接近最佳的析氢活性，是催化氢演化反应（HER）的理想选择，并且具有半金属性，且磁矩变化很大，使它们特别适合于纳米自旋电子学应用。我们的工作揭示了广泛的可合成的家族的存在，