Two-dimensional (2D) transition metal dichalcogenides (TMDCs) have attracted tremendous interest as functional materials due to their exceptionally diverse and tunable catalytic, electronic, and magnetic properties, especially at their edges. Till date only the conventional armchair and zigzag edges of hexagonal 2D materials have been studied. Recently, more complex edge reconstructions have been experimentally discovered serendipitously. This poses an intriguing question: what is the whole family of synthesizable reconstructed edges and what are they good for? Here, we develop a high-throughput ab initio based predictive computational approach, integrating ensemble-generation, force-relaxation and electronic-structure calculations to efficiently demonstrate existence of a wide family of stable and synthesizable reconstructed 2D edges. Using MoS2 as a model, we screened hundreds of edge configurations, leading to prediction of nine new reconstructions with record thermodynamic stability, in addition to successfully reproducting many of the recently discovered reconstructed edges. Application-wise, we discover that many of the reconstructed edges show near optimal hydrogen evolution activity over the conventional edges, with intrinsic tunability based on the metal/chalcogen ratio. Moreover, the reconstructed edges exhibit a wide distribution of work functions (a range of ~1.3 eV), suggesting that they can be optimized as catalysts for a wide range of reactions. We also find that they could be uniquely suited for applications in high-density information storage, spintronics, and topologically protected dissipationless transport from their exhibited half-metallicity, broad variation in magnetic moments, and intriguing topologically protected edge-states. Our work reveals the existence of a wide family of synthesizable, reconstructed edges in 2D TMDCs, thereby opening a new field of intrinsic edge engineering of 2D materials as multifunctional materials.

Predicting synthesizable multi-functional edge reconstructions in two-dimensional transition metal dichalcogenides

Macromolecular Chemistry: The Second Century

[Author Benefits](https://scimeetings.acs.org/?utm_source=pubs_content_marketing&utm_medium=website&utm_campaign=0320_MCF_NPI_Launch_Spring_Homepage&ref=pubs_content_marketing)

[How to use SciMeetings](https://storage.googleapis.com/dl.morressier.com/acs/SciMeetings-ACSSpring2020-HowToGuide_M3020-Final.pdf)

[Frequently Asked Questions](https://storage.googleapis.com/dl.morressier.com/acs/SciMtng_ACSNMSp2020_FAQ_M3120_Final.pdf)

ACS Spring 2020 National Meeting & Expo

The official archive and repository for all ACS Meetings & Expositions abstracts and select posters or presentations.