Abstract
The intrinsic activity of in-plane chalcogen atoms plays a significant role in the catalytic performance of transition metal dichalcogenides (TMDs). A rational modulation of the local configurations is essential to activating the in-plane chalcogen atoms but restricted by the high energy barrier to break the in-plane TM-X (X = chalcogen) bonds. Here, we theoretically design and experimentally realize the tuning of local configurations. The electron transfer capacity of local configurations is used to screen suitable TMDs materials for hydrogen evolution reaction (HER). Among various configurations, the triangular-shape cobalt atom cluster with a central sulfur vacancy (3CoMo-VS) renders the distinct electrocatalytic performance of MoS2 with much reduced overpotential and Tafel slope. The present study sheds light on deeper understanding of atomic-scale local configuration in TMDs and a methodology to boost the intrinsic activity of chalcogen atoms.
Highlights
The intrinsic activity of in-plane chalcogen atoms plays a significant role in the catalytic performance of transition metal dichalcogenides (TMDs)
A critical carrier density, the transport of donor states is governed by nearest-neighbor hopping at high temperatures and variable-range hopping (VRH) at low temperatures[23,34,35,36]
We have promoted the per-site electrochemical activity of inplane sulfur sites of MoS2 monolayer via tuning H–S bonding strength, which can be understood by a hypothetical model of activating the inert sulfur atom into an open valence state
Summary
The intrinsic activity of in-plane chalcogen atoms plays a significant role in the catalytic performance of transition metal dichalcogenides (TMDs). In order to improve the intrinsic activity of in-plane sulfur atoms, it is essential to understand the intrinsic correlation and explore new methodologies to enrich stable and highly efficient local configurations. We conducts both computational and experimental investigations in order to establish a correlation between local configuration and the electrocatalytic activity of monolayer MoS2. As demonstrated in the present work, it is possible to further activate the in-plane sulfur sites by rational engineering of the local configurations This result may provide a route to unleash the electrocatalytic potential of TMD materials for efficient hydrogen generation in acidic solutions
Sign-in/Register to view highlights & summary Talk to us
Join us for a 30 min session where you can share your feedback and ask us any queries you have
Schedule a callDisclaimer: All third-party content on this website/platform is and will remain the property of their respective owners and is provided on "as is" basis without any warranties, express or implied. Use of third-party content does not indicate any affiliation, sponsorship with or endorsement by them. Any references to third-party content is to identify the corresponding services and shall be considered fair use under The CopyrightLaw.
