Enhanced performance of in-plane transition metal dichalcogenides monolayers by configuring local atomic structures

Yao Zhou,Jun Lou,Jing Zhang,Jiadong Zhou,Junhao Lin,Hong Jin Fan,Wu Zhou,Jianjun Liu,Zheng Liu,Kazu Suenaga,Erhong Song

doi:10.1038/s41467-020-16111-0

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

Introduction

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

Methods

Results

Conclusion