Abstract
Molybdenum disulfide (MoS(2)) has recently emerged as a promising electrocatalyst for the hydrogen evolution reaction (HER). However, the poor in-plane electrical conductivity and inert basal plane activity pose major challenges in realizing its practical application. Herein, we demonstrate a new approach to induce biaxial strain into CVD-grown MoS(2) monolayers by draping it over an array of patterned gold nanopillar arrays (AuNAs) as an efficient strategy to enhance its HER activity. We vary the magnitude of applied strain by changing the inter-pillar spacing, and its effect on the HER activity is investigated. To capitalize on the synergistic effect of improved ΔG (H) via strain engineering and leverage basal plane activation by introduction of sulphur vacancies, we further exposed the strained MoS(2) monolayers to oxygen plasma treatment to create S-vacancies. The strained MoS(2) on AuNAs with optimal inter-pillar spacing is exposed to oxygen plasma treatment for different durations, and we study its electrocatalytic activity towards the HER using on-chip microcell devices. The strained and vacancy-rich monolayer MoS(2) draped on AuNAs with a 0.5 μm inter-pillar spacing and exposed to plasma for 50 s (S(0.5μm)V(50)-MoS(2)) is shown to exhibit remarkable improvement in HER activity, with an overpotential of 53 mV in 0.5 M H(2)SO(4). Thus, the synergistic creation of additional vacancy defects, along with strain-induced active sites, results in enhancement in HER performance of CVD-grown monolayer MoS(2). The present study provides a highly promising route for engineering 2D electrocatalysts towards efficient hydrogen evolution.