Tuning the electrocatalytic activity of MoS2 nanosheets via the in situ hybridization with ruthenium and graphene network

• Published in: Chemical engineering journal (Lausanne, Switzerland : 1996) Switzerland : 1996), 2024-05, Vol.488, p.150950, Article 150950
• Main Authors: Islam, Sk Emdadul, Hang, Da-Ren, Liang, Chi-Te, Sharma, Krishna Hari, Huang, Hui-Chun, Chou, Mitch M.C.
• Format: Article
• Language: English
• Subjects: Electrocatalyst; Hydrogen evolution reaction; Phase transition; Ruthenium; Sulfur vacancy
• ISSN: 1385-8947; 1873-3212
• DOI: 10.1016/j.cej.2024.150950

[Display omitted] •Novel Ru/MoS2/G composite catalyst excels in hydrogen evolution reaction (HER).•Ruthenium nanoparticles enhance electron transfer, lowering HER energy barrier.•Catalyst works efficiently across wide pH range for sustainable hydrogen production.•Phase-engineered MoS2 increases active sites, boosting reaction activity.•Sulfur vacancies fine-tune electronic structure, enhancing HER performance. The quest for highly efficient, stable, and non-precious electrocatalysts as alternatives to Pt in the hydrogen evolution reaction (HER) at ambient temperature is paramount. Two-dimensional (2D) layered transition metal dichalcogenides (TMDs), notably MoS2, have emerged as promising noble-metal-free candidates. However, MoS2′s limited active edge sites and sluggish electron transfer kinetics present challenges in achieving efficient HER activity under both acidic and basic conditions. In this study, we introduce a composite catalyst composed of 2D MoS2 nanosheets enveloped by graphene networks, with uniform dispersion of ruthenium (Ru) nanoparticles within the extended 2D structure. This ternary hybrid catalyst exhibits excellent catalytic activity, with a low onset overpotential of 60 mV at 10 mA cm−2, a small Tafel slope of 38 mV dec-1, and remarkable durability during continuous 10-hour operation at 100 mV potential in 1.0 M KOH, without substantial activity loss. The conductive graphene support effectively prevents the restacking of exfoliated MoS2 nanosheets, enhancing mass transport and charge transfer kinetics. Ru incorporation induces the partial phase transformation of MoS2 from its trigonal (2H) to octahedral (1 T) phase, concurrently generating sulfur vacancies. The induced phase transformation not only activates the inert basal planes of MoS2 but also reduces the energy barrier for the adsorption/desorption of H* intermediates. Beyond the structural advantages, the intrinsic synergistic effects, primarily related to electronic structure modulation and defect engineering, contribute significantly to the enhanced electrochemical HER performance. In summary, this study not only introduces an efficient, cost-effective alternative to Pt-based electrocatalysts but also lays the foundation for designing other TMD-based hybrid catalysts, characterized by abundant exposed active sites and reduced barriers for hydrogen binding energy, thereby advancing electrochemical hydrogen production.