Interlayer engineering of molybdenum disulfide toward efficient electrocatalytic hydrogenation

Area of Science:

• Materials Science
• Electrochemistry
• Sustainable Chemistry

Background:

• Electrocatalytic hydrogenation (ECH) is crucial for sustainable chemical production but faces challenges like hydrogen evolution and reliance on precious metal catalysts.
• Molybdenum disulfide (MoS2) typically exhibits high activity for hydrogen evolution, limiting its application in other electrocatalytic processes.

Purpose of the Study:

• To develop an efficient and noble-metal-free catalyst for electrocatalytic hydrogenation (ECH) of biomass-derived oxygenates.
• To engineer molybdenum disulfide (MoS2) to suppress hydrogen evolution and enhance ECH activity.

Main Methods:

• In situ intercalation of ammonia or alkyl-amine cations into MoS2 to induce phase transition (2H to 1T).
• Characterization of the modified MoS2 catalyst (MoS2-DMA) for electronic configuration and surface properties.
• Electrocatalytic hydrogenation of furfural (FAL) to furfuryl alcohol using the optimized MoS2-DMA catalyst.

Main Results:

• Intercalation engineering of MoS2 significantly altered its phase, electronic structure, and surface hydrophobicity, promoting ECH while inhibiting hydrogen evolution.
• The optimal dimethylamine-intercalated MoS2 (MoS2-DMA) achieved high Faradaic efficiency (86.3%-73.3%) and selectivity (>95.0%) for furfural hydrogenation.
• Enhanced chemisorption of intermediates and improved hydrophobicity on MoS2-DMA accelerated the reaction rate via a Langmuir-Hinshelwood mechanism.

Conclusions:

• Molybdenum disulfide, when engineered through cation intercalation, can be transformed from a hydrogen evolution catalyst into a highly effective catalyst for electrocatalytic hydrogenation.
• This approach offers a sustainable, noble-metal-free route for producing valuable chemicals from biomass-derived oxygenates.
• The study expands the potential of MoS2 in electrochemical synthesis and provides insights into catalyst design for selective transformations.