Active Basal Plane Catalytic Activity via Interfacial Engineering for a Finely Tunable Conducting Polymer/MoS₂...

Area of Science:

• Materials Science
• Electrochemistry
• Catalysis

Background:

• The catalytic performance of molybdenum disulfide (MoS₂) is highly sensitive to its interface and embedding environment.
• Interfacial engineering is crucial for designing efficient catalysts by optimizing charge transfer and electronic interactions.
• Controlling the binding agents and interfacial structure is key to enhancing MoS₂ catalyst activity.

Purpose of the Study:

• To develop a layer-by-layer (LbL) strategy for preparing interfacial MoS₂-based catalyst structures.
• To investigate the impact of different conducting polymers (polypyrrole and polyaniline) on MoS₂'s electronic structure and catalytic performance.
• To optimize the LbL assembly process for enhanced hydrogen evolution reaction (HER) activity.

Main Methods:

• Fabrication of MoS₂-based catalyst structures using a layer-by-layer (LbL) assembly technique with conducting polymers.
• Characterization of the electronic structures of MoS₂ within the assembled interfaces.
• Density functional theory (DFT) calculations to understand interfacial charge transport and hydrogen adsorption mechanisms.

Main Results:

• The LbL strategy allows precise control over the interfacial electronic structure of MoS₂.
• Polypyrrole as a binder significantly enhances catalytic efficacy for HER compared to polyaniline, increasing active sulfur species.
• DFT calculations confirm that interfacial charge transfer boosts HER activity by reducing H* adsorption energy on MoS₂ basal plane sites.
• Optimized catalytic performance was achieved with 16 assembly cycles of the conducting polymer/MoS₂ structure.

Conclusions:

• The LbL-based strategy provides a flexible and scalable method for immobilizing electrocatalysts with precise nanoscale control and centimeter-scale homogeneity.
• Interfacial engineering using conducting polymers is effective in tuning MoS₂'s electronic properties for improved HER catalysis.
• This approach offers a pathway for fundamental understanding and practical application of highly efficient interfacial electrocatalysts.