Rational Framework Engineering of 1T' Mo-Re Sulfides with Optimized Orbital Hybridization for Efficient Acidic...

Area of Science:

• Materials Science
• Catalysis
• Electrochemistry

Background:

• Metallic 1T-phase MoS2 shows promise as a platinum-group catalyst alternative for the acidic hydrogen evolution reaction (HER).
• The metastable nature of 1T-phase MoS2 hinders its practical application due to instability.
• Developing stable catalysts for HER is crucial for efficient hydrogen production.

Purpose of the Study:

• To develop a framework-stabilization strategy for metastable 1T'-phase Mo-Re sulfides.
• To investigate the structural, electronic, and catalytic properties of Mo-substituted ReS2 for HER.
• To establish a new paradigm for designing and stabilizing metastable transition metal dichalcogenides.

Main Methods:

• Synthesis of 1T'-phase Mo-Re sulfides (Re0.5Mo0.5S2) using ReS2 as a structural scaffold.
• Characterization using theoretical calculations and experimental techniques.
• Evaluation of catalytic activity and stability for the acidic hydrogen evolution reaction (HER).

Main Results:

• Formation of high-purity 1T'-phase Re0.5Mo0.5S2 with a stable structure.
• Mo incorporation induced favorable electronic changes, including orbital hybridization and charge redistribution.
• Achieved exceptional HER performance with a low overpotential (113 mV at 10 mA cm-2) and high stability (>50 h).

Conclusions:

• The framework-stabilization strategy effectively stabilizes metastable 1T'-phase Mo-Re sulfides.
• Re0.5Mo0.5S2 demonstrates superior catalytic activity and durability for acidic HER.
• This work offers insights into the rational design of metastable functional materials for catalysis.