Creating High-entropy Single Atoms on Transition Disulfides through Substrate-induced Redox Dynamics for Efficient...

Area of Science:

• Materials Science
• Catalysis
• Nanotechnology

Background:

• Controllable anchoring of multiple metal single-atoms (SAs) offers significant opportunities.
• Integrating multimetallic SAs and high-entropy SAs (HESAs) into single-atom catalysts (SACs) presents a major challenge.

Purpose of the Study:

• To develop a substrate-mediated strategy for fabricating multimetallic SAs and HESAs on MoS2 and MoSe2 supports.
• To precisely control the doping location and concentration of SAs on transition metal dichalcogenides (TMDs).

Main Methods:

• A substrate-mediated SAs formation strategy was employed.
• Reversible redox reactions at the TMDs/TM ion interface were controlled to synthesize HESAs.
• Mechanistic studies were conducted to understand the synthesis process.

Main Results:

• A library of multimetallic SAs and HESAs was successfully fabricated on MoS2 and MoSe2.
• SA doping concentration was precisely controlled, allowing for high metal loading.
• Optimized HESAs-TMDs (Pt,Ru,Rh,Pd,Re-MoSe2) exhibited superior activity and durability for hydrogen evolution reaction (HER) compared to state-of-the-art Pt catalysts.

Conclusions:

• The study presents a novel guideline for the rational design of high-performance single-atom catalysts.
• The developed method broadens the family of available single-atom catalysts.
• This approach facilitates precise control over SA doping and enables high metal content for enhanced catalytic performance.