Atomic Ru-Mediated Spontaneous Heterointerface Phase Transition Enables Ampere-Level Catalytic Performance in Paired...

Area of Science:

• Materials Science
• Electrochemistry
• Catalysis

Background:

• Phase transition regulation is key to optimizing catalyst properties for electrocatalysis.
• The link between atomic-scale interface phase transitions and catalytic performance is not well understood.

Purpose of the Study:

• To investigate the heteroatomic interfacial phase transition of Co3S4/Co heterostructures.
• To understand the role of single-atom ruthenium in triggering this transition and its impact on catalytic performance.
• To develop a high-performance catalyst for sustained paired electrosynthesis.

Main Methods:

• Fabrication of single-atom ruthenium anchored cobalt sulfide/cobalt heterostructured nanosheets (RuSA-Co9S8/Co-T).
• Utilized theoretical calculations and in situ spectroscopy to confirm the phase transition and analyze catalytic mechanisms.
• Tested the catalyst in membrane electrode assembly electrolyzers for nitrite-glycerol co-electrolysis.

Main Results:

• Achieved ampere-level catalytic performance through a thermally induced phase transition from Co3S4/Co to Co9S8/Co, triggered by single-atom ruthenium.
• The RuSA-Co9S8/Co-T catalyst demonstrated optimized intermediate formation kinetics and reduced energy barriers for rate-determining steps.
• Exhibited high average Faradaic efficiencies (>90%) for ammonia and formate production, with yields up to 95.83 mg h-1 cm-2 and 567.38 mg h-1 cm-2, respectively.
• Showcased stable operation for 100 hours at an industrial current density of 500 mA cm-2.

Conclusions:

• Single-atom ruthenium effectively induces a beneficial interfacial phase transition in cobalt sulfide catalysts.
• The developed RuSA-Co9S8/Co-T catalyst offers a promising solution for efficient and sustained paired electrosynthesis.
• This research provides critical insights into designing advanced catalysts by controlling atomic-scale phase transitions.