Synergistic Activation Mechanism of Multidefect Structures in Atomically Thin Oxygen Evolution Electrocatalysts

Area of Science:

• Materials Science
• Electrochemistry
• Catalysis

Background:

• Electrocatalytic water splitting is crucial for clean energy but hindered by slow oxygen evolution reaction (OER) kinetics.
• Defect engineering improves OER catalysis, but traditional single/dual-defect approaches have limitations.

Purpose of the Study:

• To develop a novel triple-defect coordination system in atomically thin CoOOH nanosheets for enhanced OER catalysis.
• To overcome characterization challenges in multidefect systems using an ultrathin architecture.

Main Methods:

• Atomic-scale imaging and advanced structural analysis to visualize multidefect configurations.
• Electrochemical assessment to evaluate catalytic activity and stability.
• Density functional theory (DFT) calculations to elucidate the synergistic mechanism.

Main Results:

• Demonstrated exceptional OER activity (286 mV overpotential @ 10 mA cm⁻²) and stability (>100 h).
• Confirmed multidefect configurations (Mn²⁺/W⁶⁺ dopants and Co vacancies) via direct visualization.
• DFT revealed that multidefect synergy optimizes intermediate binding energies, positioning ΔGO near the ideal midpoint.

Conclusions:

• Established a paradigm for rational electrocatalyst design through visualization of atomic-level multidefect interplay.
• The triple-defect system in ultrathin CoOOH nanosheets significantly enhances OER performance.
• This approach offers a promising strategy for developing efficient electrocatalysts for the clean energy transition.