A Dual-Coordination Strategy for Constructing Highly Active Pd Clusters to Enhance Methane Catalytic Combustion

Area of Science:

• Materials Science
• Catalysis Science
• Environmental Chemistry

Background:

• Subnanometer palladium (Pd) clusters are crucial for methane combustion catalysis.
• Developing highly efficient and stable Pd clusters remains a significant challenge.

Purpose of the Study:

• To engineer highly active and stable subnanometer Pd clusters for methane catalytic combustion.
• To explore a dual-coordination strategy for modulating Pd cluster electronic structure and metal-support interactions.

Main Methods:

• Utilized g-C3N4 as a Pd2+ anchoring agent and H3BTC as a support defect-regulating ligand.
• Achieved confined growth of low-coordination PdOx clusters on defect-rich ceria (CeO2) support.
• Employed advanced structural and electronic characterization techniques.

Main Results:

• Developed electron-deficient Pd clusters (Pd_n) with optimized metal-support interactions.
• Achieved superior methane combustion activity (T90 = 367 °C) and stability.
• Demonstrated a turnover frequency of 0.064 s^-1 at 350 °C, outperforming single-atom catalysts.

Conclusions:

• The dual-coordination strategy effectively stabilizes subnanometer Pd clusters.
• Enhanced oxygen mobility and methane C-H bond activation contribute to superior catalytic performance.
• This approach offers a promising pathway for designing advanced cluster-based catalysts for methane abatement.