A Coordination-Derived Cerium-Based Amorphous-Crystalline Heterostructure with High Electrocatalytic Oxygen Evolution...

Area of Science:

• Materials Science
• Electrochemistry
• Catalysis

Background:

• Rational design of heterogeneous catalysts is key for optimal physicochemical properties and electrochemical activity.
• Developing amorphous-crystalline heterostructures presents greater challenges than crystalline-crystalline ones.

Purpose of the Study:

• To introduce a novel coordination-assisted strategy for fabricating amorphous-crystalline heterostructures.
• To investigate the role of coordination geometry in forming high-nickel content coordination polymers.
• To enable the endogenous spillover of nickel for creating amorphous NiO/crystalline NiCeO_x (a-NiO/c-NiCeO_x) heterostructures.

Main Methods:

• Utilized a coordination-assisted strategy involving organic ligands to form coordination polymers.
• Employed annealing processes to induce nickel supersaturation and surface spillover.
• Conducted theoretical calculations to analyze charge transfer and interfacial effects.

Main Results:

• Successfully fabricated strongly coupled amorphous NiO and crystalline NiCeO_x (a-NiO/c-NiCeO_x) heterostructures.
• The resulting heterostructure demonstrated low overpotentials and high catalytic stability in the oxygen evolution reaction (OER).
• Theoretical calculations confirmed that amorphous-crystalline interfaces facilitate charge transfer and optimize Ni site activity.

Conclusions:

• The coordination-assisted strategy is effective for designing advanced amorphous-crystalline heterostructures.
• Amorphous-crystalline interfaces play a crucial role in enhancing catalytic performance by regulating electron density and lowering energy barriers.
• This approach highlights the potential of molecular-level coordination for designing novel heterogeneous catalysts.