Cation-Site Disordered Cu₃PdN Nanoparticles for Hydrogen Evolution Electrocatalysis

Area of Science:

• Materials Science
• Nanotechnology
• Inorganic Chemistry

Background:

• Transition metal nitrides (TMNs) are promising for optoelectronics and energy applications.
• Their full potential is limited by a lack of mechanistic understanding in synthesis.
• Copper-palladium nitride (Cu3PdN) is an underexplored TMN material.

Purpose of the Study:

• To develop a rapid, one-pot synthesis for phase-pure Cu3PdN nanoparticles.
• To elucidate the mechanistic pathways of Cu3PdN formation and nanocrystal growth.
• To investigate the structural properties and catalytic activity of the synthesized Cu3PdN nanoparticles.

Main Methods:

• One-pot synthesis using copper methoxide and palladium acetylacetonate in benzylamine.
• In situ X-ray absorption spectroscopy (XAS) to study complex conversion and structure.
• In situ total X-ray scattering (TXS) to reveal nucleation and growth mechanisms.
• Extended X-ray absorption fine structure (EXAFS) double-edge refinement for detailed structural analysis.
• Electrocatalytic testing for hydrogen evolution reaction (HER).

Main Results:

• Successfully synthesized 3 nm phase-pure Cu3PdN nanoparticles in 5 minutes at 140 °C.
• Mechanistic insights into nucleation and growth provided by in situ XAS and TXS.
• Discovered novel short-range cation-site disorder in the anti-perovskite structure of Cu3PdN.
• Achieved a low overpotential of 212 ± 11 mV for hydrogen evolution reaction at 10 mA cm⁻².

Conclusions:

• A facile and rapid one-pot synthesis for Cu3PdN nanoparticles has been established.
• The study provides crucial mechanistic understanding of TMN formation.
• The unique structural disorder and promising HER activity highlight Cu3PdN as a material of significant interest for energy applications.