Computation-Guided Dual-Site Electrocatalysts for Record-Performance Nitrite-to-Ammonia Conversion

Area of Science:

• Electrochemistry
• Materials Science
• Catalysis

Background:

• Electrochemical ammonia synthesis faces challenges in simultaneously activating reactants and facilitating hydrogenation.
• Developing efficient catalysts is crucial for sustainable ammonia production.

Purpose of the Study:

• To report a computation-guided, dual-site electrocatalyst design strategy.
• To bridge first-principles theory with device-level validation for catalyst development.

Main Methods:

• Density functional theory (DFT) calculations were used to identify optimal catalyst materials.
• A dual-site catalyst platform (Cu-doped ZnO) was designed and validated at the device level.
• Operando spectroscopy was employed to confirm the reaction mechanism.

Main Results:

• Cu-doped ZnO was identified as an optimal dual-site catalyst, with Cu sites enhancing nitrite adsorption and ZnO sites promoting water dissociation.
• The catalyst achieved a record ammonia (NH3) yield of 552.16 mg h⁻¹ cm⁻² with 87.9% Faradaic efficiency in a membrane electrode assembly.
• The dual-site synergy effectively suppressed the competing hydrogen evolution reaction.

Conclusions:

• The study demonstrates a successful theory-to-device workflow for predictive catalyst design.
• This approach offers a generalizable paradigm for developing advanced electrocatalysts for sustainable chemical transformations.
• The designed electrocatalyst significantly outperforms existing configurations in ammonia synthesis.