Atomically Dispersed Pd on ZrO2 for Efficient Nitrite Electroreduction to Ammonia

Abstract

Electrochemical conversion of NO2- to NH3 (NO2RR) provides an appealing route to enable effective wastewater treatment and sustainable NH3 production. Herein, we report that atomically dispersed Pd on ZrO2 substrate (Pd1/ZrO2) serves as an effective and durable NO2RR catalyst, showing the maximum NH3-Faraday efficiency of 96.75% and the corresponding NH3 yield rate of 438.06 µmol h-1 cm-2 at -0.6 V. Combined experiments and theoretical calculations reveal that Pd1 incorporation enables the construction of unique Zr-Pd1-O motifs that can effectively activate NO2-, optimize the intermediate adsorption energies and suppress the competing H2 evolution, resulting in greatly enhanced NO2RR activity and selectivity.