Modulating surface electronic structure of mesoporous Rh nanoparticles by Se-doping for enhanced electrochemical ammonia synthesis

Abstract

• The Se-mRh NPs have been fabricated by a simple and general two-step method. • Mesoporous structure can provide abundant active sites. • Se-doping could modify surface electronic structure of Se-mRh NPs. • The Se-mRh NPs exhibit superior performance for electrochemical ammonia synthesis. Electrochemical nitrogen reduction reaction (NRR) is a facile and sustainable alternative strategy to Haber-Bosch process for ammonia synthesis. Design of efficient and stable electrocatalysts is critical to NRR. Herein, a two-step method is proposed to fabricate surface Se-doping mesoporous Rh nanoparticles (Se-mRh NPs). Owing to the mesoporous structure and Se modified surface, the Se-mRh NPs exhibit a superior NH 3 yield (21.36 μg h −1 mg −1 cat. ) and Faradaic efficiency (34.54 %) in a neutral electrolyte (0.1 M Na 2 SO 4 ) relative to mesoporous Rh nanoparticles (mRh NPs). The presented synthetic approach is very valuable for design of metallic catalysts with Se modified surface for various electrocatalytic applications.