Electrochemical Synthesis of Ammonia from N₂ and H₂O under Ambient Conditions Using Pore-Size-Controlled Hollow Gold Nanocatalysts with Tunable Plasmonic Properties

Abstract

An electrochemical nitrogen reduction reaction (NRR) could provide an alternative pathway to the Haber–Bosch process for clean, sustainable, and decentralized NH3 production when it is coupled with renewably derived electricity sources. Developing an electrocatalyst that overcomes sluggish kinetics due to the challenges associated with N2 adsorption and cleavage and that also produces NH3 with a reasonable yield and efficiency is an urgent need. Here, we engineer the size and density of pores in the walls of hollow Au nanocages (AuHNCs) by tuning their peak localized surface plasmon resonance (LSPR); in this way, we aim to enhance the rate of electroreduction of N2 to NH3. The interdependency between the pore size/density, the peak LSPR position, the silver content in the cavity, and the total surface area of the nanoparticle should be realized for further optimization of hollow plasmonic nanocatalysts in electrochemical NRRs