A highly active electrode is a prerequisite to accelerate the sluggish nitrogen reduction in the otherwise promising molten alkali-metal chloride (LiCl-KCl-CsCl)-based ammonia synthesis process. In this study, four 3d metals, i.e., Ti, Fe, Co, and Ni, were selected and evaluated as candidate electrode materials. The electrochemical performance of each material was evaluated using linear sweep voltammetry (LSV) and chronoamperometry (CA). The activity in nitrogen reduction, described in terms of effective nitrogen reduction current, was in the order of Co > Ni > Fe > Ti. The variation in performance was ascribed to a synergetic relation between the electrical resistivity and wettability of the materials, indicating that both factors must be considered in selecting electrode materials, particularly in a molten-type system. Copyright (C) 2015, Hydrogen Energy Publications, LLC. Published by Elsevier Ltd. All rights reserved.