Amorphous Nanobelts for Efficient Electrocatalytic Ammonia Production.

Abstract

One-dimensional (1D) amorphous nanomaterials combine the advantages of high active site concentration of amorphous structure, high specific surface area and efficient charge transfer of 1D materials, so they present promising opportunities for catalysis. However, how to achievie the balance between the high orientation of 1D morphology and the isotropy of amorphous structure is a significant challenge, which severely obstructs the controllable preparation of 1D amorphous materials. Guided by the hard-soft acids-bases theory, here we develop a general strategy for preparing 1D amorphous nanomaterials through the precise modulation of bond strength between metal ions and organic ligands for a moderated fastness. The soft base dodecanethiol (DT) is multifunctionally served as both structure-regulating agent and morphology-directing agent. Compared with the borderline acids (e.g. Fe²⁺, Co²⁺, Ni²⁺) to construct amorphous structure, soft acid of Cu⁺ which produced crystalline nanobelts can still be amorphized by reducing the hardness of Cu ions through redox reaction to weak Cu-SR bond. Due to the combined advantages of amorphous structure and one-dimensional morphology, amorphous CuDT nanobelts exhibited excellent electrocatalytic activity in electrochemical nitrate reduction, outperformed most of the reported Cu-based catalysts. This work will effectively bridge the gap between traditional 1D crystalline nanomaterials synthesis and their amorphization preparation.