Large-Scale Synthesis of High-Loading Single Metallic Atom Catalysts by a Metal Coordination Route.

Single atom catalyst (SAC) is one of the most efficient and versatile catalysts with well-defined active sites. However, facile and large-scale preparation of single-atom catalysts, the prerequisite of industrial applications, has been very challenging. This dilemma suffers from the Gibbs-Thomson effect which renders it rather difficult to achieve high single atom loading rate that mostly is below 3 mol%. Further, most of the synthesizing procedures of SAC are rather complex which result in significant mass loss and thus low yields. Herein, a novel metal coordination route is developed to address these issues simultaneously, which is realized owing to the rapid complexation between ligands (e.g., biuret) and metal ions in aqueous solutions and subsequent in-situ polymerization of the formed complexes to synthesize SACs. The whole preparation process involves only one heating step operated in air without any special protecting atmospheres, which is generally applicable for diverse transition metals. Take Cu SACs for an example, a record yield of up to 3.565 kg in one pot and an ultrahigh metal loading 16.03 mol% on carbon nitride (Cu/CN) are both approached. The as-prepared Cu/CN SACs are demonstrated to possess high activity, outstanding selectivity and robust cyclicity for CO2 photoreduction to HCOOH. This research explores a robust route toward cost-effective, massive production of SACs for potential industrial applications. This article is protected by copyright. All rights reserved.