Underpotential Deposition of 3d Transition Metals: Versatile Electrosynthesis of Single-Atom Catalysts on Oxidized Carbon Supports.

Use of single-atom catalysts (SACs) has become a popular strategy for tuning activity and selectivity towards specific pathways. However, conventional SAC synthesis methods require high temperatures and pressures, complicated procedures, and expensive equipment. Recently, underpotential deposition (UPD) has been investigated as a promising alternative, yielding high-loading SAC electrodes under ambient conditions and within minutes. Yet only few studies have employed UPD to synthesize SACs, and all have been limited to UPD of Cu. In this work, we report a flexible UPD approach for synthesis of mono- and bi-metallic Cu, Fe, Co, and Ni SACs directly on oxidized, commercially available carbon electrodes. We investigate the UPD mechanism using in-situ x-ray absorption spectroscopy and, finally, assess the catalytic performance of a UPD-synthesized Co SAC for electrochemical nitrate reduction to ammonia. Our findings expand upon the usefulness and versatility of UPD for SAC synthesis, with hopes of enabling future research towards realization of fast, reliable, and fully electrified SAC synthesis processes. This article is protected by copyright. All rights reserved.

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This article is protected by copyright. All rights reserved.