Mn-Interconnected NiCo Layered Double Hydroxide Nanosheets on Ni Foam for Electrocatalytic Concurrent Glycerol Conversion to Hydrogen and Formate

Utilizing KMnO 4 and glycerol as co-precursors in a previously unexplored manner, we hydrothermally synthesized Mn-interconnected NiCo layered double hydroxide (LDH) ultrathin nanosheets directly grown on nickel foam (denoted as Mn–NiCo@NF-G). KMnO 4 was used as a Mn source and a strong oxidant for generating Ni 2+, while glycerol provided interlayer CO 3 2– ions and facilitated the formation of ultrathin LDH architectures. Comprehensive characterizations revealed that Mn was selectively incorporated into vacancy clusters of the Ni substrate and linked with Co, Mn, and O atoms via Mn---Co–O bonds, resulting in a robust interfacial coupling between the nanosheets and support. This unique structural configuration substantially enhanced charge transport and exposed a large electrochemically active surface area. The Mn–NiCo@NF-G electrode generated a current density of 10 mA·cm –2 at a low overpotential of 1.30 V vs RHE, and its Tafel slope was small (72 mV·dec –1 ). Furthermore, the electrocatalyst remained stable for 20 h of continuous operation. Remarkably, the catalyst exhibited over 90% selectivity for oxidizing glycerol to formate, demonstrating its potential for efficient and selective biomass conversion. These findings suggested a Mn–NiCo@NF-G electrode to be an effective bifunctional electrocatalyst for concurrent hydrogen production and synthesizing value-added chemicals.