Boosting the Hydrogen Production Coupling with Electrochemical Methanol Oxidation to Formate Using Monolayered Layered Double Hydroxide Nanosheets

The process of electrolytic water splitting for hydrogen production is considered a promising approach for achieving sustainable and environmentally friendly development. However, this is hindered by the challenge of water oxidation. The favorable methanol oxidation reaction (MOR) to formate at the anode to replace the sluggish kinetic oxygen evolution reaction (OER) can reduce power consumption and offer a new route for the production of hydrogen. Herein, we carried out a simple, commercially scaled-up synthesis method to synthesize monolayer layered double hydroxide (LDH) powders through separate nucleation and aging steps (SNAS). The acquired monolayer NiFe-LDH (m-NiFe-LDH) exhibited improved MOR activity, promoting the rate of high-value formate about 12 times that of its multilayer counterpart (u-NiFe-LDH). Moreover, the MOR catalyzed by m-NiFe-LDH can further increase the hydrogen production rate of the cathode, which is more than 5 times higher than that of u-NiFe-LDH. The effective approach to increasing the production scale of synthesizing monolayer LDH powders with defects has provided novel perspectives on the generation of formate and green hydrogen.