Highly Curved, Quasi‐Single‐Crystalline Mesoporous Metal Nanoplates Promote CC Bond Cleavage in Ethanol Oxidation Electrocatalysis

Abstract The ability to manipulate metal nanocrystals with well‐defined morphologies and structures is greatly important in material chemistry, catalysis chemistry, nanoscience, and nanotechnology. Although 2D metals serve as interesting platforms, further manipulating them in solution with highly penetrated mesopores and ideal crystallinity remains a huge challenge. Here, an easy yet powerful synthesis strategy for manipulating the mesoporous structure and crystallinity of 2D metals in a controlled manner with cetyltrimethylammonium chloride as the mesopore‐forming surfactant and extra iodine‐ion as the structure/facet‐selective agent is reported. This strategy allows for preparing an unprecedented type of 2D quasi‐single‐crystalline mesoporous nanoplates (SMPs) with highly curved morphology and controlled metal composition. The products, for example, PdCu SMPs, feature abundant undercoordinated sites, optimized electronic structures, excellent electron/mass transfers, and confined mesopore environments. Curved PdCu SMPs exhibit remarkable electrocatalytic activity of 6.09 A mg_Pd⁻¹ and stability for ethanol oxidation reaction (EOR) compared with its counterpart catalysts and commercial Pd/C. More importantly, PdCu SMPs are highly selective for EOR electrocatalysis that dramatically promotes C–C bond cleavage with a superior C1 pathway selectivity as high as 72.1%.