Assembling Metal Organic Layer Composites for High‐Performance Electrocatalytic CO 2 Reduction to Formate

Abstract 2D metal–organic‐framework (MOF) based composites have emerged as promising candidates for electrocatalysis due to their high structural flexibility and fully exposed active sites. Herein, a freestanding metal–organic layer (MOL) with kgd (kagome dual) lattice was constructed abundant surface oxygenate groups serving anchoring sites immobilize diverse guests. Taking Bi an example, tetragonal 2 O 3 nanowires can be uniformly grown on MOLs after solvothermal treatment, the evolution of which followed by ex situ electron microscopy. The as‐prepared /MOL exhibits excellent CO electroreduction activity towards formate reaching specific current 2.3 A mg −1 Faradaic efficiencies over 85 % wide potential range from −0.87 −1.17 V, far surpassing /UiO (a 3D Zr 6 ‐oxo MOF) /AB (Acetylene Black). Such post‐synthetic modification strategy flexibly extended develop versatile MOL composites, highlighting superiority optimizing MOL‐based electrocatalysis.