Scalable Synthesis of Holey Deficient 2D Co/NiO Single-Crystal Nanomeshes via Topological Transformation for Efficient Photocatalytic CO Reduction.

Preparation of holey, single-crystal, 2D nanomaterials containing in-plane nanosized pores is very appealing for the environment and energy-related applications. Herein, an in situ topological transformation is showcased of 2D layered double hydroxides (LDHs) allows scalable synthesis of holey, single-crystal 2D transition metal oxides (TMOs) nanomesh of ultrathin thickness. As-synthesized 2D Co/NiO-2 nanomesh delivers superior photocatalytic CO -syngas conversion efficiency (i.e., V of 32460 µmol h g CO and of 17840 µmol h g H ), with V about 7.08 and 2.53 times that of NiO and 2D Co/NiO-1 nanomesh containing larger pore size, respectively. As revealed in high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM), the high performance of Co/NiO-2 nanomesh primarily originates from the edge sites of nanopores, which carry more defect structures (e.g., atomic steps or vacancies) than basal plane for CO adsorption, and from its single-crystal structure adept at charge transport. Theoretical calculation shows the topological transformation from 2D hydroxide to holey 2D oxide can be achieved, probably since the trace Co dopant induces a lattice distortion and thus a sharp decrease of the dehydration energy of hydroxide precursor. The findings can advance the design of intriguing holey 2D materials with well-defined geometric and electronic properties.