Metal–Organic Layers for Electrocatalysis and Photocatalysis

[Image: see text] Metal–organic layers (MOLs) are two-dimensional analogues of metal–organic frameworks (MOFs) with a high aspect ratio and thickness down to a monolayer. Active sites on MOLs are more accessible than those on MOFs thanks to the two-dimensional feature of MOLs, which allows easier chemical modification around the catalytic center. MOLs can also be assembled with other functional materials through surface anchoring sites that can facilitate charge/energy transport through the hybrid material. MOLs are thus quite suitable for interfacial catalysis like electrocatalysis and photocatalysis. In this outlook, we focus on representative progress of constructing unique interfacial sites on MOLs with designer paths for charge separation and energy transfer, as well as cooperative cavities for superior substrate adsorption and activation. We also discuss challenges and potentials in the future development of MOL catalysts and catalysts beyond MOLs.