▎ 摘　　要

One of the bottlenecks in realizing the potential of nanoporous graphene assemblies is the difficulty of engineering narrow pores and high surface density distributions, with a nanometer resolution across multilayer graphene assemblies using scalable approaches. Here, the authors develop a photocatalyzed perforation protocol to incorporate nanopores across modified graphene assemblies via localizing the oxidation during the photo-excitation process between photo-initiators and graphitic assemblies under the ultraviolet-visible stimuli. Nanopores are engineered across the graphene nanostructures with a pore size range varying from 20 to 100 nm depending on the irradiation duration, as well as tunable densities of 10(1)-10(3) pores/mu m(2) on the same order of the loaded nanocatalysts to the graphene surfaces. By fine-tuning the graphene chemistry and the physical dimension of photo-initiators, as well as their concentrations across graphitic planes used during the perforation, the diameter, and the density distributions of generated nanopores across graphene, can be rationally confined, avoiding merging between pores during the nanopore formation. These porosity parameters engineered across graphene nanosieves are in the same order obtained by other nanolithographic techniques. Plus, this sustainable route may boost the potential of porous graphene assemblies in energy-efficient nanotechnologies based on separation and catalytic processes.