LAUSR

It is of pivotal significance to explore robust photocatalysts to promote the photoreduction of carbon dioxide (CO2) into solar fuels. Herein, we developed an intelligent metal-insulator-semiconductor (MIS) nano-architectural photosystem constructed by electrostatically self-assembling between cetyltrimethylammonium bromide (CTAB) insulator capped metal Ni nanoparticles (NPs) and covalent triazine-based frameworks (CTF-1). The metal-insulator-CTF composites unveiled a substantially higher CO evolution rate (1254.15 μmol g-1 h-1) compared with primitive CTF-1 (1.08 μmol g-1 h-1) and reached considerable selectivity (98.9%) under visible-light irradiations. The superior photocatalytic CO2 conversion activity over Ni-CTAB-CTF nano-architectural could be attributed to the larger surface area, reinforced visible-light responsive and CO2 capture capacity. More importantly, the ingenious Ni-CTAB-CTF nanoarchitecture endowed the photoexcited electrons on CTF-1 with the ability to tunnel across the thin CTAB insulating layer, directionally migrating to Ni NPs, thereby leading to the efficient separation of photogenerated electrons and holes in such photosystem. In addition, isotope-labeled (13CO2) tracer results verified that the reduction products come from CO2 rather than the decomposition of the photocatalysts. This study opens a new avenue for establishing a highly efficient and selective artificial photosystem for CO2 conversion.