Two-dimensional metal–organic layer (MOL) nanosheets,
as
nonhomogeneous catalysts, show better optical activity in the field
of photocatalysis due to their unique structural advantages. Current
research focuses on how to modify the structure of 2D nanosheets by
means of crystal engineering to modulate the intralayer electron transfer
pathway and systematically investigate the impacts of size effect
and electron transfer pathway on the energy utilization efficiency
of crystalline materials. In the present work, a triple lophine-derived
ligand was designed and prepared, which exhibits a large π-conjugation
system and multiple D–A (D: donor, A: acceptor) electron transfer
pathways. 2D MOL constructed with Cd ions can be exfoliated by physical
sonication to obtain double-walled 2D MOL nanosheets. Compared with
the bulk crystalline material, the 2D nanosheets exhibit better photovoltaic
properties. Benefiting from the excellent structural advantages, 2D
MOL nanosheets could be used as photocatalysts for a variety of aerobic
oxidation reactions under mild conditions (10 W white LED, room temperature),
such as the trifluoromethylation of coumarins, the synthesis of benzimidazole
derivatives from aromatic diamines and aromatic aldehydes, and the
preparation of 2,4,6-triarylpyridine derivatives, all with high conversion
rates and selectivity (yield typically greater than 88%). The related
results illustrate that the introduction of the photoactive triple-lophine
unit into 2D MOL nanosheets can effectively modulate the electron
transport mode and enhance energy utilization, which provides a new
research idea for the development of nonhomogeneous photocatalysts
aimed at the applications of visible light-driven organic conversion.