Covalent
triazine frameworks (CTFs) with high adsorption potential
and photocatalytic ability features are expected to be designed as
a new class of adsorbents that can regenerate themselves just by harnessing
sunlight. To simultaneously improve both the adsorption and photocatalytic
regeneration performance, a defect-abundant CTF-m was designed and
tuned effectively by varying the lengths of benzene ring chains incorporated
into the CTF backbone. It has been demonstrated that two kinds of
defects in terms of broken benzene rings and pyrrole nitrogen were
newly generated, other than the normal benzene rings and triazine
units in the CTF-m skeleton. Benefiting from these defects, the adsorption
sites with high energy for adsorbing volatile aromatic pollutants
were significantly increased, which are reflected by higher saturated
adsorption capacities of CTF-m (3.026 mmol/g for benzene (BEN), 1.490
mmol/g for naphthalene (NAP), and 0.863 mmol/g for phenol (PHE)) compared
with those of CTF-1 and CTF-2. Furthermore, these defects narrowed
the band structure and facilitated the separation of photogenerated
charge carries, thus promoting photocatalytic regeneration. The percentage
of CTF-m regenerated was still higher than 90% in the fourth cycle.
These experimental results, together with the density functional theory
(DFT) studies, soundly corroborated that the defects could optimize
the adsorption and regeneration property of CTF-m. The present work
highlights the potential of fabrication of defective CTFs as solar-driven
self-cleaning adsorbents to remove pollutants from water.