Lei Zhao,Baoyue Zhang,Xin Xiao,Feng Long Gu,Rui-Qin Zhang
Active species such as holes, electrons, hydroxyl radicals ( OH), and superoxide radical anions ( O 2 − ) involved in the photocatalytic oxidation of benzyl alcohol (BA) into benzaldehyde (BAD) on TiO 2 under ultraviolet (UV) light were investigated by adding corresponding scavengers. The experimental results show that the oxidation of BA into BAD is driven mainly by the holes and OH radical. The role of dissolved O 2 was studied by bubbling N 2 through the reaction. The results show that the dissolved O 2 is, to some extent, the source of OH. Additional density functional theory (DFT) calculations identified two H-abstraction pathways ( R abs OH and R abs α). The structure of the R abs OH product is less stable and tends to transfer resulting in the R abs α product. The holes are the main driving force for the abstracting of H from BA. The OH radical combines with the H-abstract product to form a precursor of product BAD, detected by LC–MS technique ( m / z 123), which then undergoes an intramolecular dehydration reaction to form BAD. The results will help to select the optimal active species for the photocatalytic oxidation of BA into BAD on TiO 2 under UV light.
Wang Yongqiang,Bai Yibo,Han Che,Li Zaimei,Lun Xiaowen,Zhang Conglu
Graphite-like carbon nitride (g-C 3 N 4 ) is favored for its excellent physicochemical properties. However, the high complexation rate of photogenerated carriers greatly limits its practical applications. Based on this, a novel CQDs-doped carbon nitride nanosheets composite (CNS/CQDs) was prepared and applied to the visible light–induced activation of peroxymonosulfate (PMS) for meloxicam (Mel) and tetracycline (TC) degradation. The photocatalytic degradation of Mel and TC were remarkably promoted in the CNS/CQDs+PMS+vis system. Mel photodegradation of 99.90% was achieved over 30 min with 20 mg CNS/CQDs and 20 mg PMS at pH11. And TC photodegradation of 95.97% was achieved over 45 min with 20 mg CNS/CQDs and 20 mg PMS at nature pH6.5. The TOC mineralization rates of Mel and TC were 75.49% and 52.00%, respectively. The transient photocurrent response and electrochemical impedance measurements (EIS) results indicated that the doping of CQDs could improve the charge transfer efficiency of pure g-C 3 N 4 , and CNS/CQDs had a low charge transfer resistance. Capture experiments and EPR tests explored the effective actives in the CNS/CQDs+PMS+vis system. Possible degradation pathways of Mel were also analyzed. This study provides valid residual drugs degradation under the dual conditions of visible light catalytic oxidation and persulfate oxidation, which will be a novel perspective for advanced oxidation technology to effectively remove organic pollutants from water.