Applied Catalysis B: Environmental, Vol.250, 337-346, 2019
Highly efficient visible-light-driven photocatalytic degradation of VOCs by CO2-assisted synthesized mesoporous carbon confined mixed-phase TiO2 nanocomposites derived from MOFs
Improving the visible light response and efficient separation of electron-hole pairs play vital roles in commonly used TiO2 photocatalyst for VOCs degradation. Herein, N-doped mesoporous carbon encapsulated anatase-rutile phase junction TiO2 (TiO2@C-N(x)) was successfully synthesized via the pyrolysis of a representative amine functionalized Ti-based MOF, NH2-MIL-125, under the atmosphere of Ar and subsequent CO2 treatment. Our synthesis stragety was based on the rational regulation of the formation of TiO2 phase junction and the decomposition of amorphous carbon onto the TiO2@C-N (without subsequent CO2 process) using CO2 as both anatase-rutile phase transformation promoter and mild oxidant. Compared with TiO2@C-N, TiO2@C-N(x) nanocomposites with subsequent CO2 process exhibit significantly improved photocatalytic activity as well as mineralization efficiencies. For example, the mineralization efficiency reached 51.9% at 62.4% of styrene degradation within 240 min of visible-light irradiation by using the optimal TiO2@C-N(30) nanocomposites as compared with only 19.7% mineralization efficiency at 31.0% of styrene degradation under the same conditions of TiO2@C-N. Furthermore, the primary radicals involved in degradation of VOCs was identified by electron paramagnetic resonance spectroscopy, and the possible degradation intermediates were also monitored by means of proton transfer reaction time-of-flight mass spectrometry (PTR-ToF-MS). Finally, the radicals involved degradation reaction mechanism was also tentatively proposed.