College of Environmental Science and Engineering, Hunan University, Changsha 410082, PR China; Key Laboratory of Environmental Biology and Pollution Control, Hunan University, Ministry of Education, Changsha 410082, PR China.
College of Environmental Science and Engineering, Hunan University, Changsha 410082, PR China; Key Laboratory of Environmental Biology and Pollution Control, Hunan University, Ministry of Education, Changsha 410082, PR China.
J Hazard Mater. 2023 Jun 15;452:131249. doi: 10.1016/j.jhazmat.2023.131249. Epub 2023 Mar 22.
Transition metal oxides have high photothermal conversion capacity and excellent thermal catalytic activity, and their photothermal catalytic ability can be further improved by reasonably inducing the photoelectric effect of semiconductors. Herein, MnO/CoO composites with S-scheme heterojunctions were fabricated for photothermal catalytic degradation of toluene under ultraviolet-visible (UV-Vis) light irradiation. The distinct hetero-interface of MnO/CoO effectively increases the specific surface area and promotes the formation of oxygen vacancies, thus facilitating the generation of reactive oxygen species and migration of surface lattice oxygen. Theoretical calculations and photoelectrochemical characterization demonstrate the existence of a built-in electric field and energy band bending at the interface of MnO/CoO, which optimizes the photogenerated carriers' transfer path and retains a higher redox potential. Under UV-Vis light irradiation, the rapid transfer of electrons between interfaces promotes the generation of more reactive radicals, and the MnO/CoO shows a substantial improvement in the removal efficiency of toluene (74.7%) compared to single metal oxides (53.3% and 47.5%). Moreover, the possible photothermal catalytic reaction pathways of toluene over MnO/CoO were also investigated by in situ DRIFTS. The present work offers valuable guidance toward the design and fabrication of efficient narrow-band semiconductor heterojunction photothermal catalysts and provides deeper insights into the mechanism of photothermal catalytic degradation of toluene.
过渡金属氧化物具有较高的光热转换能力和优异的热催化活性,通过合理诱导半导体的光电效应,可以进一步提高其光热催化能力。在此,我们制备了具有 S 型异质结的 MnO/CoO 复合材料,用于在紫外-可见(UV-Vis)光照射下光热催化降解甲苯。MnO/CoO 的明显异质界面有效增加了比表面积,并促进了氧空位的形成,从而有利于活性氧物种的生成和表面晶格氧的迁移。理论计算和光电化学表征表明,MnO/CoO 界面存在内置电场和能带弯曲,优化了光生载流子的转移路径,并保留了更高的氧化还原电位。在 UV-Vis 光照射下,界面间电子的快速转移促进了更多活性自由基的生成,MnO/CoO 对甲苯的去除效率(74.7%)相较于单一金属氧化物(53.3%和 47.5%)有显著提高。此外,还通过原位 DRIFTS 研究了 MnO/CoO 上甲苯的可能光热催化反应途径。本工作为设计和制备高效窄带半导体异质结光热催化剂提供了有价值的指导,并深入了解了甲苯的光热催化降解机制。