Zhou Yuanbo, Chen Dongyun, Li Najun, Xu Qingfeng, Li Hua, He Jinghui, Lu Jianmei
Collaborative Innovation Center of Suzhou Nano Science and Technology, College of Chemistry Chemical Engineering and Materials Science Soochow University, 199 Ren'ai Road, Suzhou 215123, PR China.
Collaborative Innovation Center of Suzhou Nano Science and Technology, College of Chemistry Chemical Engineering and Materials Science Soochow University, 199 Ren'ai Road, Suzhou 215123, PR China.
J Colloid Interface Sci. 2022 Feb 15;608(Pt 1):48-59. doi: 10.1016/j.jcis.2021.09.141. Epub 2021 Sep 25.
A series of hollow multi-shelled CeO (HoMS-CeO) support materials with tunable shell numbers were fabricated and applied to the catalytic oxidation of toluene. HoMS-CeO possess much higher catalytic activity (T = 236 ℃) than hollow CeO with only a single shell (h-CeO) (T = 275℃). The porous multiple-shelled structure has a higher S, which strongly promotes gas distribution and provides more active sites. The superiority of this kind of structure was also verified by comparing h-CoO and HoMS-CoO. Furthermore, Pt-Co bimetallic nanoparticles were loaded onto HoMS-CeO. The synergistic effect between Pt and Co was verified by XPS and O-TPD, which was observed to allow electron transfer between Pt and Co and thus regulate the electronic state of the Pt. Compared with Pt alone, Pt-Co bimetallic nanoparticles could stronglypromotethe activation of Oand oxygen mobility, as revealed by a much higher O content and a lower oxygen desorption temperature. Of the catalysts prepared in this study, the 1 wt% PtCo/CeO catalyst was found to be the most suitable for toluene oxidation owing to its excellent activity (T = 158 ℃), long-term stability, and water resistance. Finally, in situ DRIFTS was employed to investigate mechanism during toluene oxidation and the possible reaction pathway was proposed.
制备了一系列壳层数可调的中空多壳层CeO（HoMS-CeO）载体材料，并将其应用于甲苯的催化氧化。HoMS-CeO的催化活性（T = 236℃）比仅具有单壳层的中空CeO（h-CeO）（T = 275℃）高得多。多孔多壳层结构具有更高的比表面积（S），这极大地促进了气体分布并提供了更多的活性位点。通过比较h-CoO和HoMS-CoO也证实了这种结构的优越性。此外，将Pt-Co双金属纳米颗粒负载到HoMS-CeO上。通过XPS和O-TPD证实了Pt和Co之间的协同效应，观察到这种协同效应允许Pt和Co之间进行电子转移，从而调节Pt的电子状态。与单独的Pt相比，Pt-Co双金属纳米颗粒可以强烈促进O的活化和氧迁移，这通过更高的O含量和更低的氧脱附温度得以体现。在本研究制备的催化剂中，1 wt% PtCo/CeO催化剂因其优异的活性（T = 158℃）、长期稳定性和耐水性而被发现最适合甲苯氧化。最后，采用原位漫反射红外傅里叶变换光谱（in situ DRIFTS）研究甲苯氧化过程中的机理，并提出了可能的反应途径。
