Cui Yan, Chen Yusheng, Cao Zhen, Xu Leilei, He Jing, Zhu Zehui, Lian Linshui, Luo Xue, Yang Zhenya, Chen Mindong
Collaborative Innovation Centre of the Atmospheric Environment and Equipment Technology, School of Environmental Science and Engineering, Nanjing University of Information Science & Technology, Jiangsu Key Laboratory of Atmospheric Environment Monitoring and Pollution Control, 210044 Nanjing, China.
Jiangsu Environmental Engineering Technology Co., Ltd., Nanjing 210004, China.
Inorg Chem. 2024 Oct 21;63(42):19972-19990. doi: 10.1021/acs.inorgchem.4c03562. Epub 2024 Oct 8.
In this study, the novel Pt-embedded mesoporous CeO hollow nanospheres (Pt-MS-CeO-H) with varying Pt contents (0.5-3.0 wt %) were facilely prepared. The Pt nanoparticles were one-pot embedded within the mesoporous shell of Pt-MS-CeO-H and assisted with the reduction Ostwald ripening process. The traditional preparation methods often face challenges, such as the uneven distribution or aggregation of nanoparticles, as well as difficulty in maintaining high catalytic activity at low Pt content. Compared with the traditional supported Pt/MS-CeO catalyst, the embedding strategy facilitated precise control over the position, distribution, and uniformity of Pt nanoparticles within the CeO mesoporous shell. Additionally, the encapsulation process of Pt nanoparticles played a pivotal role in generating oxygen vacancies and activating surface chemical adsorption of oxygen. Resultantly, the toluene oxidation performances of 1Pt-MS-CeO-H catalyst showed much lower (171 °C) than 1Pt/MS-CeO (311 °C). To elucidate the underlying reasons, in situ diffuse reflectance infrared Fourier transform spectroscopy of toluene oxidation was employed to identify the reaction intermediates and pathways over these catalysts. In summary, the Pt-embedded mesoporous CeO hollow nanosphere catalysts were considered as potential candidates when designing high-performance toluene catalytic oxidation catalysts.
在本研究中,我们轻松制备了具有不同Pt含量(0.5 - 3.0 wt%)的新型Pt嵌入介孔CeO空心纳米球(Pt-MS-CeO-H)。Pt纳米颗粒通过一锅法嵌入到Pt-MS-CeO-H的介孔壳层中,并辅助奥斯特瓦尔德熟化过程的还原。传统制备方法常常面临挑战,比如纳米颗粒分布不均或聚集,以及在低Pt含量下难以保持高催化活性。与传统的负载型Pt/MS-CeO催化剂相比,这种嵌入策略有助于精确控制Pt纳米颗粒在CeO介孔壳层中的位置、分布和均匀性。此外,Pt纳米颗粒的封装过程在产生氧空位和激活氧的表面化学吸附方面发挥了关键作用。结果,1Pt-MS-CeO-H催化剂的甲苯氧化性能(171°C)比1Pt/MS-CeO(311°C)低得多。为了阐明其潜在原因,采用甲苯氧化的原位漫反射红外傅里叶变换光谱来识别这些催化剂上的反应中间体和反应途径。总之,在设计高性能甲苯催化氧化催化剂时,Pt嵌入介孔CeO空心纳米球催化剂被视为潜在的候选材料。