材料科学
介孔材料
傅里叶变换红外光谱
催化作用
魔角纺纱
扫描透射电子显微镜
扫描电子显微镜
反应性(心理学)
介孔二氧化硅
光谱学
化学工程
核磁共振波谱
化学
有机化学
复合材料
病理
工程类
物理
医学
替代医学
量子力学
作者
Xingjie Wang,Zoha H. Syed,Zhijie Chen,J. David Bazak,Xinyi Gong,Megan C. Wasson,Nancy M. Washton,Karena W. Chapman,Justin M. Notestein,Omar K. Farha
标识
DOI:10.1021/acsami.2c15046
摘要
To increase catalytic efficiency, mesoporous supports have been widely applied to immobilize well-defined metal oxide clusters due to their ability to stabilize highly dispersed clusters. Herein, a redox-active heterometallic Ce12V6-oxo cluster (CeV) was first presynthesized and then incorporated into mesoporous silica, SBA-15, via a straightforward impregnation method. Scanning transmission electron microscopy (STEM) and Fourier transform infrared spectroscopy (FTIR), in concert with scanning electron microscopy and energy-dispersive X-ray spectroscopy (SEM-EDS), verified the successful introduction of the CeV cluster inside the pore of SBA-15. The 51V magic angle spinning solid-state nuclear magnetic resonance (51V MAS NMR) spectroscopy and differential pair distribution function (dPDF) analysis confirmed the structural integrity of the CeV cluster inside the SBA-15. The composite was then benchmarked for liquid-phase oxidation of 2-chloroethyl ethyl sulfide (CEES) under mild conditions and gas-phase oxidative dehydrogenation (ODH) of propane under high temperatures (up to 550 °C). The catalytic reactivity results demonstrated 8- and 14-fold increase in turnover frequency (TOF) values of the composite (CeV@10SBA-2) than the bulk CeV cluster under the same conditions for CEES oxidation and ODH, respectively. These results highlight the improved reactivity of the catalytically active CeV cluster as attributed to the higher dispersion of the discrete cluster upon immobilization within the SBA-15 support.
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