A General Chelate-Assisted Co-Assembly to Metallic Nanoparticles-Incorporated Ordered Mesoporous Carbon Catalysts for Fischer鈥揟ropsch Synthesis

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• 作者：Zhenkun Sun ; Bo Sun ; Minghua Qiao ; Jing Wei ; Qin Yue ; Chun Wang ; Yonghui Deng ; Serge Kaliaguine ; Dongyuan Zhao
• 刊名：The Journal of the American Chemical Society
• 出版年：2012
• 出版时间：October 24, 2012
• 年：2012
• 卷：134
• 期：42
• 页码：17653-17660
• 全文大小：460K
• 年卷期：v.134,no.42(October 24, 2012)
• ISSN：1520-5126

文摘

The organization of different nano objects with tunable sizes, morphologies, and functions into integrated nanostructures is critical to the development of novel nanosystems that display high performances in sensing, catalysis, and so on. Herein, using acetylacetone as a chelating agent, phenolic resol as a carbon source, metal nitrates as metal sources, and amphiphilic copolymers as a template, we demonstrate a chelate-assisted multicomponent coassembly method to synthesize ordered mesoporous carbon with uniform metal-containing nanoparticles. The obtained nanocomposites have a 2-D hexagonally arranged pore structure, uniform pore size (4.0 nm), high surface area (500 m²/g), moderate pore volume (0.30 cm³/g), uniform and highly dispersed Fe₂O₃ nanoparticles, and constant Fe₂O₃ contents around 10 wt %. By adjusting acetylacetone amount, the size of Fe₂O₃ nanoparticles is readily tunable from 8.3 to 22.1 nm. More importantly, it is found that the metal-containing nanoparticles are partially embedded in the carbon framework with the remaining part exposed in the mesopore channels. This unique semiexposure structure not only provides an excellent confinement effect and exposed surface for catalysis but also helps to tightly trap the nanoparticles and prevent aggregating during catalysis. Fischer鈥揟ropsch synthesis results show that as the size of iron nanoparticles decreases, the mesoporous Fe鈥揷arbon nanocomposites exhibit significantly improved catalytic performances with C₅₊ selectivity up to 68%, much better than any reported promoter-free Fe-based catalysts due to the unique semiexposure morphology of metal-containing nanoparticles confined in the mesoporous carbon matrix.