Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 134, Issue 42, Pages 17653-17660Publisher
AMER CHEMICAL SOC
DOI: 10.1021/ja306913x
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Funding
- NSF of China [20890123, 20821140537, 21073043, 21073040]
- State Key 973 Program of PRC [2012CB224805]
- Shanghai Leading Academic Discipline Project [B108]
- Science & Technology Commission of Shanghai Municipality [08DZ2270500, 10jc1401800]
- program of New Century Excellent Talents [NCET-08-0126]
- Innovation Program of Shanghai Municipal Education Commission [13ZZ004]
- Shanghai Rising Star Project of STCSM [12QH1400300]
- National Basic Research Program of China [2012CB224804]
- TOTAL Cor
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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 nano-composites have a 2-D hexagonally arranged pore structure, uniform pore size (similar to 4.0 nm), high surface area (similar to 500 m(3)/g), moderate pore volume (similar to 0.30 cm(3)/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-Tropsch synthesis results show that as the size of iron nanoparticles decreases, the mesoporous Fe-carbon 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.
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