Mechanochemical Synthesis of Ruthenium Cluster@Ordered Mesoporous Carbon Catalysts by Synergetic Dual Templates |
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Authors: | Prof. Li Wang Jiahua Zhao Prof. Pengfei Zhang Dr. Shize Yang Prof. Wangcheng Zhan Prof. Sheng Dai |
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Affiliation: | 1. Institute of Industrial Catalysis, East China University of, Science and Technology, Shanghai, 200237 P. R. China;2. School of Chemistry and Chemical Engineering, Shanghai Jiao Tong University, Shanghai, 200240 P. R. China;3. Oak Ridge National Laboratory, Oak Ridge 37831, TN USA;4. Department of Chemistry, University of Tennessee, Knoxville, 37996 USA |
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Abstract: | Ruthenium (Ru)@Ordered mesoporous carbon (OMC) is a key catalyst in fine-chemical production. In general, the OMC support is prepared by a wet self-assembly requiring excessive solvent, toxic phenol–aldehyde precursors and a long reaction time, followed by post-immobilization to load Ru species. Herein, we wish to report a solid-state, rapid, and green strategy for the synthesis of Ru@OMC with biomass tannin as the precursor. The chemistry essence of this strategy lies in the mechanical-force-driven assembly, during which tannin-metal (Zn2+ and Ru3+) coordination polymerization and hydrogen-bonding interactions between tannin-block copolymer (PEO-PPO-PEO, F127) simultaneously occur. After thermal treatment, Ru@OMC catalysts with mesoporous channels, narrow pore-size distribution (≈7 nm), and high surface area (up to 779 m2 g−1) were directed by F127 micelles. Meanwhile, the Zn2+ ions dilute Ru3+ and avoid the sintering of Ru species, resulting in Ru clusters around 1.4–1.7 nm during carbonization (800 °C). Moreover, the Ru@OMC catalyst afforded a good activity (TOF: up to 4170 h−1) in the selective oxidation of benzyl alcohol to benzaldehyde by molecular oxygen. |
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Keywords: | mechanochemical synthesis mesoporous materials ordered mesoporous carbon ordered mesoporous catalysts selective oxidation |
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