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2023-09-19 14:58:05 | onclick: | Modified activated carbon as carrier!Improves catalytic activity under mild conditions

Recently, researcher Ding Yunjie, researcher Yan Li and researcher Song Xiangen of Dalian Institute of Chemical Physics, Chinese Academy of Sciences, made new progress in the study of polyphase carbonylation of methanol.The team systematically studied the polyphase methanol carbonylation of Rh mononuclear complex catalysts with modified activated carbon as the carrier.It was found that the nitrogen and sulfur co-modified activated carbon not only stabilized the anchoring of single metal site Rh, but also improved the catalytic activity under milder reaction conditions.Relevant results are published in Advanced Functional Materials.
Schematic diagram of the study of polyphase carbonylation of methanol.Dalian chemical supply map
The team developed a general strategy for dispersing precious metal nanoparticles into loaded mononuclear complexes by combining carbon monoxide and alkyl halide, which solved the problems of traditional multiphase catalysts in atomic utilization, stability and activity.Afterwards, the team systematically studied the anti-sulfur toxicity of Rh mononuclear complex, and combined with the analysis of in situ reaction mass spectrometry of Dalian coherent light source, the reaction energy barrier was reduced to 10.0 kJ/mol.
Based on the above research background and foundation, the team used nitrogen and sulfur to modify the surface of activated carbon, developed ligand configuration and stereo effect controllable carrier modification strategy.The catalyst prepared by the team showed an 88% methanol conversion rate and a reaction activity of 2812h-1.The results show that the introduction of nitrogen and sulfur modulates the electron cloud density around the active metal Rh and reduces the oxidation addition of iodomethane to 0.49eV.
By modifying the catalyst carrier to regulate the metal coordination environment, this work provides a new idea for constructing high performance single metal site active catalyst.

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