[ Instrument Network Instrument Development ] Recently, Yang Qihua and Liu Jian, researchers of the State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, have realized the catalytic hydrogenation performance through nano-reactor microenvironment regulation.
The catalytic performance of the enzyme catalyst is directly related to the microenvironment in which the active center is located. However, it is extremely challenging to achieve artificial catalyst activity and selectivity enhancement through precise regulation of the microenvironment.
Hydrogenation of benzoic acid to cyclohexylic acid is an important intermediate process for the industrial production of nylon 6 raw material caprolactam, but metal nanoparticle catalysts are not very active in this reaction, especially in aprotic solvents. In order to increase the catalytic activity of the metal nanoparticles, the team introduced Ru nanoparticles in a nanoreactor modified with organic functional groups such as amino, triphenylphosphine, diphenylphosphine, phenyl. Studies have shown that Ru nanoparticles in phosphine ligand-modified nanoreactors can efficiently catalyze the hydrogenation of benzoic acid in n-hexane, while Ru nanoparticles in other nanoreactors and commercial Ru/C do not exhibit catalytic activity. Theoretical calculations and experimental results show that the modification of phosphine ligands changes the microenvironment of bismuth, and the aromatic ring of benzoic acid is preferentially adsorbed on the surface of Ru metal, thereby enhancing its catalytic performance. At the same time, it was also found that the phosphine ligand-modified nanoreactor can greatly enhance the hydrogenation activity of Ru nanoparticles on benzene, toluene and trifluorotoluene, mainly due to the enhancement of the surface electron density of Ru by the donor effect of phosphine ligands. . The strategy of nanocatalyst microenvironment to regulate catalytic activity and selectivity provides new ideas for the development of efficient catalytic systems.
The work was funded by the National Natural Science Foundation of China and the Chinese Academy of Sciences' Strategic Pilot Science and Technology Pilot of Energy Chemistry (B). It was recently published in the "Angewandte Chemie International Edition" in the form of VIP Paper and inside cover article.
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