Program Description
Catalysis is the study of chemical reactions in which the energy barrier and rate are affected by other substances. Usually in heterogeneous catalytic processes, catalytic substrates (reactants) are reacted on the surface of the catalyst, which involves a series of processes such as adsorption, transport, chemical reactions, and desorption. Catalytic studies usually involve the following.
The structure of the catalyst, especially the surface structure.
The physical adsorption, chemisorption, and diffusion processes of the substrate on the catalyst surface.
Spectroscopic characterization of catalyst, substrate and adsorption structures.
Assessment of catalyst activity and selectivity, which mainly involves reliable validation of the reaction mechanism
Thermodynamics and kinetics of adsorption
Structure of the catalyst, especially the surface structure
Physisorption, chemisorption and diffusion processes of substrates on the catalyst surface
Study of diffusion and structural changes over a range of chemical reaction time and space scales
Spectroscopic characterization
Spectroscopic simulations of catalyst, substrate and adsorption structures and comparison with experiments for better structural analysis
Simulation of UV-Vis, IR, Raman, NMR spectra of molecules, blocks, adsorbed structures, etc.
Reaction mechanism study and rate estimation
Search for possible reaction paths to observe and study reaction processes
Reaction rate study tools that allow direct estimation of reaction rates based on potential barriers
Explore unknown reactions using force field based molecular dynamics
Catalyst activity evaluation
Reaction mechanism reliability verification
Evaluation of catalyst activity and selectivity
Special catalytic systems
Electrocatalysis. Using a unique model it is possible to study the reaction mechanism on the surface of a metal electrode in the presence of an electric field and to predict the catalytic activity
Photocatalysis. Study the arrangement between surface energy levels and catalytic substrate energy levels, and the charge transfer possibilities between them to explore the photocatalytic mechanism
Scientists use cobalt catalysts to achieve carbonylation conversion of ethers
Recently, Wu Xiaofeng, a researcher in the Catalytic Carbonylation Research Group at the Dalian Institute of Chemical Physics, Chinese Academy of Sciences, has made new progress in the carbonylation reaction of ethers, developing a cobalt catalyst to realize the amination carbonylation of ethers. The strategy starts from simple ethers and constructs structurally rich α-amide-substituted ethers under the action of cobalt catalysis.
Ethers are widely found in biomass, chemical feedstocks and fine chemicals, and are bulk chemical feedstocks for the production of value-added chemicals and biomass-derived chemicals. The presence of ethers and their related units can modify the physicochemical properties of the parent molecule, and in addition, cyclic ethers are frequently used as protease inhibitors in drug design to combat viruses. However, due to the inherent inertness of ethers, carbonylation reactions of ethers have not been achieved. Cobalt is a widely used and inexpensive metal catalyst, but it is less frequently used in carbonylation reactions because of the tendency of carbon monoxide to fit closely with cobalt metal to obtain stable carbonylcobalt complexes and the insensitivity of cobalt catalyst activity to the addition of ligands used to adjust the reaction activity. Therefore, it is quite challenging to realize carbonylation reactions of ethers.
A variety of different carbonylation reactions are devoted to the study. In this study, based on the previous work, the research team developed a novel carbonylation strategy – using inert ethers as the carbonylation substrate and inexpensive metallic cobalt as the catalyst to achieve the carbonylation of ethers in the presence of di-tert-butyl peroxide. The study utilized this strategy to construct a series of α-amide-substituted ether derivatives and to obtain the commercially available drug alfuzosin in moderate yields.
The related research results were published in the German Journal of Applied Chemistry under the title Cobalt-Catalyzed Direct Aminocarbonylation of Ethers: Efficient Access to α-Amide Substituted Ether Derivatives. The research work was supported by the Kuan-Cheng Wang Education Fund and other grants.
