Highly Pre-Organized Cooperative Catalysts
We are interested in the development of metal-organic framework (MOF)-based cooperative catalysts, where two or more catalysts interact with the same substrate to facilitate a challenging elementary step. While introducing multiple catalyst-substrate interactions has an obvious beneficial effect on the enthalpy of activation, the need for three or more molecules to be arranged in a particular orientation in the transition structure can render the entropic cost of cooperative catalysis forbidding. Using highly pre-organized catalysts, however, the entropic cost of aligning multiple catalytic centers is paid during synthesis, paving the way to highly efficient catalysis and molecular recognition of reaction substrates.