We are interested in the design of catalysts that reverse traditional definitions of reactivity by selectively transforming “less reactive” substrates in the presence of “more reactive” molecules.
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.
All nanostructures are inherently thermodynamically unstable with respect to the bulk solid. But the kinetic stability that can be achieved with even very small nanoparticles given suitable support materials can make supported nanoparticles efficient and practical heterogeneous catalysts. Stability concerns are, however, exacerbated for alloy nanoparticles that are composed of metals with unfavorable mixing enthalpies. We are interested in the development of efficient strategies for the synthesis of this promising class of catalysts and their stabilization under forcing reaction conditions.
We are interested in the design of support materials that not only lead to long-lived highly active catalysts, but take an active role in controlling the outcome of a catalytic transformation. Given the ubiquitous nature of catalyst support materials in heterogeneous catalysis, the development of novel materials that enhance the intrinsic selectivity of the catalytically active material can impact a wide range of catalytic processes.