Widenhoefer and Craig Labs Team Up to Make Advances in Further Understanding of Mechanically Coupled Ligand Effects in Catalysis

Chemical optimization and Mechanically coupled optimization of reactants. Upper portion appears as green, purple, blue and yellow ziti pasta with yellow and purple circles. Bottom half appears as zig zag spaghetti noodles with green and purple ziti noodles underneath
a, Changing ligand (X-shaped unit), metal (m), solvent, temperature or pressure (white box). Colour differences in the catalyst complex represent different ligand or metal environments. b, Coupling the catalyst complex (same X-shaped unit and m) to variable tension in a supporting polymer matrix (grey lines represent first network; orange lines represent second network polymer). R and S indicate the enantiomeric forms of the product.

We love a collaboration!! The Widenhoefer and Craig Labs have teamed up to describe what they term multi-state mechanocatalysis (MMC), which they believe is the first demonstration that externally applied mechanical forces can be directed through a polymer network into single-site catalysts, using those forces to bias the outcome of a catalytic reaction. In a sense, MMC can be thought of as top-down atomic manipulation—pushing and pulling molecules into the optimal shape for a desired function (here, catalysis). The MMC is constructed so that when a polymer network is stretched or deformed, the distribution of conformational states accessed by an embedded catalyst during the catalytic reaction is changed. Because the polymer can be stretched and deformed both incrementally and reversibly, MMCs offer the potential to tune selectivity and/or reactivity (in this case, enantioselective hydrogenation) within a single catalytic scaffold. Learn more about their recent findings in Nature Synthesis, available here.