Self-assembly of asymmetric catalysts

This project aimed to understand the remarkable self-assembling catalysts we had discovered. The mechanistic study was rather challenging and actually involved us having to redesign a new catalyst system that was more amenable for study. this was achieved and a paper that described the exact function of the two-component catalysts was published. A surprising observation made here led us to extrapolate a mechanstic feature in our catalysts to other systems more widely applied that show some similar features. Following on from our first report on such systems, the use of self-assembled organocatalysts is now quite a widespread niche topic.
We actually moved on to consider transition metal catalysts that could also assemble with a rationally designed co-catalyst to deliver a catalyst with enhanced features. Some interesting proof of concepts were established regarding the design of catalysts that are programmed to bind either additives or recognise a secondary binding site on the substrate. Some rather unusual ligands and metal complexes were also successfully synthesised. Attempts to tune these up into genuinely useful processes are still being pursued. Some other speculative studies on activation C-H bonds selectively were less successful. A side effect of these studies was contributing either key intermediates or key information to other projects in catalysis we have been studying, so these reports are also linked here. Overall, this study helped provide a solid foundation for an approach that quite a few chemists now find appealing. It also scoped out what might be achieved with transition metal complexes with bifunctional and trifunctional ligands, solved synthetic challenges in their synthesis, and studied a range of potentially important catalytic protocols.