Unravelling the secrets of Cu-based catalysts for C-H activation

Unravelling the secrets of Cu-based catalysts for C-H activation

The Holy Grail of selective C-H activation has been vigorously pursued for more than 70 years in all areas of catalysis - homogeneous, heterogeneous and biological - yet with scarce cross-fertilization. CUBE will bridge this gap, by synergistically disclosing the secrets of Cu-containing biological and synthetic catalysts and translating the acquired knowledge into rationally designed new catalysts with unprecedented activity, selectivity and turn-over numbers. CUBE will capitalize on the recent discovery of abundant and experimentally accessible natural enzymes (LPMOs) that activate resilient C-H bonds using a mono-Cu catalytic center, thus providing a biological analogue to synthetic Cu-zeolites. CUBE will also harness the potential of metal-organic frameworks (MOFs), which offer unprecedented (“enzyme-like”) flexibility in catalyst development. C-H activating Cu-containing Zr-MOFs have just been described. CUBE will generate trans-disciplinary insights into Cu-based catalysts to progress beyond the state of the art in C-H activation. To this aim, we will elucidate the key mechanistic features of oxidant activation by O2, as well as N2O and H2O2, and then C-H activation. Emerging design principles from these studies will evolve new catalysts, including engineered enzymes, enzyme-polymer hybrid materials, and MOFs. To enable these efforts, we will develop novel methodologies at the interface of spectroscopy and computational chemistry. The project brings together leading players in complementary fields: design, synthesis and testing of catalysts (UiO), enzymology and protein engineering (NMBU), spectroscopic investigations of heterogeneous catalysts (UoT) and spectroscopic/computational studies of homogeneous and biological catalysts (MPI). Through a work-plan conceived to maximize cross-fertilization within the project team, we will design and develop novel catalysts for tomorrow’s C-H activation chemistry.