ynthetic chemistry is critical to fields from biomedicine to industrial chemistry. In multiple reaction steps, new compounds can be formed through functionalization of existing ones. Catalytic functionalization of carbon-hydrogen (C-H) bonds is an intense area of research. The range of substrates is virtually limitless, including hydrocarbons, complex organic compounds, and synthetic and biological polymers. C-H functionalization based on this unlimited repertoire of starting points is believed to have the potential to revolutionize the synthesis of complex molecules. The key challenge in unleashing this potential is the extreme stability of the non-activated C-H bonds in these substrates. The EU-funded CUBE project is bringing together insights from multiple research fields addressing copper-containing biological and synthetic catalysts that can activate such C-H bonds in a controlled manner. This cross-fertilization is expected to lead to novel catalysts with unprecedented catalytic benefits.
he 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 by translating the acquired knowledge into rationally designed new synthetic and biological catalysts with unprecedented activity, selectivity and turn-over numbers.
CuBE will capitalize on the recent discovery of abundant and experimentally accessible natural enzymes (lytic polysaccharide monooxygenases, or 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. 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 the activation of oxidant such as O2, N2O and H2O2, and of the subsequent C-H bond activation. Emerging design principles from these studies will be used to evolve new catalysts, including engineered enzymes and MOFs. To enable these efforts, we will develop novel spectroscopic and computational approaches.
The project brings together leading players in complementary fields: design, synthesis and testing of synthetic 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.