This proposal addresses a clearly urgent need to develop novel homogeneous catalysts for the asymmetric hydrogenation of ketones with hydrogen gas, as a green, energy- and cost-efficient alternative to the currently used protocols. Instead of precious metals, we attempt to utilize transition metal complexes based on environmentally benign, inexpensive and non-toxic iron. First examples in the asymmetric hydrogenation using iron complexes are a promising indication that efficient systems might in principle become viable with further catalyst development and by careful selection of ligands and reaction conditions. Based on an extensive initial catalyst screening, well-defined complexes of two different classes will be designed and synthetized: 1) Complexes of general formula [Fe(P-P)(N-N)X2], which feature two bidentate ligands structurally related to the known PNNP tetradentate systems; 2) Piano-stool Fe complexes containing pendant H-donor groups as well as strongly electron-donating chiral carbene ligands. Recognizing and addressing the expected challenges, mainly related to transitioning from precious metals such as ruthenium or rhodium to a first row alternative will largely contribute to the basic scientific knowledge in this field.
The most promising catalysts will be subsequently applied in the transformation of biomass-derived ketones originating from the oxidative disassembly of lignin, therefore this proposal offers various multidisciplinary aspects while relying on solid background in classical asymmetric catalysis. In case of success this research will contribute to the transition towards a sustainable society in multiple ways.
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