期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 -, 期 -, 页码 -出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202308813
关键词
CO Coupling; Carbonyl Ligands; Electronic Structure; Iron; Metal-Metal Interactions
Researchers report a method to couple two CO molecules using a diiron complex, enabling the synthesis of synthetic carbon-neutral fuels. The complex mediates weak exchange interactions with ketenylidene, allowing for changes in spin states and coupling schemes based on DFT calculations, Mossbauer and EPR spectroscopy.
One route to address climate change is converting carbon dioxide to synthetic carbon-neutral fuels. Whereas carbon dioxide to CO conversion has precedent in homo- and heterogeneous catalysis, deoxygenative coupling of CO to products with C C bondsas in liquid fuels-remains challenging. Here, we report coupling of two CO molecules by a diiron complex. Reduction of Fe-2(CO)(2)L (2), where L2- is a bis(ss diketiminate) cyclophane, gives [K(THF)(5)][Fe-2(CO)(2)L] (3), which undergoes silylation to Fe-2(CO)(COSiMe3)L (4). Subsequent C-OSiMe3 bond cleavage and C=C bond formation occurs upon reduction of 4, yielding Fe-2(mu-CCO)L. CO derived ligands in this series mediate weak exchange interactions with the ketenylidene affording the smallest J value, with changes to local metal ion spin states and coupling schemes (ferro- vs. antiferromagnetism) based on DFT calculations, Mossbauer and EPR spectroscopy. Finally, reaction of 5 with KEt3BH or methanol releases the C2O2- ligand with retention of the diiron core
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