Manganese-Mediated Formic Acid Dehydrogenation |
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| Authors: | Dr. Nickolas H. Anderson Dr. James Boncella Dr. Aaron M. Tondreau |
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| Affiliation: | Chemistry Division, Los Alamos National Laboratory, MS J514, Los Alamos, New Mexico, 87545 USA |
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| Abstract: | A robust and rapid manganese formic acid (FA) dehydrogenation catalyst is reported. The manganese is supported by the recently developed, hybrid backbone chelate ligand tBuPNNOP (tBuPNNOP=2,6-(di-tert-butylphosphinito)(di-tert-butylphosphinamine)pyridine) ( 1 ) and the catalyst is readily prepared with MnBrCO5 to form [(tBuPNNOP)Mn(CO)2][Br] ( 2 ). Dehydrohalogenation of 2 generated the neutral five coordinate complex (tBuPNNOP)Mn(CO)2 ( 3 ). Dehydrogenation of FA by 2 and 3 was found to be highly efficient, exhibiting turnover frequencies (TOFs) exceeding 8500 h−1, rivaling many noble metal systems. The parent chelate, tBuPONOP (tBuPONOP=2,6-bis(di-tert-butylphosphinito)pyridine) or tBuPNNNP (tBuPNNNP=2,6-bis (di-tert-butylphosphinamine)pyridine), coordination complexes of Mn were synthesized, respectively affording [(tBuPONOP)Mn(CO)2][Br] ( 4 ) and [(tBuPNNNP)Mn(CO)2][Br] ( 5 ). FA dehydrogenation with the hybrid-ligand supported 2 exhibits superior catalysis to 4 and 5 . |
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| Keywords: | catalysis dehydrogenation formic acid manganese PNNOP |
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