NHC-containing manganese(I) electrocatalysts for the two-electron reduction of CO2

Jay Agarwal, Travis W. Shaw, Charles J. Stanton, George F. Majetich, Andrew Bruce Bocarsly, Henry F. Schaefer

Research output: Contribution to journalArticle

84 Scopus citations

Abstract

The synthesis and characterization of the first catalytic manganese N-heterocyclic carbene complexes are reported: MnBr(N-methyl-N'-2- pyridylbenzimidazol-2-ylidine)(CO)3 and MnBr(N-methyl-N'-2- pyridylimidazol-2-ylidine)(CO)3. Both new species mediate the reduction of CO2 to CO following two-electron reduction of the MnI center, as observed with preparative scale electrolysis and verified with 13CO2. The two-electron reduction of these species occurs at a single potential, rather than in two sequential steps separated by hundreds of millivolts, as is the case for previously reported MnBr(2,2'-bipyridine)(CO)3. Catalytic current enhancement is observed at voltages similar to MnBr(2,2'-bipyridine)(CO)3. Catalytic manganese N-heterocyclic carbene complexes have been synthesized and characterized: [MnBrL(CO)3] (see scheme; L=N-methyl-N'-2- pyridylbenzimidazol-2-ylidine or N-methyl-N'-2-pyridylimidazol-2-ylidine). Both species mediate the reduction of CO2 to CO following two-electron reduction of the MnI center at a single potential, as observed with preparative scale electrolysis and verified with 13CO2.

Original languageEnglish (US)
Pages (from-to)5152-5155
Number of pages4
JournalAngewandte Chemie - International Edition
Volume53
Issue number20
DOIs
StatePublished - May 12 2014

All Science Journal Classification (ASJC) codes

  • Catalysis
  • Chemistry(all)

Keywords

  • N-heterocyclic carbenes
  • carbon dioxide
  • catalysis
  • electrochemistry
  • manganese

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