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Carbon dioxide hydrogenation catalysed by well-defined Mn(I) PNP pincer hydride complexes

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Abstract

The catalytic reduction of carbon dioxide is of great interest for its potential as a hydrogen storage method and to use carbon dioxide as C-1 feedstock. In an effort to replace expensive noble metal-based catalysts with efficient and cheap earth-abundant counterparts, we report the first example of Mn(I)-catalysed hydrogenation of CO2 to HCOOH. The hydride Mn(I) catalyst [Mn(PNPNH-iPr)(H)(CO)2] showed higher stability and activity than its Fe(II) analogue. TONs up to 10 000 and quantitative yields were obtained after 24 h using DBU as the base at 80 °C and 80 bar total pressure. At catalyst loadings as low as 0.002 mol%, TONs greater than 30 000 could be achieved in the presence of LiOTf as the co-catalyst, which are among the highest activities reported for base-metal catalysed CO2 hydrogenations to date.

Graphical abstract: Carbon dioxide hydrogenation catalysed by well-defined Mn(i) PNP pincer hydride complexes

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Publication details

The article was received on 15 Jan 2017, accepted on 28 Apr 2017 and first published on 04 May 2017


Article type: Edge Article
DOI: 10.1039/C7SC00209B
Citation: Chem. Sci., 2017, Advance Article
  • Open access: Creative Commons BY-NC license
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    Carbon dioxide hydrogenation catalysed by well-defined Mn(I) PNP pincer hydride complexes

    F. Bertini, M. Glatz, N. Gorgas, B. Stöger, M. Peruzzini, L. F. Veiros, K. Kirchner and L. Gonsalvi, Chem. Sci., 2017, Advance Article , DOI: 10.1039/C7SC00209B

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