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"Activating Carbon Monoxide and Carbon Dioxide with Organometallic Uranium Complexes- Closing the Carbon Cycle" PowerPoint PPT Presentation


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"Activating Carbon Monoxide and Carbon Dioxide with Organometallic Uranium Complexes- Closing the Carbon Cycle". Geoff Cloke. CPD Conference June 22 nd 2012. The Carbon Cycle. ~80 % of current global energy supply depends on fossil fuels End product of combustion is CO 2

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"Activating Carbon Monoxide and Carbon Dioxide with Organometallic Uranium Complexes- Closing the Carbon Cycle"

Geoff Cloke

CPD Conference June 22nd 2012


The Carbon Cycle

  • ~80 % of current global energy supply depends on fossil fuels

  • End product of combustion is CO2

  • Oil reserves are finite- peak oil will occur

“Uncertainty in petroleum cost and supply demands that alternative sources of primary organic materials be developed. Carbon monoxide as a component of synthesis gas (H2 + CO) from coal and biomass will have a leading role in meeting these needs. ..........develop strategies that use CO as a two-carbon or larger building block to construct the organic materials needed for fuels and chemical manufacturing.”

Wayland, Science, 2006

Create C-C bonds and/or C-H bonds from CO or CO2

C≡O 1070 kJ/mol

O=C=O 800 kJ/mol


Sandwiches!


Why Uranium ??

Uranium(III)- highly reducing

UIV/III: E½ = -2.18 V

E / volts

What to do with all the depleted uranium??!

U235 0.7%

U238 99.3%

5,404,000 tonnes!


Cyclisation of Carbon Monoxide

O. T. Summerscales, F. G. N. Cloke, P. B. Hitchcock, J. C. Green, and N. Hazari,Science, 2006, 311, 829.


The Oxocarbons (CO)n2-


O. T. Summerscales, F. G. N. Cloke, P. B. Hitchcock, J. C. Green, and N. Hazari, J.Am.Chem. Soc, 2006, 128, 9602.

The Next One in the Series- Squarate


+

Carbon Dioxide Activation

A.S.P. Frey, O.T. Summerscales, F.G.N. Cloke, M.P. Coles, P.B. Hitchcock, Chem.Commun., 2009


Carbon Dioxide Activation 2

Nikos Tsoureas, unpublished results 2012


Coupling of Nitric Oxide and Carbon Monoxide

> 6000C

>2000C<3000C

+

CO

NO

+

A.S.P.Frey, F.G.N.Cloke,

M.P.Coles, P.B.Hitchcock,

Chem. Eur. J.,2010, 16, 9305.


“Methanol Synthesis”

A.S. P. Frey, F. G. N. Cloke, M. P. Coles, L. Maron, and T. Davin, Angew. Chem. Int. Ed.2011, 50, 6881


The Future…..

Chemically?

Electrochemically- controlled potential electrolysis?


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