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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

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

Geoff Cloke

CPD Conference June 22nd 2012


The carbon cycle

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

Sandwiches!


Why uranium

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

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 n 2

The Oxocarbons (CO)n2-


The next one in the series squarate

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

+

Carbon Dioxide Activation

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


Activating carbon monoxide and carbon dioxide with organometallic uranium complexes closing the carbon cycle

Carbon Dioxide Activation 2

Nikos Tsoureas, unpublished results 2012


Coupling of nitric oxide and carbon monoxide

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

“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

The Future…..

Chemically?

Electrochemically- controlled potential electrolysis?


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