1. Fundamental Properties of Surface Sys
Tailoring surface chemical properties using electronic structure theory
Frank Abild-Pedersen

2. Energy efficient fuel synthesis
Sustainable energy through catalysis
Energy efficient fuel synthesis
Better catalysts required
Efficient
Stable
Made from Earth-abundant elements

3. SUNCAT mission
To develop understanding of interface phenomena
To develop science-based design of catalysts
To apply methods to interfaces of interest in energy transformations
To close the theory-synthesis - characterization-test loop

4. Top-down approach Nørskov, Bligaard, Rossmeisl, Christensen
Nature Chem. 1, 37 (2009)

5. Syngas to fuels
Less sensitivity to feed stock compared to other bio-routes. Anything can be gasified.
Syn
CO + H2
National Energy Technology Laboratory:
Williams, R. H. et. al.; Energy Sust. Dev.; 1; 18-34; 1995
Methane (CH4)
Methanol (CH3OH),
Dimethyl ether
Syngas
CO+H2
Higher alcohols
C2H5OH, etc.
Fischer Tropsch
(CxHy)

6. Cu(211) Methanol pathway CO + 2H2 = CH3OH ΔE (eV) COH* COH*+H*

7. Abild-Pedersen et al. Phys. Rev. Lett. 2007, 99, 016105.
Tools – reducing the parameter space
BEP Relations
Scaling Relations
Abild-Pedersen et al. Phys. Rev. Lett. 2007, 99,
Bligaard et al. J. Catal 2004, 224, 206.

8. CO + 2 H2 -> CH3OH Methanol microkinetics
(1) CO(g) + * -> CO*
(2) H2(g) + 2* -> 2 H*
(3) CO* + H* -> HCO* + *
(4) HCO* + H* -> H2CO* + *
(5) H2CO* + H* -> H3CO* + *
(6) H3CO* + H* -> CH3OH(g) + 2*
All reaction energies --> described in terms of the carbon and oxygen binding energies
All activation barriers --> described in terms of the carbon and oxygen binding energies
--> two parameters describe everything !
--> construction of activity volcano

9. Methanol activity volcano
Rate
513 K
40 bar CO
40 bar H2
log (TOF) s-1

10. Screening

11. Connecting dft with industrial catalyst design
Screening
Rate
573 K
313 K
Connecting dft with industrial catalyst design
Jacobsen et al. J. Catal. 2002, 205, 382.

12. New catalyst leads

13. Higher/lower gallium content results in decreased activity
Preliminary experimental tests
Activity of Ni5Ga3/SiO2 comparable with Cu/ZnO/Al2O3 at 1 bar
Higher/lower gallium content results in decreased activity
Cu/ZnO/Al2O3 catalyst has 100% selectivity
NinGam/SiO2 catalysts exhibit decreased selectivity at higher temperatres