Nora Henriette de Leeuw - Selected Publications#

1. L. Wu, N.Y. Dzade, L. Gao, D.O. Scanlon, Z. Öztürk, N. Hollingsworth, B.M. Weckhuysen, E.J.M. Hensen, N.H. de Leeuw, J.P. Hofmann, Enhanced photoresponse of FeS2 films: The role of marcasite-pyrite phase junctions. Advanced Materials (2016) 28, 9602–9607.

In this paper, De Leeuw's group has provided the calculations which explained the experimentally observed behaviour of enhanced photo properties of mixed sulfide phases. In the literature, marcasite had always been regarded as a detrimental impurity as its band gap was deemed too small for solar cell applications. However, their calculations did not only show that the marcasite band gap is comparable to pyrite, but also explained the enhanced properties of the mixed phase, based on beneficial electron-hole separation between the two sulfide phases.

2. A. Roldan, N. Hollingsworth, A. Roffey, H.U. Islam, J.B.M. Goodall, C.R.A. Catlow, J.A. Darr, W. Bras, G. Sankar, K.B. Holt, G. Hogarth, N.H. de Leeuw, Bioinspired CO2 conversion by iron sulfide catalysts under sustainable conditions. Chem. Commun. (2015) 51, 7501.

This paper was the first study to provide quantitative evidence of the feasibility of a prominent Origin of Life theory, which suggests that the formation of biomolecules which are accepted precursors to ancient and modern life forms, could have been catalyzed by sulfide nano-particles at hydrothermal vents on the ocean floor. The joint experimental-theoretical study further shows that sulfide catalysts can convert CO2 to fuels under moderate and sustainable conditions of pressure and temperature.

3. T.A. Collier, A. Nash, H.L. Birch, N.H. de Leeuw, Preferential sites for intramolecular glucosepane cross-link formation in type I collagen: A thermodynamic study. Matrix Biology (2015) 48, 78-88.

Glucosepane cross-links in collagen strands are a serious age-related condition, which leads to stiffness and reduced of use of tendons. This is the first paper, where fully atomistic simulations have been applied to explicitly calculate cross-link formation within the collagen matrix, thus identifying the preferred sites for cross-link formation, where the glusosepane may block these sites to competing beneficial enzymatic reactions.

4. S. Irrera, A. Roldan, G. Portalone, N.H. de Leeuw, The role of hydrogen bonding and proton transfer in the formation of uracil networks on the gold (100) surface: A density functional theory approach. J. Phys. Chem. C (2013) 117, 3949-3957.

This paper shows how metal templates could be used to form very structure-specific networks of RNA constituent nucleobases, where the authors found that, contrary to what could be expected, the actual network formed is more dependent on lateral interactions between the uracil molecules than vertical interactions to the surface, although initial molecules are strongly bound to the surface, thus anchoring the rest of the growing network.

5. N. Almora-Barrios, N.H. de Leeuw, Molecular dynamics simulation of the early stages of nucleation of hydroxyapatite at a collagen template. Crystal Growth & Design (2012) 12, 756-763.

The mineral phase of bone, hydroxyapatite, is posited to nucleate and grow at collagen templates, possibly via a number of precursor phases. This paper is the first to model the nucleation of hydroxyapatite at a collagen molecule, showing that preferential nucleation does indeed occur at the collagen template rather than in solution. Furthermore, it clearly shows nucleation of calcium phosphate clusters, without the hydroxy groups found in hydroxyapatite, thus confirming that hydroxyapatite does not form initially, but is the result of a phase transition from a hydroxyl-free precursor phase.

6. T.D. Daff, N.H. de Leeuw, Ab initio molecular dynamics simulations of the cooperative adsorption of hydrazine and water on copper surfaces: Implications for shape control of nanoparticles. Chem. Mater. (2011) 23, 2718-2728.





Experimentally, the shape and size of copper nano-particles can be tuned through varying reaction conditions, particularly the concentration of the reducing agent. This paper does not only explain why certain metal surfaces become more prominent as a result of increasing the concentration of hydrazine, but it also takes into account explicitly the competing effect of water in the reaction, which is often ignored in the literature. However, the authors showed that the competitive adsorption of water is a crucial factor in the process, which tips the balance between adsorption of hydrazine at one surface over another.

7. I. Streeter, N.H. de Leeuw, Atomistic modelling of collagen proteins in their fibrillar environment. J. Phys. Chem. B (2010) 114, 13263-13270.

The natural collagen tissue has a complex three-dimensional hierarchical structure, which until this paper had always been modelled as isolated strands in an aqueous environment. In this paper, the authors have developed a first fully 3-dimensional model for collagen, which accurately reproduces the stacking of the strands in the quasi-hexagonal pattern found experimentally, including the regular overlap and gap regions and naturally found water concentration. This realistic collagen model is now used by groups worldwide working on computational collagen research.

8. N.H. de Leeuw, C.R.A. Catlow, H.E. King, A. Putnis, K. Muralidharan, P. Deymier, M. Stimpfl, M.J. Drake, Where on Earth has our water come from? Chem. Commun. (2010) 46, 8923-8925.

Many commonly accepted theories for the origin of water on Earth either cannot explain the quantity of available water or the isotope ratios. The calculations in this paper prove the feasibility of a new theory suggested by De Leeuw's experimental partners, i.e. that the most significant portion of Earth’s water originates from surface-bound water on the dust grains that accreted to form our planet. This theory rested on the surface-water interactions being strong enough to withstand the conditions in interstellar dust clouds, which the quantitative calculations in this paper showed was indeed the case.

9. N.C. Hernandez, R. Grau Crespo, N.H. de Leeuw, J.F. Sanz, Electronic charge transfer between ceria surfaces and gold atoms: a GGA+U investigation. Phys. Chem. Chem. Phys. (2009) 11, 5246-5252.

Ceria is one of the most widely used catalytic materials, both as a catalyst in its own right, but often also used as a support for metal nano-particles. However, in a metal-ceria system, it was unclear whether ceria played a role in the actual process or was just the support material. De Leeuw's calculations, in partnership with colleagues in Spain, showed that depending on the surface structure, there is significant charge transfer between the metal clusters and the ceria support, which is therefore likely to be an active participant in any catalytic processes.

10. R. Grau Crespo, S. Hamad, C.R.A. Catlow, N.H. de Leeuw, Symmetry-adapted configurational modelling of fractional site occupancy in solids. J. Phys. Condens. Matter (2007) 19, 256201.

The location of dopants within a material, or the random distribution or domain formation of solid solutions is difficult to determine experimentally but also difficult to compute. In this paper the authors have presented new software and protocol to model solid solutions and doped materials, which based on thermodynamics determines the preferred distribution of different species in a material as a function of pressure, temperature and other external conditions. This code has now been taken up by computational researchers in disciplines ranging from mineralogy to catalysis and fuel cells.