1.Big particles and Wulff construction
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1 Metal nanoclusters and Catalysis Outline 1.Big particles and Wulff construction 2.Medium-size particles 3.Descriptor for catalysis 4.Ultrananocatalysis
2 Metal nanoclusters and Catalysis: Big particles Wulff theorem Wulff theorem = tool to predict the equilibrium shape of gas-phase metal clusters. It has been developed for macroscopic particles, but can be applied to metal nanoclusters Considering the (111) and (100) surfaces (for simplicity), one has: (100)/ (111) = d(100)/d(111) (100), (111) = surface energies of (100) and (111) facets d(100), d(111) = distances of facets from the centre of the cluster Gas-phase particles This criterion is quite intuitive: the higher the surface energy, the smaller the extension of the face.
3 Metal nanoclusters and Catalysis: Big particles Wulff-Kaishev theorem Wulff-Kaishev theorem : for supported particles for the face in contact with the support, the surface energy has to be rescaled considering the adhesion to the substrate. As the adhesion usually stabilizes the particle, the face on contact with the surface is larger. This is shown in the following image. Supported particles
4 Metal nanoclusters and Catalysis: Big particles Wulff-Kaishev theorem in presence of reactants: O on Ag particles Let s now consider a silver particle adsorbed on amorphous alumina. DFT-estimated surface energies of the (111), (100) and (110) facets : aspect-ratio Roughly estimating an adhesion of 0.2 ev per atom in contact with the oxide, the equilibrium shape of silver particle (about 6 nm in diameter) resulting from the Wulff-Kaishev theorem is the following. about 6 nm in diameter Catalysis Today (2011) side-view top-view
5 Metal nanoclusters and Catalysis: Big particles Wulff-Kaishev theorem in presence of reactants : O on Ag particles when oxygen atoms are adsorbed on the surface, the surface energies have to be rescaled according to the following data: (100) surface 1/2 coverage G=-0.30 ev (111) surface 1/4 coverage G= ev (110) surface 1/2 coverage G= ev We have measured the adsorption energy of oxygen over the Ag surfaces according to the following equation: E ads = 1/No [ E tot E(Ag) No/2 E(O 2 )] We have calculated the G of the reactions by estimating of the G mol (O 2 ) at atmospheric pressure and temperature (298 K) as: G mol (O 2 ) = ev
6 Metal nanoclusters and Catalysis: Big particles Wulff-Kaishev theorem in presence of reactants: O on Ag particles The surface energies of the (111), (100) and (110) faces have to be rescaled according the following data Applying the Wulff-Kaishev theorem using the rescaled values of the surface energies, we get the following structure: about 6 nm in diameter aspect-ratio The aspect-ratio of the silver supported nanoparticles has changed side-view top-view
7 Metal nanoclusters and Catalysis: Big particles Wulff-Kaishev theorem in presence of reactants: O on Ag particles The aspect ratio of the silver particles changes according to the oxygen pressure. Supported particle without oxygen Supported particle at p(o 2 )= 5 x 10-3 atm Supported particle at p(o 2 )= 1 atm This is in line with the experiment: it is observed that the aspect ratio increases in time during partial oxidation of propylene to propylene oxide and acrolein. Our interpretation is that during the reaction the surface is chemically reduced
8 Metal nanoclusters and Catalysis: Big particles Wulff-Kaishev theorem in presence of reactants: C on Ni particles Let s now examine the case of carbon adsorption over a Ni nanoparticle. In absence of carbon adsorbed, the Wulff theorem predicts the following structure for a gas-phase nanoparticle of about 5 nm in diameter. According to DFT, only (111) and (100) facets are exposed in the gas phase
9 Metal nanoclusters and Catalysis: Big particles C atoms on the (113) surface ev ev ev ev ev ev ev ev
10 Metal nanoclusters and Catalysis: Big particles C atoms on the (113) surface ev ev ev ev the adsorption energy passes through a MAXIMUM = experimental observation of an incubation time
11 Metal nanoclusters and Catalysis: Big particles Wulff-Kaishev theorem in presence of reactants: C on Ni particles If carbon is adsorbed on the surface, we can observe the growth of the (113) facets, as carbon strongly interacts with this type of surface NB! Assuming a given carbon chemical potential submitted (2012) (113) facets are exposed due to the lowering of the surface energy This is in agreement with experimental observations
12 Metal nanoclusters and Catalysis: Big particles Wulff-Kaishev theorem in presence of reactants: C on Ni particles No Carbon Transient 1st steady state Field Electron Emission Micrographs of Ni particles
13 Metal nanoclusters and Catalysis Outline 1.Big particles and Wulff construction 2.Medium-size particles 3.Descriptor for catalysis 4.Ultrananocatalysis
14 Metal nanoclusters and Catalysis: Medium-size bare particles Energy ordering of structural motifs upon adsorption Prototypical structural motifs for 38/40 atom pure particles
15 Metal nanoclusters and Catalysis: Medium-size bare particles Energy ordering of structural motifs upon adsorption Two structural motifs with full CO coverage TO 38 Dh 39 Eur. Phys. J. D 52, 131 (2009)
16 Metal nanoclusters and Catalysis: Medium-size bare particles Energy ordering of structural motifs upon adsorption: Pt case bare + 32 CO bare bare + 32 H
17 Metal nanoclusters and Catalysis: Medium-size bare particles Energy ordering of structural motifs upon adsorption: Pd case bare + 32 CO bare bare + 32 H
18 Metal nanoclusters and Catalysis: Medium-size bare particles Energy ordering of structural motifs upon adsorption: Au case bare + 32 CO bare bare + 32 H
19 Metal nanoclusters and Catalysis: Medium-size binary particles Segregation patterns for nanoalloys Prototypical chemical ordering patterns for TO 38. Composition A 6 B 32. Core Hex Cent
20 Metal nanoclusters and Catalysis: Medium-size binary particles Segregation patterns
21 Metal nanoclusters and Catalysis: Medium-size binary particles Adsorption patterns of a single CO molecule (or H atom) on (111) facets
22 Metal nanoclusters and Catalysis: Medium-size binary particles Segregation changes upon CO adsorption Almost segregation inversion: 2 CO will be enough
23 Metal nanoclusters and Catalysis: Medium-size binary particles Segregation changes upon H adsorption No segregation inversion with a few H atoms J. Phys. Chem. C 114, (2010)
24 Metal nanoclusters and Catalysis: Medium-size binary particles Segregation changes upon adsorption: extended surfaces The Pt-CO bond is reinforced by the presence of superficial Cu atoms from: Andersson et al. J. Am. Chem. Soc. 131, 2404 (2009)
25 Metal nanoclusters and Catalysis: Medium-size binary particles Segregation changes upon adsorption: nanoparticles are different
26 Metal nanoclusters and Catalysis: Medium-size binary particles Segregation inversion upon adsorption: nanoparticles from: Tao et al. Science 322, 932 (2008)
27 Metal nanoclusters and Catalysis Outline 1.Big particles and Wulff construction 2.Medium-size particles 3.Descriptor for catalysis 4.Ultrananocatalysis
28 Metal nanoclusters and Catalysis: Descriptors Bronsted-Evans-Polanyi relationships Energy-diagram for CO methanation descriptor from: Norskov et al. Nat Chem 2009 Transition state energy vs CO dissociation energy
29 Metal nanoclusters and Catalysis: Descriptors Bronsted-Evans-Polanyi relationships Rough justification: the whole PES curve as a function of the reaction coordinate moves simultaneously in the same direction from: Hammer et al. Top Cat 2006
30 Metal nanoclusters and Catalysis: Descriptors Sabatier principle (Volcano curve) from: Norskov et al. Nat Chem 2009 Catalytic activity vs descriptor For a given mechanism, you cannot go better than this change the mechanism!
31 Metal nanoclusters and Catalysis: Descriptors Other descriptor: d-band center (Norskov) Norskov et al. Nat Chem 2009 descriptor d F is the difference between the center of the d-band and the Fermi level
32 Metal nanoclusters and Catalysis: Descriptors d-band center in alloys (Norskov) Pt subsurf metal Pt from: Norskov et al. Nat Chem 2009
33 Metal nanoclusters and Catalysis Outline 1.Big particles and Wulff construction 2.Medium-size particles 3.Descriptor for catalysis 4.Ultrananocatalysis
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