Search Directions for Direct H2O2 Synthesis Catalysts Starting from Au-12 Nanoclusters

Publication: Research - peer-reviewJournal article – Annual report year: 2012

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Search Directions for Direct H2O2 Synthesis Catalysts Starting from Au-12 Nanoclusters. / Grabow, Lars; Larsen, Britt Hvolbæk; Falsig, Hanne; Nørskov, Jens Kehlet.

In: Topics in Catalysis, Vol. 55, No. 5-6, 2012, p. 336-344.

Publication: Research - peer-reviewJournal article – Annual report year: 2012

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Author

Grabow, Lars; Larsen, Britt Hvolbæk; Falsig, Hanne; Nørskov, Jens Kehlet / Search Directions for Direct H2O2 Synthesis Catalysts Starting from Au-12 Nanoclusters.

In: Topics in Catalysis, Vol. 55, No. 5-6, 2012, p. 336-344.

Publication: Research - peer-reviewJournal article – Annual report year: 2012

Bibtex

@article{6692488596b7402db913c140efa3fa48,
title = "Search Directions for Direct H2O2 Synthesis Catalysts Starting from Au-12 Nanoclusters",
publisher = "Springer New York LLC",
author = "Lars Grabow and Larsen, {Britt Hvolbæk} and Hanne Falsig and Nørskov, {Jens Kehlet}",
year = "2012",
doi = "10.1007/s11244-012-9798-y",
volume = "55",
number = "5-6",
pages = "336--344",
journal = "Topics in Catalysis",
issn = "1022-5528",

}

RIS

TY - JOUR

T1 - Search Directions for Direct H2O2 Synthesis Catalysts Starting from Au-12 Nanoclusters

A1 - Grabow,Lars

A1 - Larsen,Britt Hvolbæk

A1 - Falsig,Hanne

A1 - Nørskov,Jens Kehlet

AU - Grabow,Lars

AU - Larsen,Britt Hvolbæk

AU - Falsig,Hanne

AU - Nørskov,Jens Kehlet

PB - Springer New York LLC

PY - 2012

Y1 - 2012

N2 - We present density functional theory calculations on the direct synthesis of H2O2 from H-2 and O-2 over an Au-12 corner model of a gold nanoparticle. We first show a simple route for the direct formation of H2O2 over a gold nanocatalyst, by studying the energetics of 20 possible elementary reactions involved in the oxidation of H-2 by O-2. The unwanted side reaction to H2O is also considered. Next we evaluate the degree of catalyst control and address the factors controlling the activity and the selectivity. By combining well-known energy scaling relations with microkinetic modeling, we show that the rate of H2O2 and H2O formation can be determined from a single descriptor, namely, the binding energy of oxygen (E-O). Our model predicts the search direction starting from an Au-12 nanocluster for an optimal catalyst in terms of activity and selectivity for direct H2O2 synthesis. Taking also stability considerations into account, we find that binary Au-Pd and Au-Ag alloys are most suited for this reaction.

AB - We present density functional theory calculations on the direct synthesis of H2O2 from H-2 and O-2 over an Au-12 corner model of a gold nanoparticle. We first show a simple route for the direct formation of H2O2 over a gold nanocatalyst, by studying the energetics of 20 possible elementary reactions involved in the oxidation of H-2 by O-2. The unwanted side reaction to H2O is also considered. Next we evaluate the degree of catalyst control and address the factors controlling the activity and the selectivity. By combining well-known energy scaling relations with microkinetic modeling, we show that the rate of H2O2 and H2O formation can be determined from a single descriptor, namely, the binding energy of oxygen (E-O). Our model predicts the search direction starting from an Au-12 nanocluster for an optimal catalyst in terms of activity and selectivity for direct H2O2 synthesis. Taking also stability considerations into account, we find that binary Au-Pd and Au-Ag alloys are most suited for this reaction.

KW - Heterogeneous catalysis

KW - Au

KW - Pd

KW - Ag

KW - H2O2 synthesis

KW - Nanocatalysis

KW - Degree of catalyst control

KW - Selectivity

KW - DFT

U2 - 10.1007/s11244-012-9798-y

DO - 10.1007/s11244-012-9798-y

JO - Topics in Catalysis

JF - Topics in Catalysis

SN - 1022-5528

IS - 5-6

VL - 55

SP - 336

EP - 344

ER -