Ethanol Conversion to Ethylene and Acetaldehyde over Rhodium(I) Exchanged Faujasite Zeolite. A QM/MM and Microkinetic Study

We have studied the structure of mononuclear gold supported on acidic form of faujasite zeolite in two oxidation states, namely, 0 and +1, using density functional theory. The binding of the gold monomer to the zeolite support is stronger in the oxidation state +1 than in the oxidation state 0. For the oxidation state 0, the hydrogenated clusters AuH/(2H)-FAU, AuH2/H-FAU generated by stepwise reverse hydrogen spillover from bridging OH groups of zeolite are energetically preferred over the Au/(3H)-FAU structure. Reverse hydrogen spillover of all the three acidic protons from the zeolite to the Au monomer did not lead to a stable structure. The calculated reverse hydrogen spillover energy per hydrogen atom for zeolite supported AuH and AuH2 clusters are −10.2 and −5.1 kJ/mol, respectively, in the oxidation state 0, while in the oxidation state +1 it is 20.9 kJ/mol for zeolite supported Au+H cluster.

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Nature and Catalytic Role of Extraframework Aluminum in Faujasite Zeolite: A Theoretical Perspective

ACS Catalysis ◽

10.1021/acscatal.5b02268 ◽

2015 ◽

Vol 5 (11) ◽

pp. 7024-7033 ◽

Cited By ~ 35

Author(s):

Chong Liu ◽

Guanna Li ◽

Emiel J. M. Hensen ◽

Evgeny A. Pidko

Keyword(s):

Theoretical Perspective ◽

Zeolite A ◽

Catalytic Role ◽

Faujasite Zeolite

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Relationship between acidity and catalytic reactivity of faujasite zeolite: A periodic DFT study

Journal of Catalysis ◽

10.1016/j.jcat.2016.10.027 ◽

2016 ◽

Vol 344 ◽

pp. 570-577 ◽

Cited By ~ 28

Author(s):

Chong Liu ◽

Guanna Li ◽

Emiel J.M. Hensen ◽

Evgeny A. Pidko

Keyword(s):

Dft Study ◽

Zeolite A ◽

Catalytic Reactivity ◽

Periodic Dft ◽

Faujasite Zeolite

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Evidence of a framework induced cation redistribution upon water adsorption in cobalt exchanged X faujasite zeolite: A joint experimental and simulation study

Microporous and Mesoporous Materials ◽

10.1016/j.micromeso.2010.09.031 ◽

2011 ◽

Vol 138 (1-3) ◽

pp. 45-50 ◽

Cited By ~ 44

Author(s):

Marie Jeffroy ◽

Elena Borissenko ◽

Anne Boutin ◽

Angela Di Lella ◽

Florence Porcher ◽

...

Keyword(s):

Simulation Study ◽

Water Adsorption ◽

Zeolite A ◽

Cation Redistribution ◽

Faujasite Zeolite

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Adsorption of NO, NO2, CO, H2O and CO2 over isolated monovalent cations in faujasite zeolite: a periodic DFT investigation

Theoretical Chemistry Accounts ◽

10.1007/s00214-018-2373-2 ◽

2018 ◽

Vol 137 (12) ◽

Cited By ~ 19

Author(s):

E. P. Hessou ◽

W. G. Kanhounnon ◽

D. Rocca ◽

H. Monnier ◽

C. Vallières ◽

...

Keyword(s):

Monovalent Cations ◽

Zeolite A ◽

Periodic Dft ◽

Faujasite Zeolite

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New material as Ni-support for hydrogen production by ethanol conversion

Advanced Materials and Information Technology Processing ◽

10.2495/amitp130141 ◽

2014 ◽

Cited By ~ 1

Author(s):

S. Candamano ◽

P. Frontera ◽

A. Macario ◽

A. Aloise ◽

F. Crea

Keyword(s):

Hydrogen Production ◽

Ethanol Conversion ◽

New Material

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The Nature of Chemisorbed CO2 in Zeolite A

10.26434/chemrxiv.7422815 ◽

2019 ◽

Author(s):

Przemyslaw Rzepka ◽

Zoltán Bacsik ◽

Andrew J. Pell ◽

Niklas Hedin ◽

Aleksander Jaworski

Keyword(s):

Solid State ◽

Ir Spectroscopy ◽

Quantum Chemical Calculations ◽

Quantum Chemical ◽

Surface Coverage ◽

Gas Mixtures ◽

Mas Nmr ◽

Significant Fraction ◽

Zeolite A

Formation of CO32- and HCO3- species without participation of the framework oxygen atoms upon chemisorption of CO2 in zeolite |Na12|-A is revealed. The transfer of O and H atoms is very likely to have proceeded via the involvement of residual H2O or acid groups. A combined study by solid-state 13C MAS NMR, quantum chemical calculations, and in situ IR spectroscopy showed that the chemisorption mainly occurred by the formation of HCO3-. However, at a low surface coverage of physisorbed and acidic CO2, a significant fraction of the HCO3- was deprotonated and transformed into CO32-. We expect that similar chemisorption of CO2 would occur for low-silica zeolites and other basic silicates of interest for the capture of CO2 from gas mixtures.

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