Linking low and high temperature NO oxidation mechanisms over Brønsted acidic chabazite to dynamic changes of the active site

Salavati-fard, Taha; Lobo, Raul F.; Grabow, Lars C.

doi:10.1016/j.jcat.2020.05.029

Linking low and high temperature NO oxidation mechanisms over Brønsted acidic chabazite to dynamic changes of the active site

Journal Article · Sat May 30 00:00:00 EDT 2020 · Journal of Catalysis

DOI:https://doi.org/10.1016/j.jcat.2020.05.029· OSTI ID:1765166

Salavati-fard, Taha ^[1]; Lobo, Raul F. ^[2]; ^[2]

Univ. of Houston, TX (United States); University of Houston
Univ. of Houston, TX (United States)

The oxidation of NO over Brønsted acid sites in chabazite (CHA) zeolites shows an atypical temperature dependence; at low temperature the apparent activation energy is negative, but it becomes positive as the temperature exceeds a transition temperature. To explain this behavior we used density functional theory and statistical mechanics to investigate high and low temperature mechanisms for this reaction and propose a dynamic active site change in response to temperature variation. Our simulations show that the apparent activation barrier in the low temperature regime is more negative over Brønsted acidic CHA as compared to the siliceous zeolite framework. This effect is attributed to further enthalpic stabilization of the transition states by physical interaction with the H-CHA Brønsted acid sites. At elevated temperature, our calculations support both the existence and the significant catalytic role of NO+ in providing a modified active site. The temperature dependent transformation of the active site from H-CHA to NO-CHA sites may occur via two plausible ion-exchange mechanisms that define a transition temperature for the reaction. This transition temperature can be tuned by incorporating different trivalent metal atoms (B, Al, Ga or In) within the CHA framework. We found the lowest transition temperature for H-[In] CHA and H-[Ga]CHA. Here, the ability to control the dynamic response of the active site and the associated switch between low and high temperature mechanism with negative and positive apparent activation energy, respectively, is of fundamental interest for the design of zeolite catalysts operating in the presence of NO.

View Accepted Manuscript (DOE)

Research Organization:: Univ. of Houston, TX (United States)

Sponsoring Organization:: USDOE; USDOE Office of Energy Efficiency and Renewable Energy (EERE), Transportation Office. Vehicle Technologies Office

Grant/Contract Number:: AC02-05CH11231; EE0008233

OSTI ID:: 1765166

Alternate ID(s):: OSTI ID: 1634127

Journal Information:: Journal of Catalysis, Journal Name: Journal of Catalysis Vol. 389; ISSN 0021-9517

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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Linking low and high temperature NO oxidation mechanisms over Brønsted acidic chabazite to dynamic changes of the active site

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