Measurements of Acidity of H-SSZ-35 by a Combined Method of IRMS-TPD Experiment and DFT Calculation

Suzuki, Katsuki; Katada, Naonobu; Niwa, Miki

doi:10.1007/s10562-010-0440-y

Catal Lett

2010

DOI: 10.1007/s10562-010-0440-y

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Measurements of Acidity of H-SSZ-35 by a Combined Method of IRMS-TPD Experiment and DFT Calculation

Katsuki Suzuki

Naonobu Katada

Miki Niwa

Abstract: Infrared/mass spectroscopy-temperature programmed desorption of ammonia experiment on an SSZ-35 zeolite was measured to characterize the acidity. Two kinds of the Brønsted acid site were detected at 3,622 and 3,505 cm -1 ; these concentrations were nearly the same, and the strengths DH were 129 and 117 kJ mol -1 , respectively. These Brønsted hydroxyls were identified to be located in the 10-ring and 5-ring in the STF cage, respectively. These measured strengths were supported well by the DFT calculation.

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Cited by 3 publications

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Analysis and interpretation of acidic nature of aluminosilicates

Katada

2018

Molecular Catalysis

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Aluminosilicate solid acid catalysts, especially zeolites, have been widely utilized in petroleum refinery and environmentally benign chemical processes. The acidic property of aluminosilicates has been a subject of advanced studies. Recently an ammonia IRMS-TPD (infrared / mass spectroscopy temperature-programmed desorption) method, an application of operando technique, has been developed to quantify the number and strength distribution of each of Brønsted and Lewis sites on a solid. With an aid of quantum chemistry, relationships among the composition, structure and acidic property are being unveiled to totally understand the chemistry of SiOHAl unit in the aluminosilicates.

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Analysis and interpretation of acidic nature of aluminosilicates

Katada

2018

Molecular Catalysis

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Correlation between Na–Cs Ion Exchange Properties in the Alkaline Form and Acid Strength in the Proton Form of Zeolite

Katada,

Tamura,

Matsuda

et al. 2024

Langmuir

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The ion exchange function of zeolite is useful for such a purpose as the removal of radioactive Cs species from water. In the very early days of zeolite science, the affinity of zeolites for metal cations was explained based on geometry. After the explanation presented above was proposed, many new zeolites and related materials were discovered or synthesized. Furthermore, it has become clear that the chemical nature of the ion exchange sites is strongly dependent on the framework topology. In this study, the ion exchange behavior between Na-form zeolites with different framework topologies and Cs-containing aqueous solutions was analyzed, and the equilibrium constant was calculated based on the Langmuir type equation to investigate the influence of the chemical nature of the zeolite framework on ion selectivity. The equilibrium constants at room temperature were in the order FAU < LTA < MFI < YFI < MOR. This order is the same as the order of Bro̷ nsted acid strengths in the corresponding proton form zeolites. It is suggested that the delocalization of charge around the ion exchange site stabilizes a large cation whose charge is delocalized. In contrast, the equilibrium constant was not related to the pore and cavity size. This opens new insight into the influence of the chemical nature of zeolite on the affinity to cation.

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Determination of the positions of aluminum atoms introduced into SSZ-35 and the catalytic properties of the generated Brønsted acid sites

Miyaji

Kimura

Shiga

et al. 2017

Phys. Chem. Chem. Phys.

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The positions of aluminum (Al) atoms in SSZ-35 together with the characteristics of the generated protons were investigated by Al multiple quantum magic-angle spinning (MQ-MAS),Si MAS, and H MAS NMR data analyses accompanied by a variable temperatureH MAS NMR analysis. The origin of the acidic -OH groups (Brønsted acid sites) generated by introducing Al atoms into the T sites was investigated and the T sites introduced into the Al atoms were revealed. To further determine the catalytic properties of the acidic protons generated in SSZ-35, the influence of the concentration of the Al atoms on the catalytic activity and selectivity during the transformation of toluene was examined.

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Measurements of Acidity of H-SSZ-35 by a Combined Method of IRMS-TPD Experiment and DFT Calculation

Cited by 3 publications

References 18 publications

Analysis and interpretation of acidic nature of aluminosilicates

Analysis and interpretation of acidic nature of aluminosilicates

Correlation between Na–Cs Ion Exchange Properties in the Alkaline Form and Acid Strength in the Proton Form of Zeolite

Determination of the positions of aluminum atoms introduced into SSZ-35 and the catalytic properties of the generated Brønsted acid sites

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