An ESR study of titanium-silicalite in presence of H2O2

Bonoldi, Lucia; Busetto, C.; Congiu, Annalisa; Marra, Gianluigi; Ranghino, Graziella; Salvalaggio, Mario; Spanò, Guido; Giamello, Elio

doi:10.1016/s1386-1425(01)00703-x

Cited by 24 publications

(26 citation statements)

References 13 publications

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“…Hydrogen peroxide interacting with oxide surfaces is a common source of reactive oxygen species [108], which are frequently implicated in the heterogenous liquid phase catalytic oxidation processes, with a paramount case provided by the titanium silicate catalysts [109,110]. Other representative catalysts used for H2O2 oxidation reactions include metallosilicate T-MCM-41 materials (T = V, Nb, Ti, Cu, Fe, Cr) [111], amorphous oxides of high valent (d 0 ) metals (ZrO2, Nb2O5, Ta2O5) [32,112] and spinels [113].…”

Section: Reactivity Of Ros Derived From H2o2mentioning

confidence: 99%

Characterisation and reactivity of oxygen species at the surface of metal oxides

Anpo

Costentin

Giamello

et al. 2021

Journal of Catalysis

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Section: Reactivity Of Ros Derived From H2o2mentioning

confidence: 99%

Characterisation and reactivity of oxygen species at the surface of metal oxides

Anpo

Costentin

Giamello

et al. 2021

Journal of Catalysis

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“…The most-used technique to investigate the nature of the active species is UV-vis DRS spectroscopy, because it is not affected by the presence of H 2 O. This technique has revealed the formation, upon contact with H 2 O 2 -water solution, of a new band around 26 000 cm À1 (385 nm, which corresponds to a yellow colour), assigned to LMCT from a O-O moiety to the Ti centre 86,87,162,[194][195][196][197][198] (vide infra; the inset in Fig. 8a).…”

Section: Reactivity Of Framework Ti Species Hosted In the Mfi Lattice...mentioning

confidence: 99%

“…8a). Other techniques, such as EPR, 196,197,[199][200][201][202] Raman 86,87,198,203 EXAFS 58,59,82,86,162,198,204 and ab initio calculations 59,81,93,181,182,203,205,206 have been adopted to investigate the complexes formed upon dosing H 2 O 2 (or more complex species, such as terbutyl hydroperoxide) on titanosilicates. Beside experimental approaches, several theoretical works appeared.…”

Section: Reactivity Of Framework Ti Species Hosted In the Mfi Lattice...mentioning

confidence: 99%

Reactivity of Ti(iv) species hosted in TS-1 towards H2O2–H2O solutions investigated by ab initio cluster and periodic approaches combined with experimental XANES and EXAFS data: a review and new highlights

Bordiga

Bonino

Damin

et al. 2007

Phys. Chem. Chem. Phys.

202

241

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This work is intended to underline how the most-advanced experimental and theoretical physical chemistry tools must be used synergistically to understand the reactivity of Ti-silicalite-1 (TS-1) in an important number of low-temperature oxidation reactions with aqueous H(2)O(2) as the oxidant. Literature results are carefully reviewed and accompanied with new, unpublished highlights of both experimental and computational origin. The first part of this work is devoted to a discussion of the defective nature of the material and to the synergic role played by Si vacancies and Ti insertion in the framework. A summary of the experimental Ti-K-edge EXAFS and XANES literature concerning the activated material in vacuo conditions is then presented and compared to the corresponding Ti geometries obtained by ab initio calculations. From such a comparison, the excellent agreement between experiment and theory is evident. A very good agreement is also obtained for the interaction with water and ammonia. For both H(2)O and NH(3), the agreement is due to the possibility to perform experiments in which the probe molecule is dosed from the gas phase, thus allowing to reach the 1 : 1 (or 1 : 2) ratio between the adsorbing Ti sites and the adsorbed molecule. Then, interaction with hydrogen peroxide is discussed, underlining the problems faced in reaching a common view between experimental and theoretical results, owing to the difficulties both in performing experiments where anhydrous H(2)O(2) is dosed on TS-1, and in taking into account the role played by the aqueous medium in the reactivity of Ti(iv) centres toward H(2)O(2) using ab initio calculations. Only once such difficulties have been overcome, by increasing the complexities of both experiments and ab initio models, is a joint-view finally obtained. Where needed, comparison with other experimental results (X-ray and neutron diffraction, NMR, IR, Raman, UV-vis and resonant Raman) is made.

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“…Ab initio quantum mechanical calculations on Zn/TS-1 cluster model, including Ti-OOH [33,34], were carried out to get more insight on the catalysis mechanism. Fig.…”

Section: Epoxidation Of Propylenementioning

confidence: 99%