Mono-substituted silicotungstates as active catalysts for sustainable oxidations: homo- and heterogeneous performance

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abstract

A series of tetrabutylammonium (TBA) salts of the transition metal mono-substituted silicotungstates [SiW11M(H2O)O-39](n-), M = Co-II, Fe-III, Mn-III, (SiW11M) were explored as homogeneous catalysts for the oxidation of geraniol and styrene with H2O2. The most active homogeneous catalysts (SiW11Co and SiW11Fe) were immobilized onto an amine-functionalized SBA-15 (aptesSBA-15) and the resulting composites were characterized using several techniques (FT-IR, FT-Raman, UV-Vis/DRS, elemental analysis, powder XRD, SEM and N-2 adsorption-desorption isotherms). The catalytic performance of the new composites SiW11Co@aptesSBA-15 and SiW11Fe@aptesSBA-15 was investigated under similar experimental conditions to those used for homogeneous counterparts. 2,3-Epoxygeraniol and benzaldehyde were the main products obtained from geraniol and styrene oxidation, respectively, for all the catalysts. SiW11Co and SiW11Co@aptesSBA-15 showed to be the most active catalysts for the oxidation of geraniol and styrene. The recyclability of the composite SiW11Co@aptesSBA-15 was investigated for three reaction cycles. The stability of the composites was confirmed using several techniques after catalytic cycles.

keywords

IRON-SUBSTITUTED POLYOXOTUNGSTATES; KEGGIN-TYPE POLYOXOTUNGSTATES; LIQUID-PHASE OXIDATION; HYDROGEN-PEROXIDE; MOLECULAR-OXYGEN; MESOPOROUS SILICA; STRUCTURAL-CHARACTERIZATION; SELECTIVE EPOXIDATION; PORPHYRIN COMPLEXES; AEROBIC EPOXIDATION

subject category

Chemistry

authors

Balula, SS; Cunha-Silva, L; Santos, ICMS; Estrada, AC; Fernandes, AC; Cavaleiro, JAS; Pires, J; Freire, C; Cavaleiro, AMV

our authors

foto Ana Cristina Estrada

Ana Cristina Estrada

Junior Researcher
foto Ana Maria Vieira Silva Viana Cavaleiro

Ana Maria Vieira Silva Viana Cavaleiro

Full professor
no photo

Isabel Cristina Maia da Silva Santos Vieira

Junior Researcher

Groups

G1 - Porous Materials and Nanosystems

acknowledgements

The authors acknowledge the Fundacao para a Ciencia e a Tecnologia (FCT, MEC, Portugal) for general funding (PEst-C/EQB/LA0006/2011 for Associated Laboratory REQUIMTE and PEst-C/QUI/UI0062/2011 for QOPNA) and Pest-OE/QUI/UI0612/2011 (CQB) and grant SFRH/BD/72058/2010(ACF).

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Publication Details

type
Journal Article
year
2013
journal
NEW JOURNAL OF CHEMISTRY
volume
37
publisher
ROYAL SOC CHEMISTRY
issn
1144-0546
issue
8
digital object identifier
10.1039/c3nj00243h
web of science article identifier
WOS:000321788100019

Journal Metrics (JCR 2019)

Journal Impact Factor
3.288
Journal Impact Factor (5 yrs)
3.153
category normalized journal percentile
61.864

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