abstract
Mesoporous silica nanoparticles (MSNs) strategically functionalized were used to immobilize a homogeneous polyoxomolybdate catalyst [PMo12O40](3-) (PMo12), active but unstable. The PMo12@TBA-MSN composite (where TBA refers to surface-tethered tributylammonium groups) conferred high stability to the polyoxomolybdate catalytic center and displayed an increase in efficiency for the oxidative desulfurization (ECODS) of a diesel simulant under sustainable conditions (using H2O2 as oxidant and an ionic liquid, [BMIM]PF6, as solvent). Continuous reuse of the catalyst and ionic liquid solvent in consecutive ECODS cycles was successfully performed, avoiding the production of residual wastes. The performance of the PMo12@TBA-MSN catalyst improved upon its reuse, leading to complete desulfurization of a multicomponent model diesel containing benzothiophene derivatives after just 1 h of the catalytic stage of the process. The robust nature of the supported catalyst was indicated by characterization of the recovered solid which showed retention of the structural and chemical integrities.
keywords
AEROBIC OXIDATIVE DESULFURIZATION; SILICA NANOPARTICLES; IONIC LIQUID; DEEP DESULFURIZATION; EFFICIENT CATALYSTS; MODEL DIESEL; POLYOXOMETALATE; SYSTEM; REAL; DIBENZOTHIOPHENE
subject category
Chemistry; Science & Technology - Other Topics; Materials Science
authors
Mirante, F; Gomes, N; Branco, LC; Cunha-Silva, L; Almeida, PL; Pillinger, M; Gago, S; Granadeiro, CM; Balula, SS
our authors
Carlos Miguel Cardeal Enes Granadeiro
Post-Doc Fellowship
Martyn Pillinger
Principal Researcheracknowledgements
This work was partly funded through the projects REQUIMTE-LAQV, POCI-01-0145-FEDER-007265 [FCT (Fundacao para a Ciencia e a Tecnologia) Ref. UID/QUI/50006/2013] and CICECO -Aveiro Institute of Materials, POCI-01-0145-FEDER-007679 (FCT Ref. UID/CTM/50011/2013), financed by national funds through the FCT/MEC and when appropriate co-financed by FEDER under the PT2020 Partnership Agreement. The FCT and the European Union are acknowledged for post-doctoral grants to C.M.G. (SFRH/BPD/109253/2015) and L.C.S. (SFRH/BPD/111899/2015) co-funded by MCTES and the European Social Fund through the program POPH of QREN. The authors also acknowledge the Portuguese Nuclear Magnetic Resonance Network (PTNMR).