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Organotin compounds immobilized on mesoporous silicas as heterogeneous catalysts for direct synthesis of dimethyl carbonate from methanol and carbon dioxide

Paper ID Volume ID Publish Year Pages File Format Full-Text
42373 45922 2010 9 PDF Available
Title
Organotin compounds immobilized on mesoporous silicas as heterogeneous catalysts for direct synthesis of dimethyl carbonate from methanol and carbon dioxide
Abstract

Organotin compounds of (MeO)2ClSi(CH2)3SnCl3 have been grafted on a series of mesosporous silicas, as proved by XRD, N2 adsorption/desorption experiments and FTIR, diffuse reflectance UV–vis and 13C CP/MAS NMR spectroscopies. A further substitution of Cl− bonded to Sn4+ by CH3O− led to the formation of a series of active heterogeneous catalysts for the direct synthesis of dimethyl carbonate from methanol and CO2. The catalytic properties of these catalysts depended on the structure, crystal size and surface properties of mesoporous silicas. SBA-15 as a host was superior to SBA-16 and large-pore Ia3d. In addition, the methods used for removing surfactants occluded in mesoporous silicas had strong influences on the catalytic performance as a result of significantly affecting the surface areas and the concentrations of surface hydroxyl groups of the mesoporous silicas. The extraction of surfactants by an ethanol–HCl solution should be available. An increase in the reaction time, reaction temperature, methanol amount and CO2 pressure significantly increased the dimethyl carbonate yield before reaching thermodynamic equilibrium. The dimethyl carbonate yield could also be increased by adding dehydration agents to the reaction system. 2,2-Dimethoxypropane gave a much higher dimethyl carbonate yield than 3A molecular sieve and tetramethyl orthorsilicate. The prepared organotin/mesoporous silica catalysts were highly stable, as corroborated by the findings that the dimethyl carbonate yield obtained over the SBA-15-immoilized organotin compound did not decrease within six repeated runs with regeneration under the same reaction conditions and that the tetrahedral coordination state of Sn species was maintained after reaction.

Graphical abstractA highly active and stable heterogeneous organotin catalyst for synthesis of dimethyl carbonate (DMC) from CH3OH and CO2 has been prepared by grafting (MeO)2ClSi(CH2)3SnCl3 on SBA-15 and successively substituting Cl− by CH3O−. The structures of mesoporous silicas, the methods used for removing surfactants, the types of dehydration agents and the reaction conditions had strong influences on the catalytic performance.Figure optionsDownload full-size imageDownload high-quality image (63 K)Download as PowerPoint slide

Keywords
Dimethyl carbonate; Organotin; Mesoporous silica; Graft; SBA-15
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Organotin compounds immobilized on mesoporous silicas as heterogeneous catalysts for direct synthesis of dimethyl carbonate from methanol and carbon dioxide
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Publisher
Database: Elsevier - ScienceDirect
Journal: Applied Catalysis A: General - Volume 372, Issue 1, 5 January 2010, Pages 94–102
Authors
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Subjects
Physical Sciences and Engineering Chemical Engineering Catalysis
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Don't Miss Today's Special Offer
Price was $35.95
You save - $31
Price after discount Only $4.95
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Any Questions? feel free to contact us