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Chloride-free Cu-modified SAPO-37 catalyst for the oxidative carbonylation of methanol in the gas phase

Paper ID Volume ID Publish Year Pages File Format Full-Text
46182 46433 2012 8 PDF Available
Title
Chloride-free Cu-modified SAPO-37 catalyst for the oxidative carbonylation of methanol in the gas phase
Abstract

The substitution of harmful phosgene or chloride-containing catalysts in the synthesis of dimethyl carbonate (DMC) and its use as “green solvent” or polycarbonate building block direct its manufacture towards environmental benign syntheses. Thus, copper was introduced into silicoaluminophosphate structure SAPO-37 (belonging to the same FAU structure family like aluminosilicate zeolites Y and X) by solid state ion exchange (SSIE) using Cu(II) acetyl acetonate. This strategy circumvented structural breakdown being observed when using aqueous copper solutions for impregnation or ion exchange. The SSIE efficiently ran when the organic template is widely extracted from the synthesis form of SAPO-37, e.g. through treatment with methanolic HCl. The parent SAPO-37, template-free SAPO-37 and Cu-SAPO-37 materials were characterized by XRD, TG, temperature programmed reduction (TPR), temperature programmed desorption of ammonia (TPDA) and FTIR spectroscopy of adsorbed pyridine and CO. The Cu-SAPO-37 catalyst pre-treated in inert gas exhibits a high selectivity for DMC and dimethoxymethane (DMM) in the oxidative carbonylation of methanol (OCM). The catalytic behavior of Cu-SAPO-37 is shown to be comparable with those of a Cu-containing Y zeolite catalyst that is so far regarded as one of the best chloride-free catalyst for the OCM reaction in the gas phase.

Graphical abstractFigure optionsDownload full-size imageDownload as PowerPoint slideHighlights► Zeolite Y analogue FAU structure SAPO-37 could be used for MeOH oxycarbonylation in the gas phase. ► No destruction of the crystallinity during template removal and loading with Cu can be detected. ► Cu-modification of SAPO-37 has been carried out by solid state ion exchange using Cu acetyl acetonate. ► The application of Cu-SAPO-37 offers an alternative to the commonly used CuY catalyst.

Keywords
SAPO-37; Cu-modified SAPO-37; Dimethyl carbonate; Oxidative carbonylation of methanol; Solid state ion exchange
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Chloride-free Cu-modified SAPO-37 catalyst for the oxidative carbonylation of methanol in the gas phase
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Publisher
Database: Elsevier - ScienceDirect
Journal: Applied Catalysis B: Environmental - Volumes 121–122, 13 June 2012, Pages 115–122
Authors
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Subjects
Physical Sciences and Engineering Chemical Engineering Catalysis
Get Full-Text Now
Don't Miss Today's Special Offer
Price was $35.95
You save - $31
Price after discount Only $4.95
100% Money Back Guarantee
Full-text PDF Download
Online Support
Any Questions? feel free to contact us