fulltext.study @t Gmail

Effects of multivariate linker substitution, metal binding, and reactor conditions on the catalytic activity of a Pd-functionalized MOF for olefin hydrogenation

Paper ID Volume ID Publish Year Pages File Format Full-Text
39513 45825 2014 8 PDF Available
Title
Effects of multivariate linker substitution, metal binding, and reactor conditions on the catalytic activity of a Pd-functionalized MOF for olefin hydrogenation
Abstract

•Pd(CH3CN)2Cl2 was covalently bonded to IRMOF-3 to form a new palladium catalyst.•Optimal metal loading and specific surface were found for propylene hydrogenation.•Kinetics and diffusion measurements showed intra-particle diffusion limitations.•The operating temperature range for avoiding thermal degradation was identified.•Catalyst showed excellent reversibility to carbon monoxide poisoning.

We investigated the performance of zinc-based metal-organic framework (MOF) catalysts that were post-synthetically modified with the homogeneous palladium catalyst Pd(CH3CN)2Cl2 for the hydrogenation of propylene in a packed-bed, tubular microreactor. The catalytic conversion and apparent reaction kinetics were analyzed across a range of metal loadings, reactant flow rates, feed concentrations, and reactor temperatures. The catalyst's deactivation in the presence of a common palladium catalyst poison, carbon monoxide, was also examined. The catalytic conversion was optimal at moderate metal loadings, stoichiometric excess of hydrogen, and relatively mild temperatures. The activity depended strongly on reactant feed composition but showed no dependence on total flow rate, indicating a diffusion-limited process. To investigate the effects of intra-particle diffusion limitations, internal diffusion coefficients for propylene in the MOF catalysts were measured with pulsed field gradient nuclear magnetic resonance (PFG NMR) and were incorporated into the kinetics analysis. Using these coefficients to compute effectiveness factors for heterogeneous catalytic reactions, diffusion-limited artifacts were accounted for to obtain intrinsic rate constants and activation energies from apparent kinetics data. The average intrinsic activation energy was found to be 51(6) kJ/mol. The MOF catalyst was also found to be reversible under carbon monoxide poisoning, suggesting a weak binding mechanism.

Graphical abstractFigure optionsDownload full-size imageDownload high-quality image (265 K)Download as PowerPoint slide

Keywords
Metal organic framework; Multivariate principle; Heterogeneous catalysis; Palladium; Propylene
First Page Preview
Effects of multivariate linker substitution, metal binding, and reactor conditions on the catalytic activity of a Pd-functionalized MOF for olefin hydrogenation
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
Publisher
Database: Elsevier - ScienceDirect
Journal: Applied Catalysis A: General - Volume 488, November 2014, Pages 248–255
Authors
, , , , , , ,
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