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Kwak, Ja Hun
Molecular Catalysis lab
Research Interests
  • Heterogeneous catalysis, molecular catalysis, ASlumima, zeolites

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Molecular active sites in heterogeneous Ir-La/C-catalyzed carbonylation of methanol to acetates

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Title
Molecular active sites in heterogeneous Ir-La/C-catalyzed carbonylation of methanol to acetates
Author
Kwak, JahunDagle, RobertTustin, Gerald C.Zoeller, Joseph R.Allard, Lawrence F.Wang, Yong
Keywords
acetic acid; carbonylation; catalysis; heterogeneous iridium catalyst; methanol; molecular active sites
Issue Date
201402
Publisher
AMER CHEMICAL SOC
Citation
JOURNAL OF PHYSICAL CHEMISTRY LETTERS, v.5, no.3, pp.566 - 572
Abstract
We report that when Ir and La halides are deposited on carbon, exposure to CO spontaneously generates a discrete molecular heterobimetallic structure, containing an Ir-La covalent bond that acts as a highly active, selective, and stable heterogeneous catalyst for the carbonylation of methanol to produce acetic acid. This catalyst exhibits a very high productivity of ∼1.5 mol acetyl/mol Ir·s with >99% selectivity to acetyl (acetic acid and methyl acetate) without detectable loss in activity or selectivity for more than 1 month of continuous operation. The enhanced activity can be mechanistically rationalized by the presence of La within the ligand sphere of the discrete molecular Ir-La heterobimetallic structure, which acts as a Lewis acid to accelerate the normally rate-limiting CO insertion in Ir-catalyzed carbonylation. Similar approaches may provide opportunities for attaining molecular (single site) behavior similar to homogeneous catalysis on heterogeneous surfaces for other industrial applications.
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DOI
http://dx.doi.org/10.1021/jz402728e
ISSN
1948-7185
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