Is It Homogeneous or Heterogeneous Catalysis Derived from [RhCp*Cl2]2? In Operando XAFS, Kinetic, and Crucial Kinetic Poisoning Evidence for Subnanometer Rh4 Cluster-Based Benzene Hydrogenation Catalysis-Reference-Cited by-同舟云学术

Is It Homogeneous or Heterogeneous Catalysis Derived from [RhCp*Cl2]2? In Operando XAFS, Kinetic, and Crucial Kinetic Poisoning Evidence for Subnanometer Rh4 Cluster-Based Benzene Hydrogenation Catalysis

Published:2011-10-28 Issue:46 Volume:133 Page:18889-18902
ISSN:0002-7863
Container-title:Journal of the American Chemical Society
language:en
Short-container-title:J. Am. Chem. Soc.

Author:

Bayram Ercan¹,Linehan John C.²,Fulton John L.²,Roberts John A. S.²,Szymczak Nathaniel K.³,Smurthwaite Tricia D.²,Özkar Saim⁴,Balasubramanian Mahalingam⁵,Finke Richard G.¹

Affiliation:

1. Department of Chemistry, Colorado State University, Fort Collins, Colorado 80523, United States

2. Pacific Northwest National Laboratory, Richland, Washington 99352, United States

3. Department of Chemistry, University of Michigan, 930 North University Avenue, Ann Arbor, Michigan 48109, United States

4. Department of Chemistry, Middle East Technical University, 06531 Ankara Turkey

5. Advanced Photon Source, Argonne National Laboratory, Argonne, Illinois 60439, United States

Publisher

American Chemical Society (ACS)

Subject

Colloid and Surface Chemistry,Biochemistry,General Chemistry,Catalysis

Link

https://pubs.acs.org/doi/pdf/10.1021/ja2073438

Reference56 articles.

1. Schwartz’s more modern definition(1b)of homogeneous vs heterogeneous catalysts is used herein (and in place of the older, historical definitions that equate “homogeneous” with soluble and “heterogeneous” with insoluble); see Figure6elsewhere.(9b)That is, homogeneity or heterogeneity of the catalyst is defined and used herein according to the catalytically active site(s): a homogeneous catalyst has a single, uniform catalyst site, whereas a heterogeneous catalyst has more than one active site. Hence, the catalytically active species uncovered herein, of Rh4clusters with the average stoichiometry of Rh4Cp*2.4Cl4Hc, will be classified (admittedly a bit arbitrarily) as a homogeneous catalyst, since a single active site per each Rh4cluster is expected given the presence of bulky Cp* and Cl–(and possibly H–) ligands and since there is no evidence for more than a single active site within each Rh4cluster. This assignment should be considered tentative, especially since the evidence to follow will indicate the presence of more than one, on average, Rh4cluster in the evolved, “homogeneous” Rh4catalyst.

2. Alkane activation by oxide-bound organorhodium complexes

3. A review of the problem of distinguishing true homogeneous catalysis from soluble or other metal-particle heterogeneous catalysis under reducing conditions

4. Supramolecular Triruthenium Cluster-Based Benzene Hydrogenation Catalysis: Fact or Fiction?

5. When is a Nanoparticle a Cluster? An Operando EXAFS Study of Amine Borane Dehydrocoupling by Rh4-6 Clusters

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