Is it single-metal homogeneous or polymetallic heterogeneous catalysis? Further investigation of the catalytically active species in benzene hydrogenation beginning with [RhCp*Cl 2] 2 via operando-XAFS, kinetic and poisoning studies

Date

2011-12-01

Author

Bayram, Ercan
Linehan, John C.
Finke, Richard G.
Fulton, John
Roberts, John A. S.
Smurthwaite, Tricia D.
Özkar, Saim
Szymczak, Nathaniel K.

Metadata

Show full item record

This work is licensed under a Creative Commons Attribution-NonCommercial-NoDerivatives 4.0 International License.

Item Usage Stats

36
views

0
downloads

Previous investigation (Hagen et al. J. Am. Chem. Soc. 2005, 127, 4423) for benzene hydrogenation starting with [RhCp*Cl 2] 2 at 100 °C and 50 atm initial H 2 pressure concluded that the true catalyst was most likely Rh(0) nanoparticles on the basis of sigmoidal kinetics, Rh(0) precipitate, and positive Hg(0) poisoning studies. There was, at the time, no other plausible hypothesis for the true catalyst in light of the extant data. Further investigation via operando-XAFS provides a new hypothesis for the active catalyst: ligated Rh 4 sub-nanometer clusters that constitute ∼98% of the total soluble Rh in solution. Kinetics and quantitative poisoning studies support this hypothesis. The results are of significant interest since determining the nature of the true catalyst continues to be a central, often vexing issue, in any and all catalytic reactions.

URI

https://www.scopus.com/inward/record.uri?partnerID=HzOxMe3b&scp=84861015817&origin=inward
https://hdl.handle.net/11511/102664

Conference Name

242nd ACS National Meeting and Exposition

Collections

Graduate School of Natural and Applied Sciences, Conference / Seminar

Suggestions

OpenMETU
Core

Comment on 'Rockfall avalance deposits associated with normal faulting in the NW of the Cankiri basin: implications for the post-collisional tectonic evolution of the Neo-Tethyan suture zone' by G. Seyitoglu, N. Kazanci, L. Karadenizli, S. Sen, B. Varol, and T. Karabiyikoglu Kaymakcı, Nuretdin (Wiley, 2003-04-01) Seyitoglu et al. (2000) described their interpretation, based on a single fault surface and rockfall avalanche deposits previously mapped as a W-vergent thrust klippen above the Neogene successions in the Hancili Basin, that in central Anatolia there was a single extensional basin throughout the Miocene - Early Pliocene. It was later fragmented by a structural high of Neo-Tethyan ophiolitic basement bounded by an E-vergent thrust fault in the east along the western margin of the Cankiri Basin and a west-dip...
Numerical simulation of scour and backfilling processes around a circular pile in waves Baykal, Cüneyt; Fuhrman, D. R.; Jacobsen, N. G.; Fredsoe, J. (2017-04-01) This study continues the investigation of flow and scour around a vertical pile, reported by Roulund et al. (2005). Flow and scour/backfilling around a vertical pile exposed to waves are investigated by using a three-dimensional numerical model based on incompressible Reynolds averaged Navier-Stokes equations. The model incorporates (1) k-omega turbulence closure, (2) vortex shedding processes, (3) sediment transport (both bed and suspended load), as well as (4) bed morphology. The numerical simulations are...
Linear Contrasts for Time Series Data with Non-Normal Innovations: An Application to a Real Life Data Yıldırım, Özgecan; Yozgatlıgil, Ceylan; Şenoğlu, Birdal (2017-12-08) Yıldırım et al. [5] estimated the model parameters and introduced a test statistic in one-way classification AR(1) model under the assumption of independently and identically distributed (iid) error terms having Student’s t distribution, see also [4]. In this study, we extend their study to linear contrasts which is a well-known and widely used comparison method when the null hypothesis about the equality of the treatment means is rejected, see [3], [4]. See also [1] and [2] in the context of ANOVA. A test ...
Anthropic likelihood for the cosmological constant and the primordial density perturbation amplitude Hong, Sungwook E.; Stewart, Ewan D.; Zoe, Heeseung (2012-04-09) Weinberg et al. calculated the anthropic likelihood of the cosmological constant Lambda using a model assuming that the number of observers is proportional to the total mass of gravitationally collapsed objects, with mass greater than a certain threshold, at t -> infinity. We argue that Weinberg's model is biased toward small Lambda, and to try to avoid this bias we modify his model in a way that the number of observers is proportional to the number of collapsed objects, with mass and time equal to certain ...
Searching for subspace trails and truncated differentials Leander, Gregor; Tezcan, Cihangir; Wiemer, Friedrich (2018-01-01) Grassi et al. [Gra+16] introduced subspace trail cryptanalysis as a generalization of invariant subspaces and used it to give the first five round distinguisher for Aes. While it is a generic method, up to now it was only applied to the Aes and Prince. One problem for a broad adoption of the attack is a missing generic analysis algorithm. In this work we provide efficient and generic algorithms that allow to compute the provably best subspace trails for any substitution permutation cipher.

Citation Formats

E. Bayram et al., “Is it single-metal homogeneous or polymetallic heterogeneous catalysis? Further investigation of the catalytically active species in benzene hydrogenation beginning with [RhCp*Cl 2] 2 via operando-XAFS, kinetic and poisoning studies,” presented at the 242nd ACS National Meeting and Exposition, Denver, CO, Amerika Birleşik Devletleri, 2011, Accessed: 00, 2023. [Online]. Available: https://www.scopus.com/inward/record.uri?partnerID=HzOxMe3b&scp=84861015817&origin=inward.