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  Structure–Activity Studies on Highly Active Palladium Hydrogenation Catalysts by X-ray Absorption Spectroscopy

Bauer, M., Schoch, R., Shao, L., Zhang, B. S., Knop-Gericke, A., Willinger, M. G., et al. (2012). Structure–Activity Studies on Highly Active Palladium Hydrogenation Catalysts by X-ray Absorption Spectroscopy. Journal of Physical Chemistry C, 116(42), 22375-22385. doi:10.1021/jp306962v.

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 Creators:
Bauer, Matthias1, Author
Schoch, Roland1, Author
Shao, Lidong2, Author           
Zhang, Bing Sen2, Author           
Knop-Gericke, Axel2, Author           
Willinger, Marc Georg2, Author           
Schlögl, Robert2, Author           
Teschner, Detre2, Author           
Affiliations:
1TU Kaiserslautern, Fachbereich Chemie, Erwin-Schrödinger-Strassee 54, D-67663 Kaiserslautern, Germany, ou_persistent22              
2Inorganic Chemistry, Fritz Haber Institute, Max Planck Society, ou_24023              

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Free keywords: Palladium; Hydrogen; Propyne; in situ XANES; EXAFS
 Abstract: Functionalized carbon nanotubes were used to produce Pd-based hydrogenation catalysts. Pd/CNT with small (1–2 nm) Pd particles showed classical catalytic behavior in propyne hydrogenation, with high propene selectivity at moderate conversion levels and propane formation near full conversion. Pd/CNT with larger (15 nm) nanoparticles, however, was selective (88%) toward propene even at practically full propyne conversion. An additionally prepared Pd2Ga/CNT catalyst exhibited even higher propene selectivity at full conversion. All of these materials were studied in situ by X-ray absorption spectroscopy at the Pd K-edge. Pd2Ga/CNT was stable under all conditions examined without variation in XANES or in the derived EXAFS parameters. Both Pd/CNT samples formed β-hydride under hydrogen, as assessed from the calculated lattice expansion and the characteristic red shift of the XANES maxima. The minor spectroscopic difference between the monometallic catalysts observed at high propyne conversion suggests the decisive role of a Pd–C (subsurface C) contribution in the structure of larger Pd particles, being absent with ultrasmall nanoparticles. In general, all factors (intermetallic phase formation, subsurface C, etc.) that reduce the surface H coverage will give rise to enhanced partial hydrogenation selectivity of palladium when secondary alkene hydrogenation at late bed segments or diffusion issues in the pores are avoided.

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Language(s): eng - English
 Dates: 2012-09-272012
 Publication Status: Issued
 Pages: -
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 Table of Contents: -
 Rev. Type: Peer
 Identifiers: DOI: 10.1021/jp306962v
 Degree: -

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Title: Journal of Physical Chemistry C
Source Genre: Journal
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Publ. Info: Washington DC : American Chemical Society
Pages: - Volume / Issue: 116 (42) Sequence Number: - Start / End Page: 22375 - 22385 Identifier: ISSN: 1932-7447
CoNE: https://pure.mpg.de/cone/journals/resource/954926947766_2