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Addressing electronic effects in the semi-hydrogenation of ethyne by InPd2 and intermetallic Ga-Pd compounds

MPS-Authors

Luo,  Yuan
Max Planck Institute for Chemical Physics of Solids, Max Planck Society;

Alarcón Villaseca,  Sebastián
Max Planck Institute for Chemical Physics of Solids, Max Planck Society;

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Friedrich,  Matthias
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;

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Teschner,  Detre
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;

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Knop-Gericke,  Axel
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;

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20160304_InPd2 revised.pdf
(Any fulltext), 760KB

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Citation

Luo, Y., Alarcón Villaseca, S., Friedrich, M., Teschner, D., Knop-Gericke, A., & Armbrüster, M. (2016). Addressing electronic effects in the semi-hydrogenation of ethyne by InPd2 and intermetallic Ga-Pd compounds. Journal of Catalysis, 338, 265-272. doi:10.1016/j.jcat.2016.03.025.


Cite as: http://hdl.handle.net/11858/00-001M-0000-002A-6CA9-E
Abstract
The intermetallic compound InPd2 was prepared as single-phase material and used in an unsupported state as catalyst in the semi-hydrogenation of ethyne in a large excess of ethene. InPd2 showed high activity and selectivity (up to 93%) toward ethene in the temperature range from 478 to 508 K. In addition, the compound revealed high stability during 20 h time on stream at 473 K at 80% selectivity and >90% conversion. Investigations by differential thermal analysis combined with thermogravimetry (DTA/TG) in H2 and near-ambient pressure X-ray photoelectron spectroscopy (NAP-XPS) exclude the formation of intermetallic hydrides, phase transitions, decomposition, and the presence of elemental palladium. The stability of InPd2 under reaction conditions allows addressing the influence of electronic factors on the catalytic properties by comparison with Ga–Pd intermetallic compounds. From the joint results of experiments and first-principles calculations, the electronic influence on the catalytic selectivity is found to be minor; selectivity seems to be largely governed by geometric effects – as suggested earlier by the site-isolation concept – as well as the absence of hydridic hydrogen.