Support effects in the gas phase hydrogenation of butyronitrile over palladium

Yufen Hao, Xiaodong Wang, Noémie Perret, Fernando Cárdenas-Lizana, Mark Keane

Research output: Contribution to journalArticle

9 Citations (Scopus)

Abstract

The role of the support in the gas phase hydrogenation of butyronitrile over Pd/Al2O3 and Pd/C (2.5–3.0 nm mean Pd size) has been studied, taking bulk Pd as benchmark. Catalyst activation by temperature programmed reduction was monitored and the metal and acid functions characterized by H2 and NH3 chemisorption/temperature programmed desorption and electron microscopy (STEM/TEM). Butyronitrile hydrogenation was stable with time on-stream to deliver butylamine where consecutive condensation with the intermediate butylidenimine generated dibutylamine and tributylamine. Condensation can occur on bulk Pd but selectivity is influenced by the support and reaction over Pd/Al2O3 generated dibutylamine as principal product. Preferential tertiary amine formation was observed over Pd/C and attributed to greater surface acidity that favors the condensation step. Increased hydrogen spillover and acidity (associated with Pd/C) elevated butyronitrile consumption rate.
Original languageEnglish
Pages (from-to)4-10
Number of pages7
JournalCatalysis, Structure & Reactivity
Volume1
Issue number1
DOIs
Publication statusPublished - Feb 2015

Fingerprint

Palladium
Hydrogenation
Condensation
Gases
Acidity
Butylamines
Temperature programmed desorption
Chemisorption
Electron microscopy
Amines
Hydrogen
Metals
Chemical activation
Transmission electron microscopy
Catalysts
Acids
Temperature
dibutylamine

Keywords

  • Pd/Al2O3
  • Pd/C
  • Bulk PD
  • butyronitrile hydrogenation
  • surface acidity
  • spillover hydrogen

Cite this

Support effects in the gas phase hydrogenation of butyronitrile over palladium. / Hao, Yufen; Wang, Xiaodong; Perret, Noémie; Cárdenas-Lizana, Fernando; Keane, Mark.

In: Catalysis, Structure & Reactivity, Vol. 1, No. 1, 02.2015, p. 4-10.

Research output: Contribution to journalArticle

Hao, Yufen ; Wang, Xiaodong ; Perret, Noémie ; Cárdenas-Lizana, Fernando ; Keane, Mark. / Support effects in the gas phase hydrogenation of butyronitrile over palladium. In: Catalysis, Structure & Reactivity. 2015 ; Vol. 1, No. 1. pp. 4-10.
@article{4de3e9d384104fff944b03b1740ca875,
title = "Support effects in the gas phase hydrogenation of butyronitrile over palladium",
abstract = "The role of the support in the gas phase hydrogenation of butyronitrile over Pd/Al2O3 and Pd/C (2.5–3.0 nm mean Pd size) has been studied, taking bulk Pd as benchmark. Catalyst activation by temperature programmed reduction was monitored and the metal and acid functions characterized by H2 and NH3 chemisorption/temperature programmed desorption and electron microscopy (STEM/TEM). Butyronitrile hydrogenation was stable with time on-stream to deliver butylamine where consecutive condensation with the intermediate butylidenimine generated dibutylamine and tributylamine. Condensation can occur on bulk Pd but selectivity is influenced by the support and reaction over Pd/Al2O3 generated dibutylamine as principal product. Preferential tertiary amine formation was observed over Pd/C and attributed to greater surface acidity that favors the condensation step. Increased hydrogen spillover and acidity (associated with Pd/C) elevated butyronitrile consumption rate.",
keywords = "Pd/Al2O3, Pd/C, Bulk PD, butyronitrile hydrogenation, surface acidity, spillover hydrogen",
author = "Yufen Hao and Xiaodong Wang and No{\'e}mie Perret and Fernando C{\'a}rdenas-Lizana and Mark Keane",
note = "Acknowledgements The authors acknowledge EPSRC support for free access to the TEM/SEM facility at the University of St Andrews and financial support to Y. Hao and X. Wang through the Overseas Research Students Award Scheme (ORSAS).",
year = "2015",
month = "2",
doi = "10.1179/2055075814Y.0000000002",
language = "English",
volume = "1",
pages = "4--10",
journal = "Catalysis, Structure & Reactivity",
issn = "2055-074X",
number = "1",

}

TY - JOUR

T1 - Support effects in the gas phase hydrogenation of butyronitrile over palladium

AU - Hao, Yufen

AU - Wang, Xiaodong

AU - Perret, Noémie

AU - Cárdenas-Lizana, Fernando

AU - Keane, Mark

N1 - Acknowledgements The authors acknowledge EPSRC support for free access to the TEM/SEM facility at the University of St Andrews and financial support to Y. Hao and X. Wang through the Overseas Research Students Award Scheme (ORSAS).

PY - 2015/2

Y1 - 2015/2

N2 - The role of the support in the gas phase hydrogenation of butyronitrile over Pd/Al2O3 and Pd/C (2.5–3.0 nm mean Pd size) has been studied, taking bulk Pd as benchmark. Catalyst activation by temperature programmed reduction was monitored and the metal and acid functions characterized by H2 and NH3 chemisorption/temperature programmed desorption and electron microscopy (STEM/TEM). Butyronitrile hydrogenation was stable with time on-stream to deliver butylamine where consecutive condensation with the intermediate butylidenimine generated dibutylamine and tributylamine. Condensation can occur on bulk Pd but selectivity is influenced by the support and reaction over Pd/Al2O3 generated dibutylamine as principal product. Preferential tertiary amine formation was observed over Pd/C and attributed to greater surface acidity that favors the condensation step. Increased hydrogen spillover and acidity (associated with Pd/C) elevated butyronitrile consumption rate.

AB - The role of the support in the gas phase hydrogenation of butyronitrile over Pd/Al2O3 and Pd/C (2.5–3.0 nm mean Pd size) has been studied, taking bulk Pd as benchmark. Catalyst activation by temperature programmed reduction was monitored and the metal and acid functions characterized by H2 and NH3 chemisorption/temperature programmed desorption and electron microscopy (STEM/TEM). Butyronitrile hydrogenation was stable with time on-stream to deliver butylamine where consecutive condensation with the intermediate butylidenimine generated dibutylamine and tributylamine. Condensation can occur on bulk Pd but selectivity is influenced by the support and reaction over Pd/Al2O3 generated dibutylamine as principal product. Preferential tertiary amine formation was observed over Pd/C and attributed to greater surface acidity that favors the condensation step. Increased hydrogen spillover and acidity (associated with Pd/C) elevated butyronitrile consumption rate.

KW - Pd/Al2O3

KW - Pd/C

KW - Bulk PD

KW - butyronitrile hydrogenation

KW - surface acidity

KW - spillover hydrogen

U2 - 10.1179/2055075814Y.0000000002

DO - 10.1179/2055075814Y.0000000002

M3 - Article

VL - 1

SP - 4

EP - 10

JO - Catalysis, Structure & Reactivity

JF - Catalysis, Structure & Reactivity

SN - 2055-074X

IS - 1

ER -