Hydrogen adsorption on two catalysts for the ortho- to parahydrogen conversion: Cr-doped silica and ferric oxide gel

Monika Hartl; Robert Chad Gillis; Luke Daemen; Daniel P. Olds; Katherine Page; Stefan Carlson; Yongqiang Cheng; Thomas Hügle; Erik B. Iverson; A. J. Ramirez-Cuesta; Yongjoong Lee; Günter Muhrer

doi:10.1039/c6cp01154c

Hydrogen adsorption on two catalysts for the ortho- to parahydrogen conversion: Cr-doped silica and ferric oxide gel

Monika Hartl, Robert Chad Gillis, Luke Daemen, Daniel P. Olds, Katherine Page, Stefan Carlson, Yongqiang Cheng, Thomas Hügle, Erik B. Iverson, A. J. Ramirez-Cuesta, Yongjoong Lee, Günter Muhrer

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Abstract

Molecular hydrogen exists in two spin-rotation coupled states: parahydrogen and orthohydrogen. Due to the variation of energy with rotational level, the occupation of ortho- and parahydrogen states is temperature dependent, with parahydrogen being the dominant species at low temperatures. The equilibrium at 20 K (99.8% parahydrogen) can be reached by natural conversion only after a lengthy process. With the use of a suitable catalyst, this process can be shortened significantly. Two types of commercial catalysts currently being used for ortho- to parahydrogen conversion are: iron(iii) oxide (Fe₂O₃, IONEX®), and chromium(ii) oxide doped silica catalyst (CrO·SiO₂, OXISORB®). We investigate the interaction of ortho- and parahydrogen with the surfaces of these ortho-para conversion catalysts using neutron vibrational spectroscopy. The catalytic surfaces have been characterized using X-ray absorption fine structure (XAFS) and X-ray/neutron pair distribution function measurements.

Original language	English
Pages (from-to)	17281-17293
Number of pages	13
Journal	Physical Chemistry Chemical Physics
Volume	18
Issue number	26
DOIs	https://doi.org/10.1039/c6cp01154c
State	Published - 2016
Externally published	Yes

Funding

M. H. is grateful to P. Karlsson at Bodo Moeller Chemie Sweden for supplying a sample of their IONEX? Type O-P catalyst. BET measurements were performed by B. Linden at the Department of Chemical Engineering, Lund University. This research benefited from the use of the VISION and NOMAD beamlines at ORNL's Spallation Neutron Source, which is supported by the Scientific User Facilities Division, Office of Basic Energy Sciences, U.S. Department of Energy under Contract No. DE-AC0500OR22725 with UT Battelle, LLC. Work performed at Argonne and use of the Advanced Photon Source were supported by the U. S. Department of Energy, Office of Science, Office of Basic Energy Sciences, under Contract No. DE-AC02-06CH11357. We gratefully acknowledge Hsiu-Wen Wang and Ying Shi for the use of reference silica PDF data. This work was also supported by the use of the Advanced Photon Source at the Argonne National Laboratory supported by the U.S. DOE under Contract No. DE-AC02-06CH11357. Portions of this research were carried out at beamline I811, MAX-lab synchrotron radiation source, Lund University, Sweden. Funding for the beamline I811 project was kindly provided by The Swedish Research Council and The Knut och Alice Wallenbergs Stiftelse.

Funders	Funder number
Scientific User Facilities Division
U.S. Department of Energy	DE-AC0500OR22725
Office of Science	DE-AC02-06CH11357
Basic Energy Sciences
Argonne National Laboratory
Lunds Universitet
Knut och Alice Wallenbergs Stiftelse
Vetenskapsrådet
Department of Chemical Engineering, Monash University

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Hartl, M., Gillis, R. C., Daemen, L., Olds, D. P., Page, K., Carlson, S., Cheng, Y., Hügle, T., Iverson, E. B., Ramirez-Cuesta, A. J., Lee, Y., & Muhrer, G. (2016). Hydrogen adsorption on two catalysts for the ortho- to parahydrogen conversion: Cr-doped silica and ferric oxide gel. Physical Chemistry Chemical Physics, 18(26), 17281-17293. https://doi.org/10.1039/c6cp01154c

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title = "Hydrogen adsorption on two catalysts for the ortho- to parahydrogen conversion: Cr-doped silica and ferric oxide gel",

abstract = "Molecular hydrogen exists in two spin-rotation coupled states: parahydrogen and orthohydrogen. Due to the variation of energy with rotational level, the occupation of ortho- and parahydrogen states is temperature dependent, with parahydrogen being the dominant species at low temperatures. The equilibrium at 20 K (99.8% parahydrogen) can be reached by natural conversion only after a lengthy process. With the use of a suitable catalyst, this process can be shortened significantly. Two types of commercial catalysts currently being used for ortho- to parahydrogen conversion are: iron(iii) oxide (Fe2O3, IONEX{\textregistered}), and chromium(ii) oxide doped silica catalyst (CrO·SiO2, OXISORB{\textregistered}). We investigate the interaction of ortho- and parahydrogen with the surfaces of these ortho-para conversion catalysts using neutron vibrational spectroscopy. The catalytic surfaces have been characterized using X-ray absorption fine structure (XAFS) and X-ray/neutron pair distribution function measurements.",

author = "Monika Hartl and Gillis, {Robert Chad} and Luke Daemen and Olds, {Daniel P.} and Katherine Page and Stefan Carlson and Yongqiang Cheng and Thomas H{\"u}gle and Iverson, {Erik B.} and Ramirez-Cuesta, {A. J.} and Yongjoong Lee and G{\"u}nter Muhrer",

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doi = "10.1039/c6cp01154c",

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AU - Gillis, Robert Chad

AU - Daemen, Luke

AU - Olds, Daniel P.

AU - Page, Katherine

AU - Carlson, Stefan

AU - Cheng, Yongqiang

AU - Hügle, Thomas

AU - Iverson, Erik B.

AU - Ramirez-Cuesta, A. J.

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N2 - Molecular hydrogen exists in two spin-rotation coupled states: parahydrogen and orthohydrogen. Due to the variation of energy with rotational level, the occupation of ortho- and parahydrogen states is temperature dependent, with parahydrogen being the dominant species at low temperatures. The equilibrium at 20 K (99.8% parahydrogen) can be reached by natural conversion only after a lengthy process. With the use of a suitable catalyst, this process can be shortened significantly. Two types of commercial catalysts currently being used for ortho- to parahydrogen conversion are: iron(iii) oxide (Fe2O3, IONEX®), and chromium(ii) oxide doped silica catalyst (CrO·SiO2, OXISORB®). We investigate the interaction of ortho- and parahydrogen with the surfaces of these ortho-para conversion catalysts using neutron vibrational spectroscopy. The catalytic surfaces have been characterized using X-ray absorption fine structure (XAFS) and X-ray/neutron pair distribution function measurements.

AB - Molecular hydrogen exists in two spin-rotation coupled states: parahydrogen and orthohydrogen. Due to the variation of energy with rotational level, the occupation of ortho- and parahydrogen states is temperature dependent, with parahydrogen being the dominant species at low temperatures. The equilibrium at 20 K (99.8% parahydrogen) can be reached by natural conversion only after a lengthy process. With the use of a suitable catalyst, this process can be shortened significantly. Two types of commercial catalysts currently being used for ortho- to parahydrogen conversion are: iron(iii) oxide (Fe2O3, IONEX®), and chromium(ii) oxide doped silica catalyst (CrO·SiO2, OXISORB®). We investigate the interaction of ortho- and parahydrogen with the surfaces of these ortho-para conversion catalysts using neutron vibrational spectroscopy. The catalytic surfaces have been characterized using X-ray absorption fine structure (XAFS) and X-ray/neutron pair distribution function measurements.

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Hydrogen adsorption on two catalysts for the ortho- to parahydrogen conversion: Cr-doped silica and ferric oxide gel

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