Hydrogenation of 9-ethylcarbazole as a prototype of a liquid hydrogen carrier

Katarzyna Morawa Eblagon; Daniel Rentsch; Oliver Friedrichs; Arndt Remhof; Andreas Zuettel; A. J. Ramirez-Cuesta; Shik Chi Tsang

doi:10.1016/j.ijhydene.2010.03.068

Hydrogenation of 9-ethylcarbazole as a prototype of a liquid hydrogen carrier

Katarzyna Morawa Eblagon, Daniel Rentsch, Oliver Friedrichs, Arndt Remhof, Andreas Zuettel, A. J. Ramirez-Cuesta, Shik Chi Tsang

Research output: Contribution to journal › Article › peer-review

160 Scopus citations

Abstract

Liquid organic hydrides, e.g. 9-ethylcarbazole, are potentially interesting hydrogen storage materials because of their reversible hydrogen sorption properties. In the present work, hydrogenation reaction of 9-ethylcarbazole in the molten form was investigated over a wide variety of noble metal and nickel supported catalysts. The catalytic activity of 8.2 × 10^-6 mol-ethylcarbazole/g of metal/s and selectivity of 98% towards a fully hydrogen loaded product were recorded over 5 wt% ruthenium on alumina which was prepared by mild chemical reduction of ruthenium salt. Using this catalyst the theoretical capacity of hydrogen uptake (5.7 wt%) was obtained and the rate of the reaction and activation energy were estimated. Due to its potential high hydrogen storage capacity, this system could be a promising on-board storage candidate for mobile applications. The structures of reaction products and intermediates were identified using 2D NMR techniques. These structures were also predicted to be thermodynamically stable using density functional theory (DFT), matching well with the experimental observations.

Original language	English
Pages (from-to)	11609-11621
Number of pages	13
Journal	International Journal of Hydrogen Energy
Volume	35
Issue number	20
DOIs	https://doi.org/10.1016/j.ijhydene.2010.03.068
State	Published - Oct 2010
Externally published	Yes

Funding

We would like to kindly acknowledge Mr Fernando Eblagon and Dr William Oduro who made a major insightful contribution to this work. Dr K.M. Kerry Yu is acknowledged for the technical support of this work. We would also like to acknowledge Prof Heyong He and Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials at Fudan University, China for TEM images; Dr Sam French of Johnson Matthey, Billingham, UK for fruitful discussion. Finally, we would like to thank University of Oxford, and STFC for financial support, computing resources provided by the U.K. e-science Centre, STFC (SCARF).

Funders	Funder number
Science and Technology Facilities Council
University of Oxford

Keywords

2D NMR
9-Ethylcarbazole
Catalytic hydrogenation
DFT calculations
Hydrogen storage

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

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10.1016/j.ijhydene.2010.03.068

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title = "Hydrogenation of 9-ethylcarbazole as a prototype of a liquid hydrogen carrier",

abstract = "Liquid organic hydrides, e.g. 9-ethylcarbazole, are potentially interesting hydrogen storage materials because of their reversible hydrogen sorption properties. In the present work, hydrogenation reaction of 9-ethylcarbazole in the molten form was investigated over a wide variety of noble metal and nickel supported catalysts. The catalytic activity of 8.2 × 10-6 mol-ethylcarbazole/g of metal/s and selectivity of 98% towards a fully hydrogen loaded product were recorded over 5 wt% ruthenium on alumina which was prepared by mild chemical reduction of ruthenium salt. Using this catalyst the theoretical capacity of hydrogen uptake (5.7 wt%) was obtained and the rate of the reaction and activation energy were estimated. Due to its potential high hydrogen storage capacity, this system could be a promising on-board storage candidate for mobile applications. The structures of reaction products and intermediates were identified using 2D NMR techniques. These structures were also predicted to be thermodynamically stable using density functional theory (DFT), matching well with the experimental observations.",

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doi = "10.1016/j.ijhydene.2010.03.068",

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AU - Eblagon, Katarzyna Morawa

AU - Rentsch, Daniel

AU - Friedrichs, Oliver

AU - Remhof, Arndt

AU - Zuettel, Andreas

AU - Ramirez-Cuesta, A. J.

AU - Tsang, Shik Chi

PY - 2010/10

Y1 - 2010/10

N2 - Liquid organic hydrides, e.g. 9-ethylcarbazole, are potentially interesting hydrogen storage materials because of their reversible hydrogen sorption properties. In the present work, hydrogenation reaction of 9-ethylcarbazole in the molten form was investigated over a wide variety of noble metal and nickel supported catalysts. The catalytic activity of 8.2 × 10-6 mol-ethylcarbazole/g of metal/s and selectivity of 98% towards a fully hydrogen loaded product were recorded over 5 wt% ruthenium on alumina which was prepared by mild chemical reduction of ruthenium salt. Using this catalyst the theoretical capacity of hydrogen uptake (5.7 wt%) was obtained and the rate of the reaction and activation energy were estimated. Due to its potential high hydrogen storage capacity, this system could be a promising on-board storage candidate for mobile applications. The structures of reaction products and intermediates were identified using 2D NMR techniques. These structures were also predicted to be thermodynamically stable using density functional theory (DFT), matching well with the experimental observations.

AB - Liquid organic hydrides, e.g. 9-ethylcarbazole, are potentially interesting hydrogen storage materials because of their reversible hydrogen sorption properties. In the present work, hydrogenation reaction of 9-ethylcarbazole in the molten form was investigated over a wide variety of noble metal and nickel supported catalysts. The catalytic activity of 8.2 × 10-6 mol-ethylcarbazole/g of metal/s and selectivity of 98% towards a fully hydrogen loaded product were recorded over 5 wt% ruthenium on alumina which was prepared by mild chemical reduction of ruthenium salt. Using this catalyst the theoretical capacity of hydrogen uptake (5.7 wt%) was obtained and the rate of the reaction and activation energy were estimated. Due to its potential high hydrogen storage capacity, this system could be a promising on-board storage candidate for mobile applications. The structures of reaction products and intermediates were identified using 2D NMR techniques. These structures were also predicted to be thermodynamically stable using density functional theory (DFT), matching well with the experimental observations.

KW - 2D NMR

KW - 9-Ethylcarbazole

KW - Catalytic hydrogenation

KW - DFT calculations

KW - Hydrogen storage

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Hydrogenation of 9-ethylcarbazole as a prototype of a liquid hydrogen carrier

Abstract

Funding

Keywords

UN SDGs

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