Towards a molecular understanding of deactivation issues in methane reforming catalysts
Lead Research Organisation:
Science and Technology Facilities Council
Department Name: ISIS Pulsed Neutron & Muon Source
Abstract
This research proposal brings together a grouping of specialists in surface chemistry, heterogeneous catalysis, solid state chemistry, infrared spectroscopy, Raman spectroscopy and inelastic neutron scattering spectroscopy to identify the critical factors responsible for maintaining hydrogen yields in methane reforming catalysts. Ormerod has already prepared, and partially characterised, a number of methane reforming catalysts that display a wide range of performance, in terms of hydrogen selectivity and operational lifetime. Whereas the standard formulations display the expected catalyst deactivation characteristics, some of the modified catalysts exhibit excellent hydrogen selectivity that can be maintained over extended periods of time, i.e. minimal deactivation is observed. A workplan is presented whereby the research team will develop a mechanistic understanding of why the 'good' catalysts favour high hydrogen selectivity and avoid the carbon laydown processes, that lead to the formation of surface oligermic species and, ultimately, catalyst deactivation. This multi-disciplinary and multi-institutional research proposal has direct connections to energy requirements of the UK chemical industry and, moreover, targets key areas of the science base as highlighted in the recent Whiteside's report and the EPSRC's Research Priorities and Opportunities document.
People |
ORCID iD |
Stewart Parker (Principal Investigator) |
Publications
Lennon D
(2011)
Inelastic neutron scattering and isotopic substitution experiments and their application in examining the CO2 reforming of methane over alumina-supported catalysts
in ACS National Meeting Book of Abstracts
McFarlane A
(2013)
The application of inelastic neutron scattering to investigate the steam reforming of methane over an alumina-supported nickel catalyst
in Chemical Physics
Ormerod R
(2010)
Conversion of waste biogas over supported nickel catalysts and solid oxide fuel cell anodes: Carbon deposition, sulphur poisoning and characterisation of hydrocarbonaceous overlayers formed during reforming
in ACS National Meeting Book of Abstracts
Parker S
(2011)
Vibrational Spectroscopy with Neutrons: A Review of New Directions
in Applied Spectroscopy
Silverwood I
(2010)
Persistent species formed during the carbon dioxide reforming of methane over a nickel-alumina catalyst
in Catalysis Today
Silverwood IP
(2012)
Application of inelastic neutron scattering to studies of CO2 reforming of methane over alumina-supported nickel and gold-doped nickel catalysts.
in Physical chemistry chemical physics : PCCP
Silverwood IP
(2010)
Quantification of surface species present on a nickel/alumina methane reforming catalyst.
in Physical chemistry chemical physics : PCCP
Silverwood IP
(2011)
Experimental arrangements suitable for the acquisition of inelastic neutron scattering spectra of heterogeneous catalysts.
in The Review of scientific instruments
Warringham R
(2014)
Sample environment issues relevant to the acquisition of inelastic neutron scattering measurements of heterogeneous catalyst samples
in Journal of Physics: Conference Series
Description | Deactivation of methane reforming catalysts by carbon is a major industrial problem. In this work we have looked at carbon formation on the industrially used Ni/alumina catalysts under steam reforming and dry reforming operation. The nature of the carbon formed, whether filamentous (and largely graphitic) or amorphous depends crucially on the source of the alumina and the catalyst preparation conditions. Dry reforming using CO2 as the oxidant is potenetially a very attractive route for its utilisation: in addirion to the hydrogen produced, we found that at steady state 95% of the CO2 is converted to economically useful CO, Isotope studies show that CO2 does contribute to the carbon laydown. Overall, we find that the catalysts are very efficient at cycling hydrogen (very little is retained on the catalyst) surface but much less so for carbon. |
Exploitation Route | The use of dry reforming has considerable potential as a way to make economic use of carbon dioxide. The work was presented at national and international conferences (including two invited talks). Five papers have been published on the work and a further one is under review. The work formed the basis of a PhD thesis by a student. |
Sectors | Chemicals,Energy,Environment |
Description | Sasol Technology |
Amount | £25,000 (GBP) |
Funding ID | 2008-1 |
Organisation | Sasol Technology |
Sector | Private |
Country | South Africa |
Start |
Description | Sasol Technology |
Amount | £65,000 (GBP) |
Funding ID | 2010-2 |
Organisation | Sasol Technology |
Sector | Private |
Country | South Africa |
Start |
Description | Sasol Technology |
Amount | £25,000 (GBP) |
Organisation | Sasol Technology |
Sector | Private |
Country | South Africa |
Start | 10/2010 |
End | 06/2013 |
Description | Sasol Technology |
Amount | £65,000 (GBP) |
Organisation | Sasol Technology |
Sector | Private |
Country | South Africa |
Start | 10/2012 |
End | 06/2015 |