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.

Publications

10 25 50

publication icon
Silverwood IP (2010) Quantification of surface species present on a nickel/alumina methane reforming catalyst. in Physical chemistry chemical physics : PCCP

 
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