New routes towards the activation of N2
Lead Research Organisation:
University of Glasgow
Department Name: School of Chemistry
Abstract
Building upon the classic work of Shilov in the area, using recent advances in structural elucidation (such as synchrotron based PDF) to identify the active phases in the system. This knowledge will then be adapted to the identification of potential biomimetically based heterogeneous catalysis for N2 activation. The project will therefore involve closely integrated synthesis, characterisation and catalytic activity evaluation. The work will also form a distinct component of a larger research effort conducted within the general area of N2 activation which is currently running within the research group.
Organisations
People |
ORCID iD |
Justin Hargreaves (Primary Supervisor) | |
Angela Daisley (Student) |
Publications
Daisley A
(2019)
The role of interstitial species upon the ammonia synthesis activity of ternary Fe-Mo-C(N) and Ni-Mo-C(N) phases
in Journal of Energy Chemistry
Daisley A
(2020)
A comparison of the activities of various supported catalysts for ammonia synthesis
in Catalysis Today
Studentship Projects
Project Reference | Relationship | Related To | Start | End | Student Name |
---|---|---|---|---|---|
EP/N509668/1 | 30/09/2016 | 29/09/2021 | |||
2366989 | Studentship | EP/N509668/1 | 02/10/2016 | 29/06/2020 | Angela Daisley |
Description | Approximately 40% of the world's population is maintained by fertiliser produced from ammonia that is formed via the Haber Bosch Process. As the population continues to increase, ammonia synthesis is becoming more important. However, this industrial process requires high temperatures and pressures and when considered in its entirety, including the production of the hydrogen feedstream, is responsible for 2% of the world's energy demand and 1.6% of global manmade CO2 emissions. Therefore, it would be of benefit if a more active ammonia synthesis catalyst could be developed that operates under more moderate conditions, allowing localised and sustainable production. This would result in a lowering of the CO2 footprint as the fertiliser would not need to travel over large distances and the hydrogen could be produced by more environmentally friendly methods, such as from renewable energy. One potential material that may have a higher activity are metal nitrides, which produce ammonia by using the nitrogen contained in the material. The development of more active materials requires an understanding of what makes a material active and this knowledge can be used to improve the activity. The activity of a material may be influenced by its composition or the way the atoms are arranged within the structure. The aim of this research was to gain an understanding on the effect these composition-activity and structure-activity relationships of metal nitrides, carbides and carbonitrides have on ammonia synthesis. Metal carbides were investigated for their ammonia synthesis capabilities, to examine whether nitrogen was required in these materials in order for them to be active. A new approach was used to attempt to synthesise the Ni2Mo3C phase via reaction of Ni2Mo3N with a carbon source, such as methane. However, Ni2Mo3C could not be synthesised and a carbonitride phase was formed instead. Ni6Mo6C and Ni3Mo3C were prepared by new synthesis methods for these materials. The carbides were observed to have an induction period before they became active and during this period, nitrogen was incorporated into the material. Therefore, this research was able to show that nitrogen may be required in these materials in order for them to be active. The nitrides were reduced under a mixture of hydrogen and argon to investigate the reactivity of the nitrogen within these materials. It was found that the ternary nitrides had different nitrogen reactivities, with some almost completely unreactive under these conditions. Therefore, this research suggests that both composition and structure type have an effect on the activity of the metal nitrides. Finally, osmium was investigated to examine whether it was active in bulk form or a more highly dispersed form. Osmium has been historically shown to have a high activity for ammonia synthesis. Understanding and improving this activity could be of benefit to developing more active materials. It was observed that osmium had greater activity when supported and therefore, when more dispersed. |
Exploitation Route | The work will provide new knowledge for researchers working in the area of nitrogen activation and ammonia synthesis. It will also provide guidance for researchers within the research group. These outcomes may help with the development of more active materials for ammonia synthesis that operate at lower conditions than the Haber Bosch Process. Further research could be performed by applying other experimental techniques such as X-ray photoelectron spectroscopy (XPS) and X-ray absorbance spectroscopy (XAS). This would provide further information on the effect structure and composition have on the activity. |
Sectors | Agriculture Food and Drink Chemicals Environment |
Description | PhD Mobility Fund Scholarship Award |
Amount | £1,000 (GBP) |
Organisation | University of Glasgow |
Sector | Academic/University |
Country | United Kingdom |
Start | 04/2019 |
Description | SURCAT Europacat Bursary Award |
Amount | £400 (GBP) |
Organisation | Royal Society of Chemistry |
Sector | Charity/Non Profit |
Country | United Kingdom |
Start | 05/2019 |
Description | Travel Scholarship Award |
Amount | £200 (GBP) |
Organisation | University of Glasgow |
Sector | Academic/University |
Country | United Kingdom |
Start | 09/2018 |
Description | West of Scotland Local Section Travel Bursary Award |
Amount | £200 (GBP) |
Organisation | Royal Society of Chemistry |
Sector | Charity/Non Profit |
Country | United Kingdom |
Start | 02/2019 |
Description | Presentation (Ecosse) |
Form Of Engagement Activity | A talk or presentation |
Part Of Official Scheme? | No |
Geographic Reach | Regional |
Primary Audience | Postgraduate students |
Results and Impact | Presentation on part of research to academics and postgraduate students. The purpose was to engage with other researchers and show research to others. Resulted in discussion with other academics. |
Year(s) Of Engagement Activity | 2018 |
Description | Presentation (Europacat) |
Form Of Engagement Activity | A talk or presentation |
Part Of Official Scheme? | No |
Geographic Reach | International |
Primary Audience | Other audiences |
Results and Impact | Presentation on part of research to academics and postgraduate students. The purpose was to engage with other researchers and gain interest in the research. Resulted in discussion with other academics and networking. |
Year(s) Of Engagement Activity | 2019 |