| EPSRC Reference: |
EP/N510038/1 |
| Title: |
Electrochemical conversion of nitrogen to ammonia-experimental and theoretical studies |
| Principal Investigator: |
Metz, Dr S |
| Other Investigators: |
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| Project Partners: |
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| Department: |
Scientific Computing Department |
| Organisation: |
STFC Laboratories (Grouped) |
| Scheme: |
Technology Programme |
| Starts: |
01 February 2016 |
Ends: |
31 January 2017 |
Value (£): |
23,790
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| EPSRC Research Topic Classifications: |
| Catalysis & Applied Catalysis |
Electrochemical Science & Eng. |
| Sustainable Energy Vectors |
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Summary on Grant Application Form |
This University of Oxford led project will demonstrate the feasibility of producing ammonia, an energy vector with multiple applications, in a carbon free synthesis powered by renewable energy. This part of the study aims to simulate the electrochemical syntheses of ammonia from nitrogen and hydrogen/water.
Bulk models to represent the experimental systems in a realistic fashion At the first stage, we will focus on electrode materials with varying amounts of Samarium, namely Sm2-xSrxNiO4 (with x=0.4, 0.5, 0.8 and 1.2) and SmFe0.7Cu0.3- xNixO3 (with x=0, 0.1, 0.2 and 0.3), that have been reported in the literature. These systems have been characterized experimentally and shown a strong difference in catalytic activity towards electrochemical synthesis of ammonia. Aim of the computational simulations is to understand the difference in activity in order to help decision making on potential improved experimental systems and/or predict trends in catalytic activity.
To succeed in this ambitions, a broad skill set of computational modelling techniques is required. As this might become a re-appearing pattern for newly identified materials or potential catalysts, we'll establish a protocol that can be followed for any new material of interest for the electrodes This will form the basis for the work undertaken in the first part of the project.
- Generation of starting structure of bulk material based on available experimental evidence
- Monte Carlo (MC) simulations (using the in-house code DL_MONTE ) to the thermodynamically stable phase
- Validation of the model by theoretical reproduction of bulk properties, e.g. the ionic conductivity with Adaptive Kinetic Monte Carlo (AKMC) techniques (using the in-house code DL_AKMC )
Establishing a bulk structure is key for validation of most experimental values. The reactivity of the electrode, however, depends on the catalytically active surface. In the secnd part of the project, we'll therefore establishe a reliable and reproducible protocol to generate different crystal surfaces and determine the likelihood of their appearance in the experimental systems (using the in-house code DL_POLY , and/or CRYSTAL)To keep the computational efficiency as low as possible, we'll establish realistic, but still efficient representations of the systems of interest by using a cutting cluster approach.
In the third part of the study, we'll use these representations to study the reactivity at the interface, taking into account different competing reactions:We'll simulate the catalytic conversion of nitrogen to ammonia, which is the reaction we are actually interested in. In addition, we'll investigate potential competing reaction like the generation of hydrogen at the cathode (2H+ + 2e- -> H2), reducing the Faradaic efficiency of the MEAs. Namely, we will evaluate the influence of the electrolyte, and/or electromagnetic fields on the reaction energies, but also on the geometries (an effect that is normally neglected).
At the end of the project, we aim to be able to use computational simulations to understand and to be anle to make predictions on the difference in activity in a diverse group of materials in order to help decision making on potential improved experimental systems and/or predict trends in catalytic activity.
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Key Findings |
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This information can now be found on Gateway to Research (GtR) http://gtr.rcuk.ac.uk
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Potential use in non-academic contexts |
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This information can now be found on Gateway to Research (GtR) http://gtr.rcuk.ac.uk
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Impacts |
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| Description |
This information can now be found on Gateway to Research (GtR) http://gtr.rcuk.ac.uk |
| Summary |
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| Date Materialised |
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Sectors submitted by the Researcher |
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This information can now be found on Gateway to Research (GtR) http://gtr.rcuk.ac.uk
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