CBET-EPSRC Molecular Engineering of Inhibitors to Self-Assembly: Fundamental structure informing in silico design
Lead Research Organisation:
Science and Technology Facilities Council
Department Name: ISIS Pulsed Neutron & Muon Source
Abstract
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Publications
Headen T
(2019)
Predicting Asphaltene Aggregate Structure from Molecular Dynamics Simulation: Comparison to Neutron Total Scattering Data
in Energy & Fuels
Headen TF
(2023)
The structure of liquid thiophene from total neutron scattering.
in Physical chemistry chemical physics : PCCP
Yang Y
(2021)
Solvent Effects on the Structure of Petroleum Asphaltenes
in Energy & Fuels
| Description | An initial finding from this grant has come from a comparison of atomistic simulation of asphaltenes to wide Q-range neutron diffraction data (published in Energy and Fuels here: DOI: 10.1021/acs.energyfuels.8b03196). Aspahletenes are the heavy fraction of crude oil, that can be responsible for blocking oil pipelines due to it's propensity for aggregation. Computer simulation has become a primary method for understanding this aggregation at the smallest atomistic lengthscale. In initial work from this grant we compared such simulations to experimental measurements of the asphaltene aggregates size and shape measured using neutron scattering. We find that standard simulation methodologies, particularly the box-size and timescales used, under predict the size of the asphaltene aggregates in both the solid and solution state. The system sizes used in the simulations are already close to the limit of what can be achieved using available computation power, highlighting the applicability of "coarse-grained" simulations, where several atoms are represented as a single "bead". The project then went on to run such coarse-grained simulations, allowing access to must longer lengthscales, and developed a workflow for calculating the neutron scattering directly from a coarse-grained simulation. For some systems, these larger simulations showed a much better match to experimental neutron scattering data, but not for all, indicating that the types of molecules used, as well as the system size are important. Finally the project also collected and analysed neutron scattering data from a number of neat liquid aromatic systems (e.g. thiophene, pyrene, phenanthrene). These liquid structure measurements are now being compared with standard simulation methods in follow up work that will help assess the accuracy of these methods in simulation aromatic systems. |
| Exploitation Route | The experimental neutron data can be used as a benchmark to test future simulations studies of asphaltene aggregation. |
| Sectors | Energy |
| URL | https://pubs.acs.org/doi/10.1021/acs.energyfuels.8b03196 |
| Description | CECAM WORKSHOP 1698. Combining multi-scale simulation and scattering for structural analysis of complex systems |
| Amount | SFr. 13,000 (CHF) |
| Funding ID | Workshop 1698. Combining multi-scale simulation and scattering for structural analysis of complex systems |
| Organisation | European Centre of Atomic and Molecular Computation (CECAM) |
| Sector | Charity/Non Profit |
| Country | Switzerland |
| Start | 03/2020 |
| End | 03/2020 |
| Description | Colaboration for a joint scattering and simulation approach to multiscale analysis of PAH solutions. |
| Organisation | Imperial College London |
| Department | Department of Chemical Engineering |
| Country | United Kingdom |
| Sector | Academic/University |
| PI Contribution | This collaboration brings together experts in small angle scattering (Michael Hoepfner - University Utah) and coarse-grained simulation (Erich Muller - Imperial College London) to develop methodologies for the understanding the structure of polyaromatic hydrocarbon (PAH) solutions, including the structure of petroleum asphaltenes. The role of my research at ISIS is to act as a bridge between the atomistic and aggregate lengthscale using both experimental (neutron diffraction) and simulation (atomistic MD) methods. |
| Collaborator Contribution | The group of Michael Hoepfner at University of Utah have been actively involved in neutron scattering experiments for PAH melts and asphaltenic solids and solutions. The group will also be conducting SAXS experiments and other analysis of the chemical makeup of the asphaltenes (e.g. high resolution mass spec), which will be highly complimentary to the neutron data. The group of Erich Muller at Imperial has been conducting coarse-grained simulations of asphaltenes and simple PAH's for comparison to the neutron data collected. This will allow an assessment of the simulation methods used and a more detailed study of asphaltene and PAH solution structure. |
| Impact | * Awarded collaborative neutron beamtime on NIMROD and SANDALS instruments at ISIS (4 experiments) * Joint paper (Headen and Hoepfner) on comparison of atomistic simulations of asphaltene solids and solutions to neutron data (10.1021/acs.energyfuels.8b03196) * Awarded funding of 13000 CHF with E. Muller and G. Jimenez Serratos (Imperial) and Tristan Youngs (ISIS) for a CECAM workshop entitled "Combining multi-scale simulation and scattering for structural analysis of complex systems" to take place in March 2020 at CECAM HQ, Lausanne. |
| Start Year | 2018 |
| Description | Colaboration for a joint scattering and simulation approach to multiscale analysis of PAH solutions. |
| Organisation | University of Utah |
| Department | Department of Chemical Engineering |
| Country | United States |
| Sector | Academic/University |
| PI Contribution | This collaboration brings together experts in small angle scattering (Michael Hoepfner - University Utah) and coarse-grained simulation (Erich Muller - Imperial College London) to develop methodologies for the understanding the structure of polyaromatic hydrocarbon (PAH) solutions, including the structure of petroleum asphaltenes. The role of my research at ISIS is to act as a bridge between the atomistic and aggregate lengthscale using both experimental (neutron diffraction) and simulation (atomistic MD) methods. |
| Collaborator Contribution | The group of Michael Hoepfner at University of Utah have been actively involved in neutron scattering experiments for PAH melts and asphaltenic solids and solutions. The group will also be conducting SAXS experiments and other analysis of the chemical makeup of the asphaltenes (e.g. high resolution mass spec), which will be highly complimentary to the neutron data. The group of Erich Muller at Imperial has been conducting coarse-grained simulations of asphaltenes and simple PAH's for comparison to the neutron data collected. This will allow an assessment of the simulation methods used and a more detailed study of asphaltene and PAH solution structure. |
| Impact | * Awarded collaborative neutron beamtime on NIMROD and SANDALS instruments at ISIS (4 experiments) * Joint paper (Headen and Hoepfner) on comparison of atomistic simulations of asphaltene solids and solutions to neutron data (10.1021/acs.energyfuels.8b03196) * Awarded funding of 13000 CHF with E. Muller and G. Jimenez Serratos (Imperial) and Tristan Youngs (ISIS) for a CECAM workshop entitled "Combining multi-scale simulation and scattering for structural analysis of complex systems" to take place in March 2020 at CECAM HQ, Lausanne. |
| Start Year | 2018 |