Understanding Liquid Phase Heterogeneous Catalysis to Develop Catalytic Processes
Lead Research Organisation:
University of Manchester
Department Name: Chem Eng and Analytical Science
Abstract
This project is associated with the understanding of heterogeneous catalysts for liquid phase reactions. In particular, we aim to develop a number of techniques by which to probe the reactions within the pores of the heterogeneous catalysts in order to correlate the activity-selectivity of the catalyst with the specific surface and liquid phase interactions. This research will bridge the knowledge gap between understanding the properties of liquids confined in the pores of typical heterogeneous catalysts, and their applications. This lack of understanding of the multiphase interactions underpinning the chemical efficacy of these complex systems is one of the major factors restraining the advancement of many sustainable catalytic processes which involve complex solid/liquid and solid/liquid/gas interfaces. For example, diffusion processes as well as adsorption are critically important in determining the selectivity of these multiphase reactions. However, within the pores of the catalyst in liquid phase reactions it is difficult to evaluate their relative contributions as the observed global kinetics observed are a combination of surface reaction kinetics as well as mass transport. A range of complementary NMR and neutron scattering techniques will be established from which, for example, the diffusion characteristics, pore liquid phase structure and adsorption modes will be elucidated under reaction conditions. The information from these new techniques will be combined with X-ray absorption and infra-red spectroscopy data as well as Density Functional Theory calculations and kinetic modelling in order to obtain a complete description of a gas/liquid reaction within a porous heterogeneous catalyst system under reaction conditions. In order to develop the techniques two families of exemplar selective hydrogenation reactions will be used. The hydrogenation of phenylacetylene to styrene and ethylbenzene will provide a test bed for the techniques which requires low pressures and temperatures and is a sequential reaction. Once established, higher pressure and temperature cells will be developed to enable the study of aromatic acid hydrogenation. The catalyst for this reaction can be tailored to favour a number of products including the aromatic alcohol, ring hydrogenated alcohol or toluidyl derivatives and presents a more challenging process with multiple pathways but one which is industrially very relevant. The project will be undertaken by the Queen's University of Belfast, University of Cambridge, ISIS and Johnson Matthey in close collaboration.
Planned Impact
Using RCUK typology, we see this project as having impact in at least seven areas:
Environmental sustainability, protection & impact
Commercialisation & Exploitation
Increasing public engagement with research & related societal issues
Worldwide academic advancement
Innovative methodologies, equipment, techniques, technologies and cross-disciplinary approaches
Training highly skilled researchers
Enhancing the knowledge economy.
The beneficiaries of the research will be society as a whole, the UK economy and industry. Within the project, strong collaborations exist between Johnson Matthey, ISIS and academic members. The presence of Johnson Matthey provides a direct path for the impact to be realised through potential commercialization of the catalysts that are developed. Although the proposed research concentrates predominantly on the development of new techniques to understand heterogeneously catalysed reactions, the ultimate aim of the project is to be able to develop more efficient catalysts. The general development of catalysts which can undertake more selective transformations on a range of functionalised compounds under benign conditions will increase the scope of the molecules synthesised. In addition, a significant decrease in the environmental impact of the processes undertaken will be achieved.
Catalysis is an enabling technology for many processes with many undertaken in the liquid phase using heterogeneous catalysts. The development of new tools will provide methods by which the actual processes within the catalyst pores can be examined in detail and an understanding of the real rate determining steps can be elucidated. The information will provide data for the whole process development and allow the UK to maintain its competitive edge in the chemicals and energy sectors that are reliant on catalysis. As well as directly benefiting catalysis, the techniques will provide high quality in situ information for use in the polymer industry, sensor devices, oil exploration/oil recovery, electronics industry, environmental protection (for example in adsorption processes) and synthesis of materials (for example supported metal catalysts). These areas have wide economic impact in the UK and will benefit significantly from the ability to monitor the composition as well as the structural changes within solid materials interacting with liquids.
The research project will deliver highly skilled scientists and engineers and will provide an excellent training environment for the researchers. This will be achieved as a result of the multidisciplinary nature of the research which will be extended through collaboration to a wide range of different disciplines including chemistry, chemical engineering, mechanical engineering and physics. In addition, the researchers will benefit from the strong interaction between industry, academia and ISIS. This close cooperation will enable the staff and students in the project to become effective academics or industrialists in the future where these interactions are critical for success.
After protection of the IPR, the results of the research would be disseminated to the academic community through publications in peer-reviewed journals, presentations at major catalysis and NMR conferences and invited lectures. Of significant importance is the dissemination of the new methodologies to the wider community in particular to groups outside the catalysis community who will benefit from the new information obtained leading to wider impact. In addition, the partners will undertake public engagement to relate the research to the benefits of society. This research will form a part of the teacher's conference in QUB, for example, which enables advanced techniques and concepts to be introduced. The teachers will be shown how MRI can be used outside the health sector as well as what neutrons can probe and the concepts of liquid structure.
Environmental sustainability, protection & impact
Commercialisation & Exploitation
Increasing public engagement with research & related societal issues
Worldwide academic advancement
Innovative methodologies, equipment, techniques, technologies and cross-disciplinary approaches
Training highly skilled researchers
Enhancing the knowledge economy.
The beneficiaries of the research will be society as a whole, the UK economy and industry. Within the project, strong collaborations exist between Johnson Matthey, ISIS and academic members. The presence of Johnson Matthey provides a direct path for the impact to be realised through potential commercialization of the catalysts that are developed. Although the proposed research concentrates predominantly on the development of new techniques to understand heterogeneously catalysed reactions, the ultimate aim of the project is to be able to develop more efficient catalysts. The general development of catalysts which can undertake more selective transformations on a range of functionalised compounds under benign conditions will increase the scope of the molecules synthesised. In addition, a significant decrease in the environmental impact of the processes undertaken will be achieved.
Catalysis is an enabling technology for many processes with many undertaken in the liquid phase using heterogeneous catalysts. The development of new tools will provide methods by which the actual processes within the catalyst pores can be examined in detail and an understanding of the real rate determining steps can be elucidated. The information will provide data for the whole process development and allow the UK to maintain its competitive edge in the chemicals and energy sectors that are reliant on catalysis. As well as directly benefiting catalysis, the techniques will provide high quality in situ information for use in the polymer industry, sensor devices, oil exploration/oil recovery, electronics industry, environmental protection (for example in adsorption processes) and synthesis of materials (for example supported metal catalysts). These areas have wide economic impact in the UK and will benefit significantly from the ability to monitor the composition as well as the structural changes within solid materials interacting with liquids.
The research project will deliver highly skilled scientists and engineers and will provide an excellent training environment for the researchers. This will be achieved as a result of the multidisciplinary nature of the research which will be extended through collaboration to a wide range of different disciplines including chemistry, chemical engineering, mechanical engineering and physics. In addition, the researchers will benefit from the strong interaction between industry, academia and ISIS. This close cooperation will enable the staff and students in the project to become effective academics or industrialists in the future where these interactions are critical for success.
After protection of the IPR, the results of the research would be disseminated to the academic community through publications in peer-reviewed journals, presentations at major catalysis and NMR conferences and invited lectures. Of significant importance is the dissemination of the new methodologies to the wider community in particular to groups outside the catalysis community who will benefit from the new information obtained leading to wider impact. In addition, the partners will undertake public engagement to relate the research to the benefits of society. This research will form a part of the teacher's conference in QUB, for example, which enables advanced techniques and concepts to be introduced. The teachers will be shown how MRI can be used outside the health sector as well as what neutrons can probe and the concepts of liquid structure.
Organisations
Publications
Szala-Bilnik J
(2017)
The Structure of Ethylbenzene, Styrene and Phenylacetylene Determined by Total Neutron Scattering.
in Chemphyschem : a European journal of chemical physics and physical chemistry
Leutzsch M
(2018)
An integrated total neutron scattering - NMR approach for the study of heterogeneous catalysis.
in Chemical communications (Cambridge, England)
Falkowska M
(2018)
Confinement Effects on the Benzene Orientational Structure
in Angewandte Chemie
Falkowska Marta
(2018)
What effect does confinement have on the structure of liquid benzene?
in ABSTRACTS OF PAPERS OF THE AMERICAN CHEMICAL SOCIETY
Falkowska M
(2018)
Confinement Effects on the Benzene Orientational Structure.
in Angewandte Chemie (International ed. in English)
Dervin D
(2020)
Probing the dynamics and structure of confined benzene in MCM-41 based catalysts.
in Physical chemistry chemical physics : PCCP
Hughes T
(2021)
Bulk and Confined Benzene-Cyclohexane Mixtures Studied by an Integrated Total Neutron Scattering and NMR Method
in Topics in Catalysis
Description | We have been investigating the structure of confined fluids in catalysts. This structure is being related to the catalyst activity and selectivity for selective hydrogenations |
Exploitation Route | The instrumentation being developed will be of significant use to many structural studies of liquids and solids |
Sectors | Chemicals,Energy,Environment,Manufacturing, including Industrial Biotechology,Pharmaceuticals and Medical Biotechnology |
Description | Johnson Matthey |
Organisation | Johnson Matthey |
Country | United Kingdom |
Sector | Private |
PI Contribution | New methods to understand liquid phase heterogeneous catalysis. |
Collaborator Contribution | Advice on systems to examine from an industrial perspective. |
Impact | None to date |
Start Year | 2016 |
Description | STFC |
Organisation | Science and Technologies Facilities Council (STFC) |
Country | United Kingdom |
Sector | Public |
PI Contribution | Industrial systems to examine and correlation of structure with phyisico-chemical properties and modelling studies. |
Collaborator Contribution | Access to ISIS beamline, modelling and synthetic expertise. |
Impact | No outputs to date. This is multidisciplinary research involving maths, physics, chemistry, mechanical engineering and chemical engineering |
Start Year | 2017 |
Description | University of Cambridge |
Organisation | University of Cambridge |
Country | United Kingdom |
Sector | Academic/University |
PI Contribution | Experimental validation of the modelling and simulation undertaken and incorporation of the models into a broader modelling framework. |
Collaborator Contribution | Equations of state with which to link the molecular scale modelling to the longer scale modelling to enable the prediction of properties for new formulation products. |
Impact | No outputs as yet. This is a multi-disciplinary collaboration involving maths, chemistry, physics, mechanical engineering and chemical engineering |
Start Year | 2017 |
Description | 4th UK Catalysis Conference, Loughborough, UK, 3-5 January 2018 |
Form Of Engagement Activity | A talk or presentation |
Part Of Official Scheme? | No |
Geographic Reach | National |
Primary Audience | Professional Practitioners |
Results and Impact | Reagents confined in catalyst support pores - structural studies by total neutron scattering M. Falkowska, D. T. Bowron, H. Manyar, T. G. A. Youngs, C. Hardacre (talk) |
Year(s) Of Engagement Activity | 2018 |
Description | Combined Neutron Scattering and NMR Spectroscopy Studies Examining Benzene Hydrogenation in Porous Media |
Form Of Engagement Activity | A talk or presentation |
Part Of Official Scheme? | No |
Geographic Reach | International |
Primary Audience | Third sector organisations |
Results and Impact | Talk at International Seminar on Neutron Scattering Investigation in Condensed Matter |
Year(s) Of Engagement Activity | 2018 |
Description | Conference presentation at UK Catalysis Hub Combined total neutron scattering and NMR studies of confined hydrocarbons. (July 2021) |
Form Of Engagement Activity | A talk or presentation |
Part Of Official Scheme? | No |
Geographic Reach | National |
Primary Audience | Third sector organisations |
Results and Impact | UK Catalysis Hub conference presentation |
Year(s) Of Engagement Activity | 2021 |
Description | Effect of confinement on the structure of liquid benzene |
Form Of Engagement Activity | A talk or presentation |
Part Of Official Scheme? | No |
Geographic Reach | International |
Primary Audience | Third sector organisations |
Results and Impact | Talk at 8th International Workshop on the Characterization of Porous Materials, Delray Beach, USA, May 2018 |
Year(s) Of Engagement Activity | 2018 |
Description | Faraday Joint Interest Group Conference 2017, Warwick, UK, 11-13 April 2017 |
Form Of Engagement Activity | A talk or presentation |
Part Of Official Scheme? | No |
Geographic Reach | National |
Primary Audience | Professional Practitioners |
Results and Impact | Structural studies on aromatic and aliphatic liquids under confinement by total neutron scattering (talk) M. Falkowska, D. T. Bowron, H. Manyar, T. G. A. Youngs, C. Hardacre |
Year(s) Of Engagement Activity | 2017 |
Description | Talk at NMUM2020 |
Form Of Engagement Activity | A talk or presentation |
Part Of Official Scheme? | No |
Geographic Reach | International |
Primary Audience | Third sector organisations |
Results and Impact | Research Presentation |
Year(s) Of Engagement Activity | 2020 |
Description | Talk at UKCC 2020 |
Form Of Engagement Activity | A talk or presentation |
Part Of Official Scheme? | No |
Geographic Reach | International |
Primary Audience | Third sector organisations |
Results and Impact | Research presentation |
Year(s) Of Engagement Activity | 2020 |
Description | The ISIS Disordered Materials Group meeting, Abingdon, UK , 14-15 February 2017 |
Form Of Engagement Activity | A talk or presentation |
Part Of Official Scheme? | No |
Geographic Reach | National |
Primary Audience | Professional Practitioners |
Results and Impact | Structure of liquids in the MCM-41 pores (Invited talk) M. Falkowska, D. T. Bowron, C. Hardacre, T. G. A. Youngs |
Year(s) Of Engagement Activity | 2017 |
Description | Total Neutron Scattering integrated with NMR to Study Heterogeneous Catalysis |
Form Of Engagement Activity | A talk or presentation |
Part Of Official Scheme? | No |
Geographic Reach | International |
Primary Audience | Third sector organisations |
Results and Impact | Talk at 5th UK Catalysis Conference, Loughborough, UK, Jan 2019 |
Year(s) Of Engagement Activity | 2019 |
Description | Total Neutron Scattering integrated with NMR to Study Heterogeneous Catalysis |
Form Of Engagement Activity | A talk or presentation |
Part Of Official Scheme? | No |
Geographic Reach | National |
Primary Audience | Third sector organisations |
Results and Impact | Talk at Neutron and Muon Science and User Meeting, Warwick, UK, Apr 2019 |
Year(s) Of Engagement Activity | 2019 |
Description | UKCC 2017 |
Form Of Engagement Activity | A talk or presentation |
Part Of Official Scheme? | No |
Geographic Reach | National |
Primary Audience | Professional Practitioners |
Results and Impact | Confined liquids studied by total neutron scattering, M. Falkowska, D. T. Bowron, H. Manyar, T. G. A. Youngs, C. Hardacre (talk) |
Year(s) Of Engagement Activity | 2017 |
Description | What effect does confinement have on the structure of liquid benzene? |
Form Of Engagement Activity | A talk or presentation |
Part Of Official Scheme? | No |
Geographic Reach | International |
Primary Audience | Third sector organisations |
Results and Impact | Talkl at 256th ACS National Meeting, Boston, USA, Sep 2018 |
Year(s) Of Engagement Activity | 2018 |