Integrated Computational Solutions for Catalysis

Lead Research Organisation: University College London
Department Name: Chemistry

Abstract

The aim of this Platform grant is to initiate a new protocol for catalytic modelling where the different components relating to synthesis and growth; crystal, surface and active site structure; reactivity and deactivation; are fully integrated to achieve a comprehensive description of catalytic processes at the molecular level.
The platform funding will be used first, to stabilise and strengthen the joint programmes of the applicants in catalytic science and surface chemistry; key areas of computational materials science that have developed strongly over the last five years with EPSRC support. Secondly, the platform grant will be used to facilitate the development of our programme in new directions of strategic priority to EPSRC and high potential impact to the UK economy and Society in general.
The investigators have collaborated for more than ten years, initially in the field of computational mineralogy, followed by work on eScience technologies, and more recently in surface and catalytic science. They have joint publications and joint research grants and have co-supervised a number of doctoral students and postdoctoral research fellows. Most recently, they have initiated a computational programme on surface processes in interplanetary space, in collaboration with experimental groups in UCL and Arizona. The applicants' teams are firmly embedded in the large UCL materials modelling community and have strong interactions with industry and experimental groups within UCL and elsewhere in the UK and abroad.
The Platform grant is people-centric and will be used to provide flexible, underpinning support to allow strategic planning of our research programme. Although there will be a number of related sub-themes, the platform will be run as a whole thus promoting the maximum synergy between its different components and staff. The Platform funding will be used first to allow a coherent and strategic approach in those areas where our team has currently a very high profile (catalysis, surface science and reactivity); secondly to allow us to develop in new directions which respond to EPSRC priority themes and have the potential for high impact, eg. materials for energy applications (solid oxide fuel cells, hydrogen storage, photo-catalysis) and the environment (biomass utilisation, carbon capture and conversion); and thirdly to foster long-term international collaborations.
Staff funded by the grant will be assigned to themes and projects and not to individual investigators, thereby enhancing the strategic nature of the platform support. The flexibility of the Platform grant will be used to appoint a critical mass of key people to carry out research which best uses their particular skills, but applied to a number of topical applications areas. This approach will encourage the PDRAs to work effectively as a team and to take a broader view of research issues beyond individual projects. In addition, the Platform programme will seek to enhance the PDRAs' professional development by encouraging research independence and the initiation of scientific collaborations, in preparation for applications for competitive lectureships/fellowships or positions in industry.
In summary, the Platform grant will allow us the flexibility to (i) draw together our team into an integrated predictive computational research programme on "Total Catalysis"; (ii) carry out feasibility studies in new and strategic areas of catalytic science; (iii) initiate overseas collaborations and recruit promising researchers from abroad; (iv) retain key staff with unique expertise between relevant project funding, (v) carry through successful research that is close to commercial implementation beyond the duration of an individual project, and (v) assist in career development of the staff.

Planned Impact

Catalysis is the lynchpin of a large number of industrial processes, which are instrumental in maintaining global wealth and health, as well as playing a key role in developing processes that are both environmentally and economically sustainable. This project and its outcomes will therefore impact on:

* Society, by developing effective and more benign catalysts to allow the use of sustainable alternatives to fossil fuels, thus assisting in maintaining our quality of life;
* The Economy, through the design of new catalysts for alternative routes to important products. Catalysis is at the heart of the chemical industry - an immensely successful and important part of the overall UK economy, generating in excess of £50 billion per annum.
* Knowledge, both academic and commercial, as the new computational models will deliver significant advances in catalyst design and optimisation and more widely in materials (nano-)science;
* People, through the technical expertise developed by the researchers during the project, the training received by them in societal and ethical issues and the transferable skills developed in engagement with the media, the general public, policy makers and legislators.

In addition to the obvious benefits to academic researchers in the field (see Academic Beneficiaries section), the research will benefit in particular (i) ) the UK and global commercial sector, but also (ii) the general public, (iii) the public sector, and, more speculatively (iv) voluntary workers and charities.

(i) Commercial sector
Many industrially crucial processes, e.g. the water-gas shift reaction, still take place under extreme conditions of pressure and temperature, thus making them environmentally unsustainable in the long term. Furthermore, existing catalysts often depend on the use of expensive noble metals (Pt, Pd, Au) and transition metal compounds (e.g. ceria), which are often only available from limited sources and countries, or toxic elements, such as chromium in iron-oxide catalysts, whose use is increasingly limited by EU legislation. The development of novel catalysts, which operature under milder conditions and can utilise sustainable alternatives to fossil fuels, will clearly benefit both the catalyst manufacturing industry and the companies employing these catalysts in their production processes, e.g. pharmaceuticals and fine chemicals manufacturers, oil refineries and energy industries generally.

(ii) The general public
Everyone, whether living in highly industrialised countries or, increasingly, in the developing world, is dependent on products produced by catalytic processes. Moreover, catalytic science will be vital in developing technologies for CO2 conversion and the utilisation of agricultural residues for bio-energy production, which is of particular benefit to primarily agricultural societies, such as those in West Africa. Underpinning research on catalytic science therefore has very broad economic and societal benefits.

(iii) Government/Public Sector
With ever more stringent legislation put in place to guarantee a cascade of international agreements to reduce CO2 and other greenhouse gases to acceptable levels, viable routes to reduction in CO2 generation are clearly of prime importance to policy makers and legislators. As biomass is currently the only truly sustainable alternative source of energy, and with lingering public opposition to nuclear energy and more (off-shore) wind farms, bio-energy is clearly of interest.

(iv) Third Sector
More speculative beneficiaries of this research are charities and voluntary organisations. Catalytic science is of key importance in environmental remediation and energy technologies. With the consequences of environmental degradation and rising energy costs leading to increased disruption and hardship, the call on voluntary aid organisations is growing rapidly and alternative energy sources would alleviate this burden to sustainable levels.

Publications

10 25 50

Related Projects

Project Reference Relationship Related To Start End Award Value
EP/K009567/1 15/09/2013 31/12/2014 £1,215,346
EP/K009567/2 Transfer EP/K009567/1 01/04/2015 30/11/2019 £1,019,445
 
Description The aim of this Platform grant is to initiate a new protocol for catalytic modelling where the different components relating to synthesis and growth; crystal, surface and active site structure; reactivity and deactivation; are fully integrated to achieve a comprehensive description of catalytic processes at the molecular level.

The aim of the platform funding is to stabilise and strengthen our research programmes in catalytic science and surface chemistry; key areas of computational materials science that have developed strongly over the last five years. Secondly, the platform grant aims to facilitate the development of our programme in new directions of strategic priority to EPSRC and high potential impact to the UK economy and Society in general.

The Platform grant is people-centric and used to provide flexible, underpinning support to allow strategic planning of our research programme. Although there are a number of related sub-themes, the platform will be run as a whole thus promoting the maximum synergy between its different components and staff. The Platform funding will be used first to allow a coherent and strategic approach in those areas where our team has currently a very high profile (catalysis, surface science and reactivity); secondly to allow us to develop in new directions which respond to EPSRC priority themes and have the potential for high impact, eg. materials for energy applications (solid oxide fuel cells, hydrogen storage, photo-catalysis) and the environment (biomass utilisation, carbon capture and conversion); and thirdly to foster long-term international collaborations.

In the first year of the grant, we have made excellent progress in a number of fields:

1. We have identified the major surface structures and properties of molybdenum carbide, a promising material for catalytic applications;

2. Our calculations have shown the activity of the reactive iron sulfide mackinawite towards the catalytic conversion of exhaust gases NO and NO2;

3. Potential homogeneous catalysts based on base metal iron, rather than more expensive noble metals, have been investigated for their activity towards the conversion of biomass to fuels and chemicals.
Exploitation Route Catalysis is a cornerstone of the chemical industry and our computational investigations, identifying catalytic pathways and mechanisms and suggesting new catalysts could be taken forward by industrial catalysts manufacturers to improve existing catalytic systems or design new procedures.
Sectors Chemicals,Energy,Environment

 
Description Peer-reviewed scientific publications, presentations at international conferences, exchange visits with overseas research groups
First Year Of Impact 2013
Sector Chemicals,Energy,Environment
Impact Types Societal,Economic

 
Description Bath programme
Amount £3,333,000 (GBP)
Funding ID EP/K016288/1 
Organisation Engineering and Physical Sciences Research Council (EPSRC) 
Sector Public
Country United Kingdom
Start 11/2013 
End 11/2018
 
Description DFID
Amount £1,243,000 (GBP)
Organisation The Royal Society 
Sector Charity/Non Profit
Country United Kingdom
Start 03/2015 
End 02/2020
 
Description FOM
Amount € 250,000 (EUR)
Organisation Netherlands Organisation for Scientific Research (NWO) 
Department Foundation for Fundamental Research on Matter
Sector Public
Country Netherlands
Start 10/2014 
End 09/2017
 
Title Carbon dioxide reduction on strontium titanate perovskites - data 
Description The dataset was generated during a density functional theory study of the mechanism of reaction of CO2 to CO using strontium titanate (SrTiO3) perovskites. Technologies such as photocatalysis which mimic the natural process of photosynthesis to convert the CO2 molecule into useful hydrocarbons are extremely attractive. The detailed knowledge of the reaction mechanism is crucial to help improve the SrTiO3 conversion efficiency. Data consist of a sequential set of 12 VASP CONTCAR files containing the optimised coordinates for all the intermediates and transition states along the reaction mechanism from CO2 to CO. 
Type Of Material Database/Collection of data 
Year Produced 2019 
Provided To Others? Yes  
URL https://research.cardiff.ac.uk/converis/portal/detail/Dataset/86887209?auxfun=&lang=en_GB
 
Title Ethylene carbonate adsorption on the major surfaces of lithium manganese oxide Li1-xMn2O4 spinel (0.000 < x < 0.375) - data 
Description The ethylene carbonate (EC) adsorption on the spinel LiMn2O4 {001}, {011} and {111} surfaces has been studied using density functional theory (DFT) calculations. Spinel LiMn2O4 is a promising cathode material that has a 3D structure that allows the reversible Li+ diffusion during charge/discharge processes. This work involves studying the charge transfers from the major LiMn2O4 surfaces to the EC molecule and the effect of EC adsorption on the particle morphologies. The data described here are ASCII files containing the vibrational modes, charge transfers, particle morphologies of the adsorbed surfaces before and after adsorption. Calculations were carried out using the Vienna Ab-initio Simulation Package (VASP). 
Type Of Material Database/Collection of data 
Year Produced 2020 
Provided To Others? Yes  
URL https://research.cardiff.ac.uk/converis/portal/detail/Dataset/85116020?auxfun=&lang=en_GB
 
Title Interaction of SO2 with the Platinum (001), (011) and (111) Surfaces: A DFT Study - data 
Description >Density functional theory (DFT) calculations were uasd with long-range dispersion corrections to study the interaction of SO2 with Pt (001), (011), and (111) surfaces. Platinum is a noble metal that is widely used for the electro-catalytic production of H2, which surface reactivity towards SO2 is not yet fully understood. The work involved studying the surface energies of the mayor Pt surfaces with 4 layers, adsorption energy for SO2 on these surfaces, the thermodynamic effect of SO2 on Pt and the changes in Pt. The data described here are Excel files containing the data for the atomic charges and displacements for the pristine surfaces, as well as the SO2 adsorbed surfaces. Benchmarking results with the pristine 6- and 8 layered surfaces and the adsorption of SO2 on these surfaces. Calculations were carried out using the Vienna Ab-initio Simulation Package (VASP). 
Type Of Material Database/Collection of data 
Year Produced 2020 
Provided To Others? Yes  
URL https://research.cardiff.ac.uk/converis/portal/detail/Dataset/102392045?auxfun=&lang=en_GB
 
Title Substitutional doping with Ag of the zinc oxide ZnO(0001) surface - dataset 
Description The substitutional doping with Ag of the reconstructed and Zn-deficient zinc oxide ZnO(0001) surface has been investigated using density functional theory (DFT) calculations. Wurtzite ZnO is used in the latest generation of devices for detecting biomarkers during the diagnosis of several diseases as well as for continuous air quality monitoring. Fine-tuning the reactivity of these sensors towards the molecules of interest requires functionalization of their surfaces using metallic dopants and nanoparticles. The data described here are the ASCII files containing the atomic charges and displacements as well as density of states for the pristine and Ag-doped ZnO(0001) surfaces. Calculations were carried out using the Vienna Ab-initio Simulation Package (VASP). 
Type Of Material Database/Collection of data 
Year Produced 2019 
Provided To Others? Yes  
 
Title Substitutional doping with Fe of the zinc oxide ZnO(10-10) surfaces 
Description The substitutional doping with Fe of the two non-polar terminations of the zinc oxide ZnO(10-10) surface has been investigated using density functional theory (DFT) calculations. Wurtzite ZnO is a candidate material for the detection of volatile organic compounds (VOC), which properties can be tuned through doping and decoration with clusters of metal oxide nanoparticles for the highly selective and sensitive detection of ethanol vapours. The data described here are the ASCII files containing the atomic charges, displacements and spin moments of the wurtzite ZnO bulk phase and the pristine as well as the Fe-doped ZnO(10-10) surfaces. Calculations were carried out using the Vienna Ab-initio Simulation Package (VASP). 
Type Of Material Database/Collection of data 
Year Produced 2019 
Provided To Others? Yes  
 
Title Surface Oxidation of Troilite FeS 
Description The dataset was generated during density functional theory and X-ray photoelectron spectroscopy studies of the prismatic surfaces of the troilite FeS catalyst in an oxidising environment. Iron sulfides are very reactive towards molecular oxygen, which is easily incorporated into their surfaces. In order for the catalytic mechanisms to be understood, it is crucial to achieve a detailed knowledge of the oxidised substrate available to the reactants. Data consist of 1) VASP CONTCAR files with the optimised coordinates of the clean (01-10) surface of troilite and incorporating one, two and three oxygen atoms; 2) Plain text files containing the Fe2p and S2p XPS spectra of Fe(1-x)S nanoparticles. 
Type Of Material Database/Collection of data 
Year Produced 2018 
Provided To Others? Yes  
 
Title Tautomerization of Phenol at the External Lewis Acid Sites of Sc-, Fe- and Ga-substituted Zeolite MFI 
Description The data set was generated during the computational study of the tautomerization of phenol at the external Lewis acid sites of zeolite MFI. The Lewis sites consist on three-coordinated Sc, Fe and Ga atoms replacing one of the framework Si atom. This work intents to analyse the possible role of doped zeolites when they are used as supports during the hydroprocessing of lignin-derived compounds. The data set consists on excel files with the following information: (i) The Bader charges and projected density of states (PDOS) of the metal-substituted zeolite. (ii) The reaction pathways for the dehydration of the metal-substituted silanol at the external surface of zeolite MFI. (iii) The reaction pathways for the tautomerization of phenol at the external surface of zeolite MFI. These files follows the same order of the information presented in the main manuscript and they are numbered according to the subsection within the manuscript. 
Type Of Material Database/Collection of data 
Year Produced 2018 
Provided To Others? Yes