Initial Catalysis Design Projects
Project 1: Developments in neutron scattering to characterise adsorbed species.
This project seeks to develop the use of neutron diffraction techniques available at ISIS (eg NIMROD) to study adsorbed overlayers on catalyst surfaces in real time. One of the primary areas of work will be to investigate the poorly understood nature of catalyst deactivation and the formation of adsorbed carbonaceous material.
Initial aims include two demonstration projects are envisaged: the first is to structurally characterise a molecular adsorbate on a catalyst and the second is to follow the formation of a hydrocarbonaceous overlayer on a working catalyst. To develop in situ cells and build a suitable (or adapt an existing) gas handling rig. As part of a separate collaboration with Aqura GmbH, Parker has been awarded beamtime on SANDALS to study surface hydrides on β-PdH. This beamtime will be used to test a first generation of cells
Project 2: Technical developments for probing the nature of the active site and catalytic mechanisms.
This area of work focuses on one of the key benefits of the RCaH – its location and access to facilities on the RAL campus (Diamond, ISIS and the Central Laser Facility). The project will develop the techniques required for understanding the fundamental processes in catalysis; the nature of the active site at the atomic and molecular level, mechanistic pathways for enhancing catalytic synergy and deactivation.
There are three main areas where resource will be focused initially:(i) Commissioning of the combined XAFS/DRIFTS set-up: Development of control systems and integration ready for 1st experiments in 2014.(ii) Assist Belfast with the relocation of the SPACI-MS system to Harwell. (iii) Commissioning of silicon fabricated microfluidic reactors for in situ infrared measurements on
B22 (March ’14)
Project 3: Active-Site Design for Effecting and Affecting Catalysis at the Nano-scale.
The aim is to (i) design novel stable monodispersed and multimetallic nanoparticles and clusters by controlling the crucial parameters of size, shape and morphology (ii) to understand the parameters for controlling final morphology and (iii) to study the effect of metal-support interactions.
Develop Microfluidic synthesis using silicon cells based on systematic studies of colloidal synthesis conditions (e.g.Au nanoparticles) and then monitor changes in a continuous flow reactor and microfluidic cell for insitu studies (linking with Project 2) and comparison with larger scale reactions in the vapourtech reactor.
Use similar methods to develop and optimise bimetallic (Au-Ag, Au-Pd) nano systems.
Project 4: Microporous and Hierarchical Architectures with Multifunctional Active Sites.
A wide-range of microporous and hybrid hierarchical architectures containing a diverse array of active sites will be rationally designed. The main objectives are (i) understanding the fundamental principles associated with the design of active sites with atomic precision within molecular frameworks; (ii) probing the electronic and structural environment, at the molecular level, and (iii) eliciting catalytic synergies with controlled pore-apertures for maximising shape-selective, regiospecific and enantioselective catalytic transformations.
Create Porous structures such as MOFF and Zeolites including AlPOs and polyoxometalates to look at how double substitutions affect the active site and catalyst performance. Link with Project 2 to probe the structure and environment of the substitutions.
Transfer the knowledge gained from the first part to look at new systems and different substitutions and probe how this affects catalytic performance.
Project 5: Multiscale modelling of catalytic pathways and kinetics.
The project aims to develop a multiscale modelling framework for catalyst and reactor design, ranging from the molecular to the reactor-scale. The framework will employ first-principles methodologies at the nano-scale, kinetic Monte Carlo (KMC) at the micro-scale, micro-kinetic models at the meso-scale, and CFD and reactor models at the macro-scale.
Initial aims include Fully modelling Au-Pd nanoparticles for Water Gas Shift reactions looking at i) structures, ii) mechanism, and iii) kinetic monte-carlo simulations.
Project 6: Hierarchically Structured Porous Catalysts with Superior Performance due to Nano-confinement and Multiscale Optimisation of the Pore Space.
This project provides a platform (i) to steer nano-confinement effects (of homogeneous complexes, enzymes and nanoparticles) to enhance intrinsic catalytic activity, selectivity and stability, and (ii) to utilize the intrinsic catalytic performance (as realized at the nanoscale) up to macroscopic scales by optimal engineering and synthesis of the 3D hierarchical pore network architecture and active site location.
Aims include i) Construct model for hierarchically structured meso/macroporous zeolite composites, and diffusion and reaction in these composites. The model integrates detailed, atomistic information), but allows to simulate entire catalyst particles or pellets, thus permitting direct comparison with experiments. ii) Apply hierarchically structured porous catalyst model to alkylation reaction, to design a hierarchically structured porous catalyst that maximizes selectivity toward desired alkylation product, at high conversion and iii) Construct model for nano-confinement in mesopores: construct coarse-grained model that allows us to study the effect of pore diameter and surface chemistry on homogeneous catalytic complexes anchored to the surface; complements the efforts on micropores project 4, spectroscopic work at Harwell, chemical transformation work in Bath