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Tandem Catalysts Design towards Efficient Selective Catalytic Oxidation of ammonia (TCatSCO)

Lead Research Organisation: UNIVERSITY COLLEGE LONDON
Department Name: Chemical Engineering

Abstract

Selective catalytic oxidation (SCO) of NH3 to N2 is one of the best ways to eliminate NH3 emissions. A major challenge in NH3-SCO is to achieve high conversion for a wide operating temperature range, avoiding over-oxidation to N2O and N2. The commercial Pt catalysts have full NH3 conversion at low temperatures but suffer from low N2 selectivity. To mitigate this challenge, it is crucial to limit the overoxidation of NH3. The researcher proposes that by integrating highly active Pt with highly selective Cu or Pd, new tandem Pt-CuO/Al2O3 and Pt-Pd/Al2O3 catalysts will form and help improve the N2 formation. The simultaneously high conversion and selectivity can be achieved by modifying the bimetallic catalysts with atomic-level precision. This will change the NH3 adsorption, N-N formation and the O2 activation on the surface, which can be probed via a series of operando spectroscopy, including X-ray absorption fine structure, X-ray emission, Infrared, and electron paramagnetic resonance. The possible intermediates and reaction pathways for internal selective catalytic reduction mechanism and N2- mechanism will be explored with those operando methods combined with density-functional theory calculations. The results are expected to provide a solution towards the upcoming Euro-7 regulations, which are valid from 2025 onwards for NH3 emissions.

Publications

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Related Projects

Project Reference Relationship Related To Start End Award Value
EP/X022986/1 31/08/2022 05/07/2023 £204,031
EP/X022986/2 Transfer EP/X022986/1 31/08/2023 24/10/2024 £117,318
 
Description We have designed a binary catalyst that shows better performance than the commercial ones. The Pt component is used to oxidize NH3 into either N2 or NO. The CuO component will then reduce the NO with NH3 to form N2 as the inert product. With only 0.6 wt% Pt atoms dispersed on the surface of Cu nanoparticles,
simultaneously high conversion and selectivity are achieved over a wide temperature window.
The catalysts preparation is based on standard precipitation and galvanic exchange procedure, which can be easily
scale up. In the next stage, the researchers will:
1. Evaluate the catalysts under realistic NH3 slip conditions and test the on stream stability
2. Scaling up the production of the catalysts to kg level by collaborating with industrial partners
3. Deliver prototypes of catalyst bed for NH3 emission control
Exploitation Route The catalysts developed by this funding can be taken over by industry to produce more active catalysts for NH3 slip reactions.
Sectors Chemicals

Manufacturing

including Industrial Biotechology

Transport

 
Description In general, the we have discovered a new material that has the potential of replacing commercial ones. A UK patent application has been made and initial contacts have been secured with several companies including Johnson Matthey, BASF and Umicore. In the next stage, we will 1. Evaluate the catalysts under realistic NH3 slip condi?ons and test the on stream stability 2. Scaling up the production of the catalysts to kg level by collaborating with industrial partners 3. Deliver prototypes of catalyst bed for NH3 emission control
First Year Of Impact 2023
Sector Chemicals,Manufacturing, including Industrial Biotechology,Transport
 
Title Kinetics of partial reaction 
Description With the QXAFS method, we were able to measure the kinetics of the Cu+ oxidation and Cu2+ reduction within a turnover of NH3 oxidation. Comparing such kinetics with the full reaction reals that Cu2+ reduction by NH3 is the rate-determining step of the reaction. This method is generally applicable to all catalytic reactions and will help improve the accuracy of kinetic models. 
Type Of Material Technology assay or reagent 
Year Produced 2023 
Provided To Others? Yes  
Impact The current kinetic modelings are all based on the full reaction and the assumption that the active centres do not change during the reaction. This has significantly limits the application of kinetic models. We provide here the new method that look into the individual steps of a reaction. Being able to measure the formation and conversion rates of each intermediate step can help build accurate models that are not possible before. This is fundamentally important for chemical engineering and chemistry. 
 
Description N2O emission control in nitric acide production 
Organisation Johnson Matthey
Country United Kingdom 
Sector Private 
PI Contribution We are developing a reactor for NH3 oxidation reaction. We will measure the reaction kinetics and understand the N2O emission during the reaction.
Collaborator Contribution The partner provide 1 million GBP to this project. The funding is provided to develop the reactor, support 4 year PDRA and one 4 year PhD studentship.
Impact We just start the project, so there is no output so far.
Start Year 2022
 
Title NH3 Slip Catalyst for Clean Air Technology 
Description Selective catalytc oxidation (SCO) of NH3 to N2 is one of the best ways to eliminate NH3 emissions. The major challenge in NH3-SCO is to achieve high conversion over a wide operating temperature range, while avoiding overoxidation to NOx. Commercial Pt catalysts have full NH3 conversion at low temperatures but suffer from low N2 selectivity. Its low temperature performance needs to be improved to meet the upcoming EU7 emission standards. 
IP Reference  
Protection Patent / Patent application
Year Protection Granted 2023
Licensed No
Impact We have been discussing with several companies to the follow on development of this technology