Sustainable nitrogen activation 2023 - Book of abstracts

Gas-phase synthesis of HCN via chemical looping fixation of N 2 Spencer Mizon 1 , Dr Sven Titlbach 2 , Dr Christian Holtze 2 , Prof. Klaus Hellgardt 1 1 Imperial College, UK, 2 BASF,Ludwigshafen, Germany Industrial synthesis of ammonia has allowed the world’s population to flourish over the past century however consequences of its manufacturing have led to it being responsible for 1.9% of annual global anthropogenic CO 2 emissions 1 . Improvements to operating conditions and less harmful sources of feedstocks for the Haber- Bosch process will aid it lessening the impact currently felt but an alternative approach is to attack the supply chain of ammonia by reacting nitrogen directly with materials which can yield products that currently rely upon ammonia. A process for direct C-N coupling from N 2 and hydrocarbon feedstock would eliminate a massive portion of the damaging emissions produced from typical methods and would change the global market of building block molecular synthesis. Herein lies the work carried out in this poster in which experimental studies observing the ability for hydrogen cyanide (HCN), a strongly desired intermediate for the manufacture of acrylics and nylons, to be produced via reaction with N 2 and CH 4 utilising a high-temperature chemical looping methodology. Screening a wide range of catalyst candidiates, the different behaviours that are observed in a hydrocarbon environment at high temperatures was explored and the degree to which HCN was produced via analysis of product gas streams using a temperature programmed reaction system. Rationalising the different outcomes of each reaction using relative bonding contributions in the catalyst, ternary metal systems have been targeted to optimise the degree to which carbon and nitrogen couple (in both gas-phase and solid-phase). Ultimately, these results build a chemical framework for the design of catalytic materials to couple nitrogen and hydrocarbons together directly without the need for ammonia. References 1. J. Norskov and J. Chen, Sustainable Ammonia Synthesis, US DoE Round Table Report, 2016.

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