Lu, Xiuyuan and Roldan Martinez, Alberto  ORCID: https://orcid.org/0000-0003-0353-9004
2024.
Ammonia cracking on single-atom catalysts: A mechanistic and microkinetic study.
Applied Catalysis A: General
673
, 119589.
10.1016/j.apcata.2024.119589
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Abstract
Ammonia cracking has been identified as a crucial step to unlocking a sustainable economy. Using the density functional theory, we modeled transition metal single-atom catalysts (SACs) supported on graphene and nitrogen-modified graphene to investigate the catalytic NH3 cracking process. The results showed that (i) N-modified graphene secures the transition metal atoms (M) stronger than C-matrixes, and (ii) structures with three anchoring nitrogens (MN3) are more reactive than MN4 ones. On IrN3 and RuN3 SAC models, the N2 evolution determines the total rate, while, on RhN3-SAC, it is the NH3 dehydrogenation. Temperature-programmed desorption simulations on SACs showed variations compared to extended metal surfaces. Batch reactor simulations were employed to balance the sequence of elementary steps as a function of the temperature, revealing the overall NH3 cracking activity. Results suggested IrN3 and RhN3 are strong candidates for NH3 cracking at temperatures as low as 230 °C.
| Item Type: | Article |
|---|---|
| Date Type: | Publication |
| Status: | Published |
| Schools: | Professional Services > Advanced Research Computing @ Cardiff (ARCCA) Research Institutes & Centres > Cardiff Catalysis Institute (CCI) Schools > Chemistry |
| Publisher: | Elsevier |
| ISSN: | 0926-860X |
| Funders: | EPSRC |
| Date of First Compliant Deposit: | 21 February 2024 |
| Date of Acceptance: | 29 January 2024 |
| Last Modified: | 20 Jun 2025 15:59 |
| URI: | https://orca.cardiff.ac.uk/id/eprint/166434 |
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