2022/12/04 by Duchamp, Noëlie, Feschet, Chloé, Tarragó, Maria M. +1
Chemical Engineering · Materials Science · Physics and Astronomy · #Advanced Chemical Physics Studies #Catalysis and Oxidation Reactions #Catalytic Processes in Materials Science #Chemical Physics (physics.chem-ph) #FOS: Physical sciences #Materials Science (cond-mat.mtrl-sci)
paper · pdf · doi:10.48550/arxiv.2212.01823
openalex publication_date 2022/12/04 · openalex created_date 2022/12/18 · openalex updated_date 2026/07/28
Hydrogen production as a clean, sustainable replacement for fossil fuels is gathering pace. Doubling the capacity of Paris-CDG airport has been halted, even with the upcoming Olympic Games, until hydrogen-powered planes can be used. It is thus timely to work on catalytic selective hydrogen production and optimise catalyst structure. Over 90 % of all chemical manufacture uses a solid catalyst. This work describes the dissociation of a C-H bond in formyl radicals, chemisorbed at Ni(111) that stabilises the ensuing Ni-H linkage. As part of this mechanistic step, gaseous hydrogen is given off. Many chemical reactions involve bond-dissociation. This process is often the key to rate-limiting reaction steps at solid surfaces. Since bond-breaking is poorly described by Hartree-Fock and DFT methods, our embedded active site approach is used. This work demonstrates Quantum Monte Carlo (QMC) methodology using a very simple monolayer Ni(111) surface model.