Quantum Monte Carlo method modeling supported metal catalysis: Ni(111) converting adsorbed formyl 'en route' to hydrogen

TL;DR

This paper applies Quantum Monte Carlo methods to model the dissociation of formyl radicals on Ni(111) surfaces, providing insights into catalytic hydrogen production crucial for sustainable energy solutions.

Contribution

It introduces the use of Quantum Monte Carlo methodology for modeling bond dissociation on a Ni(111) surface, improving accuracy over traditional methods.

Findings

QMC accurately models C-H bond dissociation on Ni(111)

Stabilization of Ni-H linkage observed during formyl dissociation

Gaseous hydrogen release mechanism elucidated

Abstract

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.