Fate of hydrogen sulphide on refractory oxide nanoparticles via foundation model-accelerated atomistic modelling and in situ spectroscopy
4 affiliations
- 1Departament de Química, Universitat Autònoma de Barcelona 08193 Bellaterra Catalonia Spain
- 2Dipartimento di Chimica and Nanomaterials for Industry and Sustainability (NIS) Centre, Università degli Studi di Torino via P. Giuria 7 I-10125 Torino Italy
- 3Dipartimento di Chimica, Biologia e Biotecnologie, Università degli Studi di Perugia Via Elce di Sotto 8 I-06123 Perugia Italy
- 4Accademia delle Scienze di Torino Via Maria Vittoria 3 I-10123 Torino Italy
Abstract
Understanding the intricate interactions between hydrogen sulphide (H2S) and complex metal oxides is of paramount interest for both advancing industrial catalysis, such as H2S conversion to H2, and fundamental perspectives, such as unravelling the role of refractory interstellar dust in the sulphur depletion problem or in prebiotic catalysis. In both settings, the chemistry is governed by the high-surface-area, structurally heterogeneous terminations that dominate at the nanoscale, including facets of differing stability, steps, and point defects; however, the vast configurational space of these chemically diverse and reactive interfaces makes exhaustive first-principles sampling prohibitively expensive. In this work, we address this challenge by integrating unbiased, automated high-throughput adsorption sampling with readily available atomistic foundation models in a hierarchical screen-and-refine workflow. We systematically investigate H2S adsorption across three prototypical refractory oxide materials: amorphous silica, forsterite (Mg2SiO4), and pristine and defective MgO. A state-of-the-art foundation model was used to explore, without chemical bias, the configurational space of H2S–surface interactions, revealing a broad range of surface phenomena, transitioning from non-covalent, hydrogen-bonded physisorption on hydroxylated silica to dissociative adsorption on Mg2SiO4 facets and highly reactive Schottky divacancy pairs in MgO. The resulting atomistic datasets are assessed against experimental in situ infrared (IR) spectroscopy. Our multiconfigurational compound IR spectra, computed at the density functional theory level for a set of machine-learning potential refined minima, reproduce the position, ordering and qualitative shape of the experimental features, including the complex low-frequency tails and the progressive red-shifting of characteristic H–S and O–H stretching modes across the three materials. This combined theoretical and experimental framework establishes a transferable methodology for the study of refractory nanostructured surfaces in Earth and astrochemical settings, and provides a pipeline for the rational design of next-generation catalysts for sustainable processes and green chemistry applications.
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BibTeX
@article{matestorres2026fate,
title = {{Fate of hydrogen sulphide on refractory oxide nanoparticles via foundation model-accelerated atomistic modelling and in situ spectroscopy}},
author = {Eric Mates-Torres and Lorenzo Mino and Guillermo Escolano-Casado and Nadia Balucani and Piero Ugliengo and Albert Rimola},
journal = {Nanoscale},
year = {2026},
month = nov,
doi = {10.1039/d6nr02993k},
url = {https://doi.org/10.1039/d6nr02993k},
note = {CC BY 3.0},
}
RIS
TY - JOUR
TI - Fate of hydrogen sulphide on refractory oxide nanoparticles via foundation model-accelerated atomistic modelling and in situ spectroscopy
AU - Eric Mates-Torres
AU - Lorenzo Mino
AU - Guillermo Escolano-Casado
AU - Nadia Balucani
AU - Piero Ugliengo
AU - Albert Rimola
PY - 2026
DA - 2026/11/02
JO - Nanoscale
DO - 10.1039/d6nr02993k
UR - https://doi.org/10.1039/d6nr02993k
AB - Understanding the intricate interactions between hydrogen sulphide (H2S) and complex metal oxides is of paramount interest for both advancing industrial catalysis, such as H2S conversion to H2, and fundamental perspectives, such as unravelling the role of refractory interstellar dust in the sulphur depletion problem or in prebiotic catalysis. In both settings, the chemistry is governed by the high-surface-area, structurally heterogeneous terminations that dominate at the nanoscale, including facets of differing stability, steps, and point defects; however, the vast configurational space of these chemically diverse and reactive interfaces makes exhaustive first-principles sampling prohibitively expensive. In this work, we address this challenge by integrating unbiased, automated high-throughput adsorption sampling with readily available atomistic foundation models in a hierarchical screen-and-refine workflow. We systematically investigate H2S adsorption across three prototypical refractory oxide materials: amorphous silica, forsterite (Mg2SiO4), and pristine and defective MgO. A state-of-the-art foundation model was used to explore, without chemical bias, the configurational space of H2S–surface interactions, revealing a broad range of surface phenomena, transitioning from non-covalent, hydrogen-bonded physisorption on hydroxylated silica to dissociative adsorption on Mg2SiO4 facets and highly reactive Schottky divacancy pairs in MgO. The resulting atomistic datasets are assessed against experimental in situ infrared (IR) spectroscopy. Our multiconfigurational compound IR spectra, computed at the density functional theory level for a set of machine-learning potential refined minima, reproduce the position, ordering and qualitative shape of the experimental features, including the complex low-frequency tails and the progressive red-shifting of characteristic H–S and O–H stretching modes across the three materials. This combined theoretical and experimental framework establishes a transferable methodology for the study of refractory nanostructured surfaces in Earth and astrochemical settings, and provides a pipeline for the rational design of next-generation catalysts for sustainable processes and green chemistry applications.
SN - 2040-3364
SN - 2040-3372
ER -