{"status":"ok","message-type":"work","message-version":"1.0.0","message":{"indexed":{"date-parts":[[2025,10,10]],"date-time":"2025-10-10T01:16:38Z","timestamp":1760058998080,"version":"build-2065373602"},"reference-count":53,"publisher":"MDPI AG","issue":"10","license":[{"start":{"date-parts":[[2025,5,14]],"date-time":"2025-05-14T00:00:00Z","timestamp":1747180800000},"content-version":"vor","delay-in-days":0,"URL":"https:\/\/creativecommons.org\/licenses\/by\/4.0\/"}],"funder":[{"name":"National Agency for Research and Development (ANID, Chile)","award":["1241066","1251871","1221019"],"award-info":[{"award-number":["1241066","1251871","1221019"]}]}],"content-domain":{"domain":[],"crossmark-restriction":false},"short-container-title":["Molecules"],"abstract":"<jats:p>Silicon\u2013lithium clusters are promising candidates for hydrogen storage due to their lightweight composition, high gravimetric capacities, and favorable non-covalent binding characteristics. In this study, we employ density functional theory (DFT), global optimization (AUTOMATON and Kick\u2013MEP), and Born\u2013Oppenheimer molecular dynamics (BOMD) simulations to evaluate the structural stability and hydrogen storage performance of key Li\u2013Si systems. The exploration of their potential energy surface (PES) reveals that the true global minima of Li6Si6 and Li10Si10 differ markedly from those of the earlier Si\u2013Li structures proposed as structural analogs of aromatic hydrocarbons such as benzene and naphthalene. Instead, these clusters adopt compact geometries composed of one or two Si4 (Td) units and a Si2 dimer, all stabilized by surrounding Li atoms. Motivated by the recurrence of the Si4\u2013Td motif, we explore oligomers of Li4Si4, which can be viewed as electronically transmuted analogues of P4, confirming the additive H2 uptake across dimer, trimer, and tetramer assemblies. Within the series of Si\u2013Li clusters evaluated, the Li12Si5 sandwich complex, featuring a \u03c3-aromatic Si510\u2212 ring encapsulated by two Li65+ moieties, achieves the highest hydrogen capacity, adsorbing 34 H2 molecules with a gravimetric density of 23.45 wt%. Its enhanced performance arises from the high density of accessible Li+ adsorption sites and the electronic stabilization afforded by delocalized \u03c3-bonding. BOMD simulations at 300 and 400 K confirm their dynamic stability and reversible storage behavior, while analysis of the interaction regions confirms that hydrogen adsorption proceeds via weak, dispersion-driven physisorption. These findings clarify the structure\u2013property relationships in Si\u2013Li clusters and provide a basis for designing modular, lightweight, and thermally stable hydrogen storage materials.<\/jats:p>","DOI":"10.3390\/molecules30102163","type":"journal-article","created":{"date-parts":[[2025,5,14]],"date-time":"2025-05-14T12:22:17Z","timestamp":1747225337000},"page":"2163","update-policy":"https:\/\/doi.org\/10.3390\/mdpi_crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["From Aromatic Motifs to Cluster-Assembled Materials: Silicon\u2013Lithium Nanoclusters for Hydrogen Storage Applications"],"prefix":"10.3390","volume":"30","author":[{"ORCID":"https:\/\/orcid.org\/0009-0006-6442-8059","authenticated-orcid":false,"given":"Williams","family":"Garc\u00eda-Argote","sequence":"first","affiliation":[{"name":"Centro de Investigaci\u00f3n para el Dise\u00f1o de Materiales (CEDEM), Facultad de Ciencias Exactas, Departamento de Ciencias Qu\u00edmicas, Universidad Andr\u00e9s Bello, Avenida Rep\u00fablica 275, Santiago 8370146, Chile"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"ORCID":"https:\/\/orcid.org\/0009-0001-2239-5790","authenticated-orcid":false,"given":"Erika","family":"Medel","sequence":"additional","affiliation":[{"name":"Departamento de Qu\u00edmica, Divisi\u00f3n de Ciencias B\u00e1sicas e Ingenier\u00eda, Universidad Aut\u00f3noma Metropolitana, Iztapalapa CP 09340 CDMX, Mexico"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-0160-0337","authenticated-orcid":false,"given":"Diego","family":"Inostroza","sequence":"additional","affiliation":[{"name":"Departamento de F\u00edsica, Facultad de Ciencias, Universidad de Chile, \u00d1u\u00f1oa, Santiago 7800024, Chile"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-3501-7905","authenticated-orcid":false,"given":"Alejandro","family":"V\u00e1squez-Espinal","sequence":"additional","affiliation":[{"name":"Qu\u00edmica y Farmacia, Facultad de Ciencias de la Salud, Universidad Arturo Prat, Casilla 121, Iquique 1100000, Chile"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-2290-169X","authenticated-orcid":false,"given":"Jos\u00e9","family":"Solar-Encinas","sequence":"additional","affiliation":[{"name":"Laboratory of Theoretical Chemistry, Faculty of Chemistry and Biology, University of Santiago de Chile (USACH), Santiago 8370146, Chile"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-4210-1868","authenticated-orcid":false,"given":"Luis","family":"Leyva-Parra","sequence":"additional","affiliation":[{"name":"Centro de Investigaci\u00f3n en Ingenier\u00eda de Materiales (CIIM), Facultad de Ingenier\u00eda y Arquitectura, Universidad Central de Chile (UCEN), Santa Isabel 1186, Santiago 8370146, Chile"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-9363-2730","authenticated-orcid":false,"given":"Lina Mar\u00eda","family":"Ruiz","sequence":"additional","affiliation":[{"name":"Institute of Biomedical Sciences, Faculty of Health Sciences, Universidad Aut\u00f3noma de Chile, Santiago 8910060, Chile"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-8993-9353","authenticated-orcid":false,"given":"Osvaldo","family":"Ya\u00f1ez","sequence":"additional","affiliation":[{"name":"Centro de Modelaci\u00f3n Ambiental y Din\u00e1mica de Sistemas (CEMADIS), Facultad de Ingenier\u00eda y Negocios, Universidad de Las Am\u00e9ricas, Santiago 7500975, Chile"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-6061-8879","authenticated-orcid":false,"given":"William","family":"Tiznado","sequence":"additional","affiliation":[{"name":"Centro de Investigaci\u00f3n para el Dise\u00f1o de Materiales (CEDEM), Facultad de Ciencias Exactas, Departamento de Ciencias Qu\u00edmicas, Universidad Andr\u00e9s Bello, Avenida Rep\u00fablica 275, Santiago 8370146, Chile"}],"role":[{"role":"author","vocabulary":"crossref"}]}],"member":"1968","published-online":{"date-parts":[[2025,5,14]]},"reference":[{"key":"ref_1","doi-asserted-by":"crossref","first-page":"112743","DOI":"10.1016\/j.rser.2022.112743","article-title":"Hydrogen storage methods: Review and current status","volume":"167","author":"Usman","year":"2022","journal-title":"Renew. 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