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Across these regimes, Si\u2500H activation and H\n                    <jats:sub>2<\/jats:sub>\n                    evolution arise from the interplay of structure, coordination environment, and access to reactive geometries. In extended silicon systems, hydrogen release is governed by structure\u2010dependent recombinative desorption processes. Zintl phases bridge solid\u2010state and molecular silicon chemistry by enabling transfer of polyanionic silicon units into solution, thereby providing access to discrete Si\u2500H reactivity. In molecular systems, metal\u2010mediated and metal\u2010free pathways contribute to hydrogen release, including oxidative addition, \u03c3\u2010bond metathesis, electrophilic activation, cooperative heterolysis, and donor\u2010assisted Si\u2500H activation. These mechanistic manifolds form a continuum in which variations in coordination environment and electronic structure determine whether dehydrocoupling, hydrogen transfer, or bond\u2010forming processes dominate. A recurring mechanistic feature is the involvement of higher\u2010coordinate silicon species. However, productive H\n                    <jats:sub>2<\/jats:sub>\n                    evolution depends on their formation, but also on the ability of the silicon framework to access reactive geometries through fluxional behavior and dynamic permutational isomerism. Overall, silicon\u2010based hydrogen\u2010release chemistry illustrates how structure, coordination, and molecular dynamics collectively govern bond activation and hydrogen evolution, providing a conceptual basis for the design of silicon\u2010based hydrogen storage and release systems.\n                  <\/jats:p>","DOI":"10.1002\/chem.71612","type":"journal-article","created":{"date-parts":[[2026,9,1]],"date-time":"2026-09-01T04:42:07Z","timestamp":1788237727000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":1,"title":["Hydrogen Release From Silicon\u2500Hydrogen Systems: From Surface Chemistry to Higher\u2010Coordinate Molecular Mechanisms"],"prefix":"10.1002","author":[{"given":"Robin","family":"Rothfelder","sequence":"first","affiliation":[{"name":"Faculty of Chemistry and Pharmacy, Institute of Inorganic Chemistry University of Regensburg  Regensburg 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