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Here, we report, inspired by molecular chemistry, the assembly of a bimetallic nickel system grafted onto mesoporous SBA\u201015 (Ni\u2010NDI\u2010APTES@SBA\u201015\n                    <jats:sub>250<\/jats:sub>\n                    ). The well\u2010defined mesostructure of SBA\u201015 enables the immobilization of dinuclear nickel units while preserving their proximity and cooperative reactivity. Comprehensive characterization, including PXRD, N\n                    <jats:sub>2<\/jats:sub>\n                    physisorption, DRIFT\u2010IR, S\/TEM, XPS, EA, ICP\u2010OES, TGA, and solid\u2010state NMR, confirms the successful incorporation of Ni\n                    <jats:sub>2<\/jats:sub>\n                    species and retention of the mesoporous framework. The catalytic performance of Ni\u2010NDI\u2010APTES@SBA\u201015\n                    <jats:sub>250<\/jats:sub>\n                    was evaluated in the cyclotrimerization of terminal alkynes and compared with representative homogeneous mono\u2010 and dinuclear nickel catalysts. Ni\u2010NDI\u2010APTES@SBA\u201015\n                    <jats:sub>250<\/jats:sub>\n                    preserves the cooperative reactivity and high regioselectivity of the molecular dinuclear catalyst while the surface\u2010bound environment introduces a distinct, substrate\u2010dependent chemoselectivity, as exemplified by the selective monocyclotrimerization of diyne substrates instead of the double cyclization favored by the homogeneous analogue. Moreover, Ni\u2010NDI\u2010APTES@SBA\u201015\n                    <jats:sub>250<\/jats:sub>\n                    combines excellent catalytic performance with operational stability, recyclability, and negligible nickel leaching demonstrating that an immobilized catalyst can preserve molecular bimetallic reactivity while modulating catalytic pathways through the local supported environment.\n                  <\/jats:p>","DOI":"10.1002\/anie.5073615","type":"journal-article","created":{"date-parts":[[2026,8,23]],"date-time":"2026-08-23T18:01:23Z","timestamp":1787508083000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Defined Dinuclear Nickel Sites on Mesoporous Silica Translate Molecular Surface Mimics to Heterogeneous Catalysis"],"prefix":"10.1002","volume":"65","author":[{"given":"Jitpisut","family":"Poolwong","sequence":"first","affiliation":[{"name":"Institut F\u00fcr Anorganische Chemie Eberhard Karls 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