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During syngas conversion, sintering is known to deactivate the catalyst owing to the loss of active surface area. However, the growth of nanoparticles might induce the formation of new active sites such as grain boundaries (GBs) which perform differently from the original nanoparticles. Herein, we reported a unique Cu\u2010based catalyst, Cu nanoparticles with in situ generated GBs confined in zeolite Y (denoted as activated Cu\/Y), which exhibited a high selectivity for C<jats:sub>5+<\/jats:sub> hydrocarbons (65.3\u2005C%) during syngas conversion. Such high selectivity for long\u2010chain products distinguished activated Cu\/Y from typical copper\u2010based catalysts which mainly catalyze methanol synthesis. This unique performance was attributed to the GBs, while the zeolite assisted the stabilization through spatial confinement. Specifically, the GBs enabled H\u2010assisted dissociation of CO and subsequent hydrogenation into CH<jats:sub>x<\/jats:sub>*. CH<jats:sub>x<\/jats:sub>* species not only serve as the initiator but also directly polymerize on Cu GBs, known as the carbide mechanism. Meanwhile, the synergy of GBs and their vicinal low\u2010index facets led to the CO insertion where non\u2010dissociative adsorbed CO on low\u2010index facets migrated to GBs and inserted into the metal\u2010alkyl bond for the chain growth.<\/jats:p>","DOI":"10.1002\/anie.202404983","type":"journal-article","created":{"date-parts":[[2024,4,2]],"date-time":"2024-04-02T15:47:50Z","timestamp":1712072870000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":14,"title":["The Importance of Sintering\u2010Induced Grain Boundaries in Copper Catalysis to Improve Carbon\u2010Carbon Coupling"],"prefix":"10.1002","volume":"63","author":[{"given":"Wenlong","family":"Wu","sequence":"first","affiliation":[{"name":"Deep Space Exploration Laboratory  Hefei 230088 P.\u2005R. 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