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Herein, single-atom ruthenium (Ru) supported on N-heterocyclic carbene (NHC)-functionalized hypercrosslinked polymers were fabricated and applied as recyclable catalysts for the N-formylation of amines using CO2 and H2 as feedstocks. Catalytic evaluations demonstrated that the chemical structure of the NHC ligand had a significant influence on catalytic activity. Specifically, P(PhPy-TPB)-Ru, functionalized with a single pyridine moiety on the NHC ligand, exhibited the optimal catalytic performance, even slightly outperforming its homogeneous counterpart. Furthermore, mechanistic studies indicated that both the base and solvent played pivotal roles in modulating the reaction activity. In particular, the use of methanol as the solvent in the presence of a base significantly enhanced reaction efficiency, which was attributed to the in situ generation of methyl formate as a key intermediate. Notably, the developed catalytic system possessed excellent catalytic efficiency, a broad substrate scope, superior stability, and easy recyclability, allowing the catalyst to be reused for up to eight consecutive cycles without significant loss of catalytic activity.<\/jats:p>","DOI":"10.3390\/molecules31173054","type":"journal-article","created":{"date-parts":[[2026,9,1]],"date-time":"2026-09-01T01:05:26Z","timestamp":1788224726000},"page":"3054","update-policy":"https:\/\/doi.org\/10.3390\/mdpi_crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Single-Atom Ru on N-Heterocyclic Carbene-Functionalized Hypercrosslinked Polymers for N-Formylation of Amines with CO2 and H2"],"prefix":"10.3390","volume":"31","author":[{"given":"Lulu","family":"Dang","sequence":"first","affiliation":[{"name":"Guizhou Provincial Key Laboratory of Green Catalysis and Materials for Resource Conversion, School of Chemistry and Materials Engineering, Liupanshui Normal University, Liupanshui 553004, China"},{"name":"College of Environmental and Chemical Engineering, Dalian University, Dalian 116622, China"}],"role":[{"vocabulary":"crossref","role":"author"},{"role":"methodology","vocabulary":"credit"},{"role":"formal-analysis","vocabulary":"credit"},{"role":"investigation","vocabulary":"credit"},{"role":"resources","vocabulary":"credit"},{"role":"data-curation","vocabulary":"credit"},{"role":"writing-original-draft","vocabulary":"credit"}]},{"given":"Yinfang","family":"Gao","sequence":"additional","affiliation":[{"name":"Guizhou Provincial Key Laboratory of Green Catalysis and Materials for Resource Conversion, School of Chemistry and Materials Engineering, Liupanshui Normal University, Liupanshui 553004, China"},{"name":"College of Environmental and Chemical Engineering, Dalian University, Dalian 116622, China"}],"role":[{"vocabulary":"crossref","role":"author"},{"role":"validation","vocabulary":"credit"},{"role":"investigation","vocabulary":"credit"}]},{"given":"Yali","family":"Wan","sequence":"additional","affiliation":[{"name":"School of Chemical Engineering, Guizhou Institute of Technology, Guiyang 550025, China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0009-0007-1766-2835","authenticated-orcid":false,"given":"Qingsong","family":"Li","sequence":"additional","affiliation":[{"name":"Guizhou Laboratory of Energy Intelligent Development and Efficient Utilization, Guizhou Research Institute of Coal Mine Design Co., Ltd., Guiyang 550025, China"}],"role":[{"vocabulary":"crossref","role":"author"},{"role":"software","vocabulary":"credit"},{"role":"funding-acquisition","vocabulary":"credit"}]},{"given":"Yizhu","family":"Lei","sequence":"additional","affiliation":[{"name":"Guizhou Provincial Key Laboratory of Green Catalysis and Materials for Resource Conversion, School of Chemistry and Materials Engineering, Liupanshui Normal University, Liupanshui 553004, China"},{"name":"College of Environmental and Chemical Engineering, Dalian University, Dalian 116622, China"}],"role":[{"vocabulary":"crossref","role":"author"},{"role":"conceptualization","vocabulary":"credit"},{"role":"methodology","vocabulary":"credit"},{"role":"writing-review-editing","vocabulary":"credit"},{"role":"supervision","vocabulary":"credit"},{"role":"project-administration","vocabulary":"credit"},{"role":"funding-acquisition","vocabulary":"credit"}]}],"member":"1968","published-online":{"date-parts":[[2026,8,31]]},"reference":[{"key":"ref_1","doi-asserted-by":"crossref","first-page":"100905","DOI":"10.1016\/j.pecs.2021.100905","article-title":"Recent Advances in CO2 Hydrogenation to Value-Added Products\u2014Current Challenges And Future Directions","volume":"85","author":"Saeidi","year":"2021","journal-title":"Prog. 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