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Herein, a series of ionic liquids (ILs) with excellent CO\n                    <jats:sub>2<\/jats:sub>\n                    activation capabilities was designed and combined with copper(I) chloride to form a synergistic catalytic system. This system efficiently promoted the carboxylative cyclization of propargylic alcohols with CO\n                    <jats:sub>2<\/jats:sub>\n                    under mild conditions, such as at room temperature and atmospheric pressure. Among the explored ILs, tetramethyl guanidinium 2,4\u2010dihydroxybenzoate ([TMGH]\n                    <jats:sub>3<\/jats:sub>\n                    [2,4\u2010DHBA]) was the most effective catalyst, achieving a conversion of 68.9% for the model substrate 2\u2010methyl\u20103\u2010butyn\u20102\u2010ol within 12 h. The superior performance of [TMGH]\n                    <jats:sub>3<\/jats:sub>\n                    [2,4\u2010DHBA] is attributed to the presence of multiple CO\n                    <jats:sub>2<\/jats:sub>\n                    \u2010philic sites on its anionic scaffold, which significantly enhances the cooperative activation of CO\n                    <jats:sub>2<\/jats:sub>\n                    . Furthermore, theoretical simulations revealed that the structural features of the anion play a decisive role in CO\n                    <jats:sub>2<\/jats:sub>\n                    adsorption and activation, exhibiting a positive correlation with the overall catalytic activity. This work systematically elucidates, from both experimental and theoretical perspectives, the catalytic mechanism of ILs with different cation\u2013anion combinations in CO\n                    <jats:sub>2<\/jats:sub>\n                    transformation reactions, providing critical insights for the rational design of highly efficient and mild catalytic systems for CO\n                    <jats:sub>2<\/jats:sub>\n                    utilization.\n                  <\/jats:p>","DOI":"10.1002\/chem.70963","type":"journal-article","created":{"date-parts":[[2026,4,8]],"date-time":"2026-04-08T06:26:43Z","timestamp":1775629603000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Design Principles and Mechanistic Insights for Ionic Liquid\u2010Catalyzed CO\n                    <sub>2<\/sub>\n                    Cyclization Under Mild 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