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Although cobalt phthalocyanine (CoPc) is recognized as promising catalyst for this reaction, achieving high methanol selectivity at high current density remains a critical challenge, due to insufficient stabilization of *CO intermediate and sluggish hydrogenation kinetics. Here we report a molecular-ionic hybrid catalyst constructed by integrating amino-functionalized CoPc with imidazolium-based ionic liquid (IL) on carbon nanotubes (CoPc-NH2 + IL\/CNT). The hybrid catalyst achieves a methanol Faradaic efficiency of 75.0% with a partial current density of 300 mA cm\u20132. This outstanding performance originates from the cooperative interplay between CoPc-NH2 and imidazolium cations. The imidazolium serves as a CO2 adsorption reservoir that enriches and delivers CO2 to Co centers for activation, while simultaneously inducing a more electron-deficient Co center that stabilizes diverse *CO adsorption states for deep hydrogenation. In parallel, imidazolium cations reorganize interfacial hydrogen-bond networks, accelerate water dissociation and proton supply, and facilitate charge transfer to reaction intermediates through an electronic relay effect. These synergistic effects suppress the competing CO pathway and selectively steer CO2 electroreduction toward methanol at high current densities. The effectiveness of this molecular-ionic coupling is further validated across a range of imidazolium cations, demonstrating the generality of this microenvironment-engineering strategy.<\/jats:p>","DOI":"10.1021\/jacs.6c11699","type":"journal-article","created":{"date-parts":[[2026,8,20]],"date-time":"2026-08-20T17:02:02Z","timestamp":1787245322000},"page":"37193-37202","source":"Crossref","is-referenced-by-count":0,"title":["Molecular-Ionic Hybrid\nModulates Intermediate Evolution\nfrom CO2 to Methanol at High Current Density"],"prefix":"10.1021","volume":"148","author":[{"ORCID":"https:\/\/orcid.org\/0000-0002-5255-6268","authenticated-orcid":true,"given":"Pengsong","family":"Li","sequence":"first","affiliation":[{"name":"Chinese Academy of Sciences , , ,","place":["Beijing, China, 100190"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xiang-Da","family":"Zhang","sequence":"additional","affiliation":[{"name":"Chinese Academy of Sciences , , ,","place":["Beijing, China, 100190"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yuqing","family":"Hou","sequence":"additional","affiliation":[{"name":"Chinese Academy of Sciences , , ,","place":["Beijing, China, 100190"]},{"name":"University of the Chinese Academy of Sciences , , ,","place":["Beijing, P. R. China, 100049"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yong","family":"Wang","sequence":"additional","affiliation":[{"name":"Chinese Academy of Sciences , , ,","place":["Beijing, China, 100190"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Ganwen","family":"Zhang","sequence":"additional","affiliation":[{"name":"Chinese Academy of Sciences , , ,","place":["Beijing, China, 100190"]},{"name":"University of the Chinese Academy of Sciences , , ,","place":["Beijing, P. R. China, 100049"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Changlong","family":"Zhu","sequence":"additional","affiliation":[{"name":"Chinese Academy of Sciences , , ,","place":["Beijing, China, 100190"]},{"name":"University of the Chinese Academy of Sciences , , ,","place":["Beijing, P. R. China, 100049"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-0593-0840","authenticated-orcid":true,"given":"Xinchen","family":"Kang","sequence":"additional","affiliation":[{"name":"Chinese Academy of Sciences , , ,","place":["Beijing, China, 100190"]},{"name":"University of the Chinese Academy of Sciences , , ,","place":["Beijing, P. R. China, 100049"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Peng","family":"Liu","sequence":"additional","affiliation":[{"name":"China Huaneng Clean Energy Research Institute , Changping District, ,","place":["Beijing, China, 102209"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xiaolong","family":"Wang","sequence":"additional","affiliation":[{"name":"China Huaneng Clean Energy Research Institute , Changping District, ,","place":["Beijing, China, 102209"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-8730-8486","authenticated-orcid":true,"given":"Qinggong","family":"Zhu","sequence":"additional","affiliation":[{"name":"Chinese Academy of Sciences , , ,","place":["Beijing, China, 100190"]},{"name":"University of the Chinese Academy of Sciences , , ,","place":["Beijing, P. R. China, 100049"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-0440-809X","authenticated-orcid":true,"given":"Buxing","family":"Han","sequence":"additional","affiliation":[{"name":"Chinese Academy of Sciences , , ,","place":["Beijing, China, 100190"]},{"name":"University of the Chinese Academy of Sciences , , ,","place":["Beijing, P. R. China, 100049"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,8,20]]},"reference":[{"issue":"9","key":"2026090312082869700_cit1","doi-asserted-by":"publisher","first-page":"732","DOI":"10.1038\/s41560-019-0450-y","article-title":"Advances and challenges in understanding\nthe electrocatalytic conversion of carbon dioxide to fuels","volume":"4","author":"Birdja","year":"2019","journal-title":"Nat. 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Ed."},{"issue":"18","key":"2026090312082869700_cit5","doi-asserted-by":"publisher","first-page":"2636","DOI":"10.1002\/anie.200462121","article-title":"Beyond\noil and gas: the methanol economy","volume":"44","author":"Olah","year":"2005","journal-title":"Angew. Chem.,\nInt. Ed."},{"issue":"1","key":"2026090312082869700_cit6","doi-asserted-by":"publisher","first-page":"7768","DOI":"10.1038\/s41467-022-35450-8","article-title":"Selective CO2 electroreduction to methanol via enhanced\noxygen bonding","volume":"13","author":"Zhang","year":"2022","journal-title":"Nat. Commun."},{"issue":"8","key":"2026090312082869700_cit7","doi-asserted-by":"publisher","first-page":"564","DOI":"10.1038\/s41570-021-00289-y","article-title":"Highlights and challenges in the\nselective reduction\nof carbon dioxide to methanol","volume":"5","author":"Navarro-Jae\u0301n","year":"2021","journal-title":"Nat. Rev. Chem."},{"issue":"8","key":"2026090312082869700_cit8","doi-asserted-by":"publisher","first-page":"2400129","DOI":"10.1002\/smsc.202400129","article-title":"Electrocatalytic\nCO2 reduction to alcohols: progress and perspectives","volume":"4","author":"Long","year":"2024","journal-title":"Small Sci."},{"issue":"7784","key":"2026090312082869700_cit9","doi-asserted-by":"publisher","first-page":"639","DOI":"10.1038\/s41586-019-1760-8","article-title":"Domino electroreduction\nof CO2 to methanol on a molecular catalyst","volume":"575","author":"Wu","year":"2019","journal-title":"Nature"},{"issue":"32","key":"2026090312082869700_cit10","doi-asserted-by":"publisher","first-page":"12717","DOI":"10.1021\/jacs.9b04907","article-title":"Scalable production\nof efficient single-atom copper\ndecorated carbon membranes for CO2 electroreduction to\nmethanol","volume":"141","author":"Yang","year":"2019","journal-title":"J. Am. Chem. 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Soc."},{"issue":"16","key":"2026090312082869700_cit17","doi-asserted-by":"publisher","first-page":"3149","DOI":"10.1021\/acs.accounts.1c00200","article-title":"Heterogeneous molecular catalysts\nof metal phthalocyanines for electrochemical CO2 reduction\nreactions","volume":"54","author":"Wu","year":"2021","journal-title":"Acc. Chem. Res."},{"issue":"10","key":"2026090312082869700_cit18","doi-asserted-by":"publisher","first-page":"4957","DOI":"10.1021\/acsenergylett.5c02397","article-title":"Molecular catalyst enables CO2 electroreduction\nat 650 mA\/cm2 CO partial current\ndensity","volume":"10","author":"Liu","year":"2025","journal-title":"ACS Energy Lett."},{"issue":"1","key":"2026090312082869700_cit19","doi-asserted-by":"publisher","first-page":"3602","DOI":"10.1038\/s41467-019-11542-w","article-title":"CO2 electrochemical\ncatalytic reduction with a highly active cobalt phthalocyanine","volume":"10","author":"Wang","year":"2019","journal-title":"Nat. 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Soc."},{"issue":"1","key":"2026090312082869700_cit22","doi-asserted-by":"publisher","first-page":"78","DOI":"10.1038\/s41565-025-02059-z","article-title":"Efficient CO2-to-methanol\nelectrocatalysis in acidic media via microenvironment-tuned cobalt\nphthalocyanine","volume":"21","author":"Song","year":"2026","journal-title":"Nat. Nanotechnol."},{"issue":"45","key":"2026090312082869700_cit23","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202517033","article-title":"Strengthening\nintermediate adsorption\non a cobalt phthalocyanine assembly by polymeric modification for\nelectrochemical carbon dioxide reduction into methanol","volume":"64","author":"Win","year":"2025","journal-title":"Angew. Chem., Int. Ed."},{"issue":"21","key":"2026090312082869700_cit24","doi-asserted-by":"publisher","first-page":"2502644","DOI":"10.1002\/adma.202502644","article-title":"Modulating\nactive center microenvironment in phthalocyanine-based covalent organic\nframeworks for enhanced electrocatalytic CO2 to CH3OH","volume":"37","author":"Wang","year":"2025","journal-title":"Adv. Mater."},{"issue":"1","key":"2026090312082869700_cit25","doi-asserted-by":"publisher","first-page":"7359","DOI":"10.1038\/s41467-025-62656-3","article-title":"Nanoconfinement promotes\nCO2 electroreduction to methanol on a molecular catalyst","volume":"16","author":"Shi","year":"2025","journal-title":"Nat. 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Rev."},{"issue":"13","key":"2026090312082869700_cit28","doi-asserted-by":"publisher","first-page":"6057","DOI":"10.1021\/acs.chemrev.4c00696","article-title":"Ionic liquids\npromoted transformation of carbon dioxide","volume":"125","author":"Wang","year":"2025","journal-title":"Chem.\nRev."},{"issue":"1","key":"2026090312082869700_cit29","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202417562","article-title":"Fundamentals and challenges of ligand\nmodification in heterogeneous electrocatalysis","volume":"64","author":"Kong","year":"2025","journal-title":"Angew. Chem., Int. Ed."},{"issue":"21","key":"2026090312082869700_cit30","doi-asserted-by":"publisher","first-page":"9849","DOI":"10.1039\/D5CS00554J","article-title":"Organic interface enhanced\nelectrocatalysis","volume":"54","author":"Hong","year":"2025","journal-title":"Chem. Soc. 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Ed."},{"issue":"17","key":"2026090312082869700_cit36","doi-asserted-by":"publisher","DOI":"10.1002\/cssc.202300418","article-title":"Trace ionic\nliquid-assisted orientational growth of Cu2O (110) facets\npromote CO2 electroreduction to C2 products","volume":"16","author":"Wang","year":"2023","journal-title":"ChemSusChem"},{"issue":"1","key":"2026090312082869700_cit37","doi-asserted-by":"publisher","first-page":"74","DOI":"10.1038\/s44160-025-00892-7","article-title":"Imidazolium\nradical-mediated electron transfer enhances electrochemical C\u2013N\ncoupling for glycine synthesis","volume":"5","author":"Wang","year":"2026","journal-title":"Nat. Synth."},{"issue":"3","key":"2026090312082869700_cit38","doi-asserted-by":"publisher","first-page":"1701694","DOI":"10.1002\/aenm.201701694","article-title":"Single-Crystalline\nUltrathin Co3O4 Nanosheets with Massive Vacancy\nDefects for Enhanced Electrocatalysis","volume":"8","author":"Cai","year":"2018","journal-title":"Adv.\nEnergy Mater."},{"issue":"12","key":"2026090312082869700_cit39","doi-asserted-by":"publisher","first-page":"1727","DOI":"10.1007\/s11426-020-9847-9","article-title":"Electron-withdrawing functional ligand promotes CO2 reduction catalysis\nin single atom catalyst","volume":"63","author":"Ren","year":"2020","journal-title":"Sci. China:Chem."},{"issue":"31","key":"2026090312082869700_cit40","doi-asserted-by":"publisher","first-page":"27278","DOI":"10.1021\/jacs.5c01314","article-title":"Chemostructurally\nstable polyionomer coatings regulate proton-intermediate landscape\nin acidic CO2 electrolysis","volume":"147","author":"Polesso","year":"2025","journal-title":"J. Am.\nChem. Soc."},{"issue":"17","key":"2026090312082869700_cit41","doi-asserted-by":"publisher","first-page":"2310037","DOI":"10.1002\/adma.202310037","article-title":"Ultrathin, cationic\ncovalent organic nanosheets for enhanced CO2 electroreduction\nto methanol","volume":"36","author":"Song","year":"2024","journal-title":"Adv. Mater."},{"issue":"11","key":"2026090312082869700_cit42","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202400206","article-title":"H* Species\nregulation by Mn-Co(OH)2 for efficient nitrate electro-reduction\nin neutral solution","volume":"63","author":"Liang","year":"2024","journal-title":"Angew. Chem., Int. Ed."},{"issue":"42","key":"2026090312082869700_cit43","doi-asserted-by":"publisher","first-page":"2204089","DOI":"10.1002\/adma.202204089","article-title":"Heterogeneous-interface-enhanced\nadsorption of organic and hydroxyl for biomass electrooxidation","volume":"34","author":"Zhou","year":"2022","journal-title":"Adv. Mater."},{"issue":"1","key":"2026090312082869700_cit44","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202413334","article-title":"Unveiling\nthe structure and dissociation\nof interfacial water on RuO2 for efficient acidic oxygen\nevolution reaction","volume":"64","author":"Wu","year":"2025","journal-title":"Angew. Chem., Int. Ed."},{"issue":"14","key":"2026090312082869700_cit45","doi-asserted-by":"publisher","first-page":"10904","DOI":"10.1021\/acscatal.4c01670","article-title":"Cu-Induced interfacial water engineering\nof SnO2 for durable and highly selective CO2 electroreduction","volume":"14","author":"Tian","year":"2024","journal-title":"ACS Catal."},{"issue":"1","key":"2026090312082869700_cit46","doi-asserted-by":"publisher","first-page":"3743","DOI":"10.1038\/s41467-025-59025-5","article-title":"Metal-organic double layer to stabilize selective multi-carbon electrosynthesis","volume":"16","author":"Cheng","year":"2025","journal-title":"Nat. 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Catal."},{"issue":"44","key":"2026090312082869700_cit49","doi-asserted-by":"publisher","DOI":"10.1002\/smll.202506545","article-title":"Atomistic\nand Oxophilic Ce Raises the Inertia of CO Intermediates Toward Enhanced\nElectrocatalytic Methanation","volume":"21","author":"Zheng","year":"2025","journal-title":"Small"}],"container-title":["Journal of the American\nChemical Society"],"original-title":[],"language":"en","link":[{"URL":"https:\/\/pubs.acs.org\/doi\/pdf\/10.1021\/jacs.6c11699","content-type":"application\/pdf","content-version":"vor","intended-application":"unspecified"},{"URL":"https:\/\/pubs.acs.org\/jacsat\/article-pdf\/148\/34\/37193\/66913127\/jacs.6c11699.pdf","content-type":"application\/pdf","content-version":"vor","intended-application":"syndication"},{"URL":"https:\/\/pubs.acs.org\/jacsat\/article-pdf\/148\/34\/37193\/66913127\/jacs.6c11699.pdf","content-type":"unspecified","content-version":"vor","intended-application":"similarity-checking"}],"deposited":{"date-parts":[[2026,9,3]],"date-time":"2026-09-03T16:20:10Z","timestamp":1788452410000},"score":1,"resource":{"primary":{"URL":"https:\/\/pubs.acs.org\/jacsat\/article\/148\/34\/37193\/5278502\/Molecular-Ionic-Hybrid-Modulates-Intermediate"}},"subtitle":[],"short-title":[],"issued":{"date-parts":[[2026,8,20]]},"references-count":49,"journal-issue":{"issue":"34","published-online":{"date-parts":[[2026,8,20]]},"published-print":{"date-parts":[[2026,9,2]]}},"URL":"https:\/\/doi.org\/10.1021\/jacs.6c11699","relation":{},"ISSN":["0002-7863","1520-5126"],"issn-type":[{"value":"0002-7863","type":"print"},{"value":"1520-5126","type":"electronic"}],"subject":[],"published":{"date-parts":[[2026,8,20]]}}}