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Unfortunately, achieving efficient multi\u2010carbon products (C\n                    <jats:sub>2+<\/jats:sub>\n                    ) production in acidic media remains challenging due to two main limitations: weak CO adsorption on Cu sites and competitive H* adsorption caused by the high concentration protons (H\n                    <jats:sup>+<\/jats:sup>\n                    ). To overcome these challenges, a cation\u2010anion\u2010modification strategy is proposed using an ionic liquid layer\u20141\u2010Propyl\u20103\u2010methylimidazolium bis(trifluoromethylsulfonyl)imide ([PMIM][NTf\n                    <jats:sub>2<\/jats:sub>\n                    ])\u2014on Cu surface. Density functional theory calculations predict that PMIM\n                    <jats:sup>+<\/jats:sup>\n                    cation strengthens *CO adsorption through quasi\u2010hydrogen bonding, while NTf\n                    <jats:sub>2<\/jats:sub>\n                    <jats:sup>\u2212<\/jats:sup>\n                    anion creates a hydrophobic environment, effectively reducing H* coverage and promoting *CO adsorption. Resistance tests demonstrate that [PMIM][NTf\n                    <jats:sub>2<\/jats:sub>\n                    ] modification effectively reduced proton diffusion. Attenuated total reflection infrared spectroscopy (ATR\u2010IR) confirmed the reinforcement of *CO adsorption on the modified Cu surface. As a result, the [PMIM][NTf\n                    <jats:sub>2<\/jats:sub>\n                    ] modified Cu catalyst achieved a remarkable partial current density of \u2248640 mA cm\n                    <jats:sup>\u22122<\/jats:sup>\n                    for C\n                    <jats:sub>2+<\/jats:sub>\n                    products, with exceptional faradaic efficiency of 80.1% and durability of \u224820 h at a partial current density exceeding 500 mA cm\n                    <jats:sup>\u22122<\/jats:sup>\n                    in a flow cell. This study highlights the potential of cation\u2010anion modification strategies for significantly enhancing CO\n                    <jats:sub>2<\/jats:sub>\n                    RR in acidic media.\n                  <\/jats:p>","DOI":"10.1002\/smll.202412293","type":"journal-article","created":{"date-parts":[[2025,3,11]],"date-time":"2025-03-11T16:56:59Z","timestamp":1741712219000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":13,"title":["Enhanced Acidic CO\n                    <sub>2<\/sub>\n                    \u2010to\u2010C\n                    <sub>2+<\/sub>\n                    Reduction via Ionic Liquid Layer Modification"],"prefix":"10.1002","volume":"21","author":[{"given":"Qiyou","family":"Wang","sequence":"first","affiliation":[{"name":"Hunan Joint International Research Center for Carbon Dioxide Resource Utilization State Key Laboratory of Powder Metallurgy School of Physics Central South University  Changsha 410083 P. 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China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Hongmei","family":"Li","sequence":"additional","affiliation":[{"name":"Hunan Joint International Research Center for Carbon Dioxide Resource Utilization State Key Laboratory of Powder Metallurgy School of Physics Central South University  Changsha 410083 P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Cheng\u2010Wei","family":"Kao","sequence":"additional","affiliation":[{"name":"National Synchrotron Radiation Research Center  Hsinchu 300092 Taiwan"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Ting\u2010Shan","family":"Chan","sequence":"additional","affiliation":[{"name":"National Synchrotron Radiation Research Center  Hsinchu 300092 Taiwan"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Haiqing","family":"Zhou","sequence":"additional","affiliation":[{"name":"Department of Physics and Synergetic Innovation Center for Quantum Effects and Applications Hunan Normal University  Changsha 410081 P. R. 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