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Electrosynthesis of DMC from CO\n                    <jats:sub>2<\/jats:sub>\n                    offers a sustainable alternative but faces challenges of inert CO\n                    <jats:sub>2<\/jats:sub>\n                    activation and unfavorable C\u2010O coupling, leading to low selectivity and current density. Herein, we propose a tandem electrocatalysis strategy for efficient DMC production from CO\n                    <jats:sub>2<\/jats:sub>\n                    under ambient conditions, utilizing a cobalt polyphthalocyanine framework (CoPPc) with single\u2010atom sites and atomically precise palladium\u2010sulfur clusters (Pd\n                    <jats:sub>6<\/jats:sub>\n                    S\n                    <jats:sub>12<\/jats:sub>\n                    ). The CoPPc\u2010Pd\n                    <jats:sub>6<\/jats:sub>\n                    S\n                    <jats:sub>12<\/jats:sub>\n                    tandem catalyst system synergistically activates CO\n                    <jats:sub>2<\/jats:sub>\n                    and enhances mass transport, elevating the local concentration of key intermediates (CO and methoxy species) for improving DMC production efficiency. Thus, the tandem system delivers exceptional performance with 93.4% DMC selectivity and 34.9\u00a0mmol L\n                    <jats:sup>\u22121<\/jats:sup>\n                    h\n                    <jats:sup>\u22121<\/jats:sup>\n                    production in 0.1\u00a0M NaBr methanol electrolyte, while achieving a recorded current density of 155.2\u00a0mA cm\n                    <jats:sup>\u22122<\/jats:sup>\n                    at 0.5\u00a0M electrolyte concentration. In situ generated CO and methoxy over CoPPc efficiently transfer to the Pd\u2010S site, where achieves intermediate stabilization and optimal coupling orientation, boosting DMC selectivity and current density. Moreover, DFT calculations reveal that the CoPPc\u2010Pd\n                    <jats:sub>6<\/jats:sub>\n                    S\n                    <jats:sub>12<\/jats:sub>\n                    system reduces the energy barrier for C\u2010O coupling, facilitating DMC formation. This work provides an efficient tandem electrocatalysis system for DMC production from CO\n                    <jats:sub>2<\/jats:sub>\n                    with high selectivity and large current density.\n                  <\/jats:p>","DOI":"10.1002\/anie.4855063","type":"journal-article","created":{"date-parts":[[2026,2,4]],"date-time":"2026-02-04T06:55:10Z","timestamp":1770188110000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":5,"title":["Highly Efficient Tandem Electrosynthesis of Dimethyl Carbonate From CO\n                    <sub>2<\/sub>"],"prefix":"10.1002","volume":"65","author":[{"given":"Hui","family":"Guo","sequence":"first","affiliation":[{"name":"State Key Laboratory of Structural Chemistry, Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences  Fuzhou Fujian P. R. China"},{"name":"University of Chinese Academy of Sciences  Beijing P. R. 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