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Here, we report a membrane\u2010free LEGO\u2010like granular\u2010electrode CDI (GCDI) system, in which ultrahigh mass loading is achieved by assembling carbon granular electrodes (GE) rather than continuously thickening monolithic electrodes. This design avoids the conventional trade\u2010off between increased loading and impaired ion transport caused by longer transport distances and inaccessible internal active sites. Under forced convection, GCDI induces an ion\u2010entrainment effect that renews ions in both inter\u2010GE and intra\u2010GE domains. Hydrodynamic and electrochemical kinetic analyses confirm effective ion transport throughout the electrode volume. Consequently, GCDI reaches an ultrahigh mass loading of \u223c274\u00a0mg cm\n                    <jats:sup>\u22122<\/jats:sup>\n                    and an areal ion flux of 0.59 \u00b5mol\n                    <jats:sub>NaCl<\/jats:sub>\n                    cm\n                    <jats:sup>\u22122<\/jats:sup>\n                    min\n                    <jats:sup>\u22121<\/jats:sup>\n                    , outperforming most flow\u2010by and flow\u2010through CDI systems. Even at a high areal flux of 7338 L h\n                    <jats:sup>\u22121<\/jats:sup>\n                    m\n                    <jats:sup>\u22122<\/jats:sup>\n                    , it maintains an areal ion\u2010capture capacity of 16.74 \u00b5mol\n                    <jats:sub>NaCl<\/jats:sub>\n                    cm\n                    <jats:sup>\u22122<\/jats:sup>\n                    . GCDI operates for over 500 cycles with \u223c60% capacity retention. Cost analysis and carbon footprint estimates further indicate reduced electrode, membrane, and electricity\u2010related burdens for membrane\u2010free GCDI. These results establish membrane\u2010free GCDI as a scalable structural strategy for improving CDI system efficiency in practical saline and complex water treatment.\n                  <\/jats:p>","DOI":"10.1002\/anie.9170775","type":"journal-article","created":{"date-parts":[[2026,8,25]],"date-time":"2026-08-25T04:02:07Z","timestamp":1787630527000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["LEGO\u2010Like Granular\u2010Electrode Capacitive Deionization with Ultrahigh Mass Loading for Ultrafast Electrochemical Ion Capture"],"prefix":"10.1002","author":[{"ORCID":"https:\/\/orcid.org\/0009-0001-2230-9813","authenticated-orcid":false,"given":"Xiaochen","family":"Zhang","sequence":"first","affiliation":[{"name":"Research Center for Environmental Functional Materials State Key Laboratory of Water Pollution Control and Green Resource Recycling College of Environmental Science and Engineering Tongji University  Shanghai People's Republic of China"},{"name":"National Museum of China  Beijing People's Republic of China"},{"name":"Key Scientific Research Base of Metal Conservation (National Museum of China) National Cultural Heritage Administration  Beijing People's Republic of China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zixiao","family":"Xu","sequence":"additional","affiliation":[{"name":"Research Center for Environmental Functional Materials State Key Laboratory of Water Pollution Control and Green Resource Recycling College of Environmental Science and Engineering Tongji University  Shanghai People's Republic of China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Fei","family":"Yu","sequence":"additional","affiliation":[{"name":"College of Oceanography and Ecological Science Shanghai Ocean University  Shanghai People's Republic of China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Ye","family":"Zhao","sequence":"additional","affiliation":[{"name":"National Energy Group Zhejiang Beilun First Power Generation Co., Ltd.  Ningbo People's Republic of China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Mingkuan","family":"Zhang","sequence":"additional","affiliation":[{"name":"Xi'an TPRI Water\u2010Management &amp; Environmental Protection Co., Ltd.  Xi'an People's Republic of China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-4494-1844","authenticated-orcid":false,"given":"Jie","family":"Ma","sequence":"additional","affiliation":[{"name":"Research Center for Environmental Functional Materials State Key Laboratory of Water Pollution Control and Green Resource Recycling College of Environmental Science and Engineering Tongji University  Shanghai People's Republic of China"},{"name":"National Museum of China  Beijing People's Republic of China"},{"name":"Key Scientific Research Base of Metal Conservation (National Museum of China) National Cultural Heritage Administration  Beijing People's Republic of China"},{"name":"Water Resources and Water Environment Engineering Technology Center Xinjiang Key Laboratory of Synthesis and Application of Carbon Nanomaterials School of Civil Engineering Kashi University  Kashi People's Republic of 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