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Here we present a covalently supported interlayer engineering strategy that transforms layered molybdenum sulfide (MoS\n                    <jats:sub>2<\/jats:sub>\n                    ) into a high\u2010performance electrode with exceptional capacity and stability. By precisely intercalating butane\u20101,4\u2010diol, we replace weak van der Waals interactions with rigid covalent linkages, simultaneously expanding interlayer spacing and inducing local 2H\u2010to\u20101T lattice reconstruction. This dual structural reprogramming fundamentally reconfigures Mo\u2010S orbital hybridization, generating high\u2010energy antibonding states that promote strong Na\n                    <jats:sup>+<\/jats:sup>\n                    chemisorption while preventing framework collapse. Consequently, the engineered electrode delivers an ultrahigh salt removal capacity of 77.4\u00a0mg g\n                    <jats:sup>\u22121<\/jats:sup>\n                    , over threefold higher than pristine MoS\n                    <jats:sub>2<\/jats:sub>\n                    , without measurable decay over 50 cycles, and demonstrates scalable brine treatment outperforming state\u2010of\u2010the\u2010art 2D electrodes. This work establishes a generalized paradigm for covalently reinforced 2D frameworks, resolving the long\u2010standing performance\u2010stability paradox in CDI and advancing practical, high\u2010capacity desalination.\n                  <\/jats:p>","DOI":"10.1002\/anie.202525780","type":"journal-article","created":{"date-parts":[[2026,2,21]],"date-time":"2026-02-21T09:12:05Z","timestamp":1771665125000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":1,"title":["Interlayer Covalent Reinforcement\u2010Enabled Lattice Reprogramming for Durable Capacitive Deionization"],"prefix":"10.1002","volume":"65","author":[{"given":"Zewei","family":"Hao","sequence":"first","affiliation":[{"name":"State Key Laboratory of Water Pollution Control and Green Resource Recycling College of Environmental Science and Engineering Tongji University  Shanghai China"},{"name":"Yellow River Laboratory of Shanxi Province College of Environmental and Resource Science Shanxi University  Taiyuan China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-4790-5873","authenticated-orcid":false,"given":"Jiabin","family":"Chen","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Water Pollution Control and Green Resource Recycling College of Environmental Science and Engineering Tongji University  Shanghai China"},{"name":"Key Laboratory of Urban Water Supply, College of Environmental Science and Engineering Water Saving and Water Environment Governance in the Yangtze River Delta of Ministry of Water Resources Tongji University  Shanghai China"},{"name":"Shanghai Institute of Pollution Control and Ecological Security Tongji University  Shanghai China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Qipeng","family":"Zhao","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Water Pollution Control and Green Resource Recycling College of Environmental Science and Engineering Tongji University  Shanghai China"},{"name":"Shanghai Institute of Pollution Control and Ecological Security Tongji University  Shanghai China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xiaoqian","family":"Liu","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Water Pollution Control and Green Resource Recycling College of Environmental Science and Engineering Tongji University  Shanghai China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Mingchao","family":"Yang","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Water Pollution Control and Green Resource Recycling College of Environmental Science and Engineering Tongji University  Shanghai China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xuefei","family":"Zhou","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Water Pollution Control and Green Resource Recycling College 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