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Herein, a hydroxyl\u2010rich Mg\n                    <jats:sub>0.55<\/jats:sub>\n                    Al layered double hydroxide (LDH) support is developed via aqueous miscible organic solvent treatment, circumventing energy\u2010intensive calcination while engineering mesopores for efficient polyethyleneimine (PEI) loading. The optimized 60\u00a0wt.% PEI modified Mg\n                    <jats:sub>0.55<\/jats:sub>\n                    Al\u2010CO\n                    <jats:sub>3<\/jats:sub>\n                    AMO\u2010LDH achieves a CO\n                    <jats:sub>2<\/jats:sub>\n                    uptake of 3.92\u00a0mmol g\n                    <jats:sup>\u22121<\/jats:sup>\n                    under simulated wet air at 25\u00a0\u00b0C and retains 90.8% capacity over 20 cycles. Crucially, the abundant surface hydroxyls of uncalcined LDH, validated by\n                    <jats:sup>1<\/jats:sup>\n                    H Nuclear Magnetic Resonance and in situ X\u2010ray Photoelectron Spectroscopy, form hydrogen bonds with PEI, suppressing oxidative degradation. After 3\u00a0h at 120\u00a0\u00b0C in simulated air, PEI\u2010LDH retains a CO\n                    <jats:sub>2<\/jats:sub>\n                    capacity of 1.06\u00a0mmol g\n                    <jats:sup>\u22121<\/jats:sup>\n                    , significantly outperforming PEI\/mixed metal oxide and conventional silica\u2010based adsorbents. In situ Diffuse Reflectance Infrared Fourier Transform Spectroscopy further reveals that hydroxyl\u2010mediated amine anchoring minimizes water co\u2010adsorption. This work establishes a dual strategy of hydroxyl preservation and mesopore engineering to design cost\u2010effective DAC adsorbents, achieving both high capacity and exceptional stability under realistic operating conditions.\n                  <\/jats:p>","DOI":"10.1002\/advs.202507756","type":"journal-article","created":{"date-parts":[[2025,6,30]],"date-time":"2025-06-30T23:50:36Z","timestamp":1751327436000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":10,"title":["Innovative Design of PEI\u2010Modified AMO\u2010Layered Double Hydroxide for Efficient and Stable Direct Air Capture of CO\n                    <sub>2<\/sub>"],"prefix":"10.1002","volume":"12","author":[{"given":"Meng","family":"Zhao","sequence":"first","affiliation":[{"name":"College of Environmental Science and Engineering Beijing Forestry University  Beijing 100083 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Liang","family":"Huang","sequence":"additional","affiliation":[{"name":"College of Environmental Science and Engineering Beijing Forestry University  Beijing 100083 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yanshan","family":"Gao","sequence":"additional","affiliation":[{"name":"College of Environmental Science and Engineering Beijing Forestry University  Beijing 100083 China"},{"name":"State Key Laboratory of Efficient Production of Forest Resources Beijing Forestry University  Beijing 100083 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Ziling","family":"Wang","sequence":"additional","affiliation":[{"name":"College of Environmental Science and Engineering Beijing Forestry University  Beijing 100083 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xuancan","family":"Zhu","sequence":"additional","affiliation":[{"name":"Research Center of Solar Power &amp; Refrigeration Institute of Refrigeration and Cryogenics Shanghai Jiao Tong University  Shanghai 200240 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-2719-2762","authenticated-orcid":false,"given":"Qiang","family":"Wang","sequence":"additional","affiliation":[{"name":"College of Environmental Science and Engineering Beijing Forestry University  Beijing 100083 China"},{"name":"State Key Laboratory of Efficient Production of Forest Resources Beijing Forestry University  Beijing 100083 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Dermot","family":"O'Hare","sequence":"additional","affiliation":[{"name":"Chemistry Research Laboratory Department of Chemistry University of Oxford  Mansfield Road Oxford OX1 3TA UK"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"311","published-online":{"date-parts":[[2025,6,30]]},"reference":[{"key":"e_1_2_7_1_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41586-019-1541-4"},{"key":"e_1_2_7_2_1","doi-asserted-by":"publisher","DOI":"10.1039\/D0CS00025F"},{"key":"e_1_2_7_3_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41467-024-53961-4"},{"key":"e_1_2_7_3_2","doi-asserted-by":"publisher","DOI":"10.1038\/s41560-025-01714-y"},{"key":"e_1_2_7_4_1","doi-asserted-by":"publisher","DOI":"10.1039\/D1CS00970B"},{"key":"e_1_2_7_5_1","doi-asserted-by":"publisher","DOI":"10.1007\/s42114-022-00567-3"},{"key":"e_1_2_7_6_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.201906756"},{"key":"e_1_2_7_7_1","doi-asserted-by":"publisher","DOI":"10.1021\/acs.est.0c07973"},{"key":"e_1_2_7_8_1","doi-asserted-by":"publisher","DOI":"10.1002\/adfm.202415211"},{"key":"e_1_2_7_8_2","doi-asserted-by":"publisher","DOI":"10.1002\/advs.202207253"},{"key":"e_1_2_7_8_3","doi-asserted-by":"publisher","DOI":"10.1016\/j.matt.2023.10.019"},{"key":"e_1_2_7_9_1","doi-asserted-by":"publisher","DOI":"10.1021\/acs.est.4c08500"},{"key":"e_1_2_7_9_2","doi-asserted-by":"publisher","DOI":"10.1038\/s41467-024-48994-8"},{"key":"e_1_2_7_9_3","author":"Sun M.","year":"2025","journal-title":"Environ. 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