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Direct air capture (DAC) has emerged as a promising approach to achieving a net-zero carbon future, which offers several practical advantages, such as independence from specific CO2 emission sources, economic feasibility, flexible deployment, and minimal risk of CO2 leakage. The design and optimization of DAC sorbents are crucial for accelerating industrial adoption. Metal\u2013organic frameworks (MOFs), with high structural order and tunable pore sizes, present an ideal solution for achieving strong guest\u2013host interactions under trace CO2 conditions. This perspective highlights recent advancements in using MOFs for DAC, examines the molecular-level effects of water vapor on trace CO2 capture, reviews data-driven computational screening methods to develop a molecularly programmable MOF platform for identifying optimal DAC sorbents, and discusses scale-up and cost of MOFs for DAC.<\/jats:p>","DOI":"10.1021\/jacs.4c12200","type":"journal-article","created":{"date-parts":[[2025,2,7]],"date-time":"2025-02-07T17:49:46Z","timestamp":1738950586000},"page":"5495-5514","source":"Crossref","is-referenced-by-count":105,"title":["Architecting Metal\u2013Organic\nFrameworks at Molecular\nLevel toward Direct Air Capture"],"prefix":"10.1021","volume":"147","author":[{"ORCID":"https:\/\/orcid.org\/0000-0001-6728-2952","authenticated-orcid":true,"given":"Zi-Ming","family":"Ye","sequence":"first","affiliation":[{"name":"Fujian Normal University , , , ,","place":["Fuzhou, Fujian, China, 350007"]},{"name":"Northwestern University , , , ,","place":["Evanston, Illinois, United States, 60208"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-7647-9666","authenticated-orcid":true,"given":"Yi","family":"Xie","sequence":"additional","affiliation":[{"name":"University of Texas at San Antonio , , , ,","place":["San Antonio, Texas, United States, 78249"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-8329-1015","authenticated-orcid":true,"given":"Kent O.","family":"Kirlikovali","sequence":"additional","affiliation":[{"name":"Northwestern University , , , ,","place":["Evanston, Illinois, United States, 60208"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-6016-2587","authenticated-orcid":true,"given":"Shengchang","family":"Xiang","sequence":"additional","affiliation":[{"name":"Fujian Normal University , , , ,","place":["Fuzhou, Fujian, China, 350007"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-9904-9845","authenticated-orcid":true,"given":"Omar K.","family":"Farha","sequence":"additional","affiliation":[{"name":"Northwestern University , , , ,","place":["Evanston, Illinois, United States, 60208"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-8707-8115","authenticated-orcid":true,"given":"Banglin","family":"Chen","sequence":"additional","affiliation":[{"name":"Fujian Normal University , , , ,","place":["Fuzhou, Fujian, China, 350007"]},{"name":"Zhejiang Normal University , , ,","place":["Jinhua, China, 321004"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2025,2,7]]},"reference":[{"key":"2026090713160671300_cit1","unstructured":"IEA.\n          .  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