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By integrating nuclear magnetic resonance (NMR) experiments with molecular dynamics (MD) simulations, the differential behaviors of these two EOR agents at the pore scale were elucidated. NMR T2 spectroscopy reveals that CO2 huff-and-puff achieved superior cumulative recovery rates (37.30%) compared to surfactants (24.01%), primarily due to its miscibility with crude oil and efficient mobilization of mesopores (53.1% \u00b1 3.7% contribution). Conversely, surfactants exhibited higher efficacy in micropores (47.8% \u00b1 4.3% contribution), attributed to multiple synergistic mechanisms, including interfacial slip induced by near-zero interactions with rock surfaces, wettability alteration, and solubilization of adsorbed oil films. MD simulations further confirmed that CO2 exhibits a stronger affinity for saturated hydrocarbons, while surfactants preferentially interact with polar components (nonanoic acid, nonanone) via Coulomb-dominated hydrogen bonding and hydration, enhancing light oil extraction. The results from experimental observations and molecular-level insights underscore the distinct advantages of CO2 and surfactants in huff-and-puff processes, providing a theoretical foundation for designing composite methods to optimize recovery efficiency. This research bridges macroscopic performance discrepancies with nanoscale mechanisms, advancing the understanding of carbon dioxide utilization in carbon capture, utilization, and storage (CCUS) frameworks.<\/jats:p>","DOI":"10.1021\/acsomega.6c06479","type":"journal-article","created":{"date-parts":[[2026,8,20]],"date-time":"2026-08-20T15:03:05Z","timestamp":1787238185000},"page":"51881-51892","source":"Crossref","is-referenced-by-count":1,"title":["Pore-Scale and\nMolecular Insights into Surfactant\nand CO2 Huff-and-Puff for Enhanced Oil Recovery in Shale\nReservoirs"],"prefix":"10.1021","volume":"11","author":[{"ORCID":"https:\/\/orcid.org\/0009-0009-0505-7835","authenticated-orcid":true,"given":"Pengzhi","family":"Wei","sequence":"first","affiliation":[{"name":"China University of Petroleum Beijing at Karamay , , ,","place":["Xinjiang, China, 834000"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Hongxian","family":"Liu","sequence":"additional","affiliation":[{"name":"China University of Petroleum Beijing at Karamay , , ,","place":["Xinjiang, China, 834000"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Shixun","family":"Bai","sequence":"additional","affiliation":[{"name":"China University of Petroleum Beijing at Karamay , , ,","place":["Xinjiang, China, 834000"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Dunqing","family":"Liu","sequence":"additional","affiliation":[{"name":"China University of Petroleum Beijing at Karamay , , ,","place":["Xinjiang, China, 834000"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jie","family":"Dong","sequence":"additional","affiliation":[{"name":"China University of Petroleum Beijing at Karamay , , ,","place":["Xinjiang, China, 834000"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,8,20]]},"reference":[{"key":"2026090307193063500_cit1","volume-title":"Global Energy Review","author":"International Energy Agency.","year":"2026"},{"key":"2026090307193063500_cit2","doi-asserted-by":"publisher","first-page":"2196","DOI":"10.1016\/S0140-6736(19)30303-4","article-title":"Health and Climate Change","volume":"393","author":"Florin","year":"2019","journal-title":"Lancet"},{"key":"2026090307193063500_cit3","doi-asserted-by":"publisher","DOI":"10.1002\/wcc.830","article-title":"Collective\nResponsibility for Climate Change","volume":"14","author":"Hormio","year":"2023","journal-title":"WIREs Clim.\nChange"},{"key":"2026090307193063500_cit4","doi-asserted-by":"publisher","DOI":"10.1016\/j.eiar.2021.106679","article-title":"Structural Path and Sensitivity Analysis of the CO2 Emissions in the Construction Industry","volume":"92","author":"Chen","year":"2022","journal-title":"Environ. 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