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As classical descriptions of aqueous ion transport break down under extreme confinement, experimental studies often face challenges in controlling both nanoconfined structure and surface chemistry, limiting our ability to explain and predict water and ion behavior in subnanometer channels and membranes. Here, we show that 2D Ti3C2Tx MXene nanosheets with precisely controlled interlayer spacing (0.9\u20135.0 \u00c5), surface terminations, and electrode potentials provide a platform to systematically tune ion transport. Combined experimental measurements, including ion permeation, spatial secondary-ion mass spectrometry, and Fourier transform infrared spectroscopy, together with molecular dynamics simulations, reveal that ultranarrow confinement reorganizes confined water, imposes ion-specific energetic penalties for dehydration, and modulates ion\u2013MXene interactions. Li+ permeation in horizontally aligned Ti3C2Tx channels is 2 orders of magnitude faster than in conventional vertically aligned MXene membranes, while electrochemical surface charge modulation further regulates ion selectivity. These coupled effects of confinement, surface chemistry, and water-mediated energetics define a transport regime beyond classical diffusion, offering design principles for artificial ion channels and high-performance membranes for ion separation, water desalination, and sustainable water treatment technologies.<\/jats:p>","DOI":"10.1021\/jacs.6c07978","type":"journal-article","created":{"date-parts":[[2026,7,2]],"date-time":"2026-07-02T03:23:58Z","timestamp":1782962638000},"page":"31253-31262","source":"Crossref","is-referenced-by-count":0,"title":["Water-Mediated Ion\nSelectivity in 2D MXene Channels"],"prefix":"10.1021","volume":"148","author":[{"ORCID":"https:\/\/orcid.org\/0000-0002-4083-0928","authenticated-orcid":true,"given":"Yuan","family":"Zhang","sequence":"first","affiliation":[{"name":"Drexel University , , , ,","place":["Philadelphia, Pennsylvania, United States, 19104"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Ming","family":"Chen","sequence":"additional","affiliation":[{"name":"Imperial College London , , White City Campus, Wood Lane , ,","place":["London, U.K., W12 0BZ"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-4939-0594","authenticated-orcid":true,"given":"Teng","family":"Zhang","sequence":"additional","affiliation":[{"name":"Drexel University , , , ,","place":["Philadelphia, Pennsylvania, United States, 19104"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Tetiana","family":"Parker","sequence":"additional","affiliation":[{"name":"Drexel University , , , ,","place":["Philadelphia, Pennsylvania, United States, 19104"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Danzhen","family":"Zhang","sequence":"additional","affiliation":[{"name":"Drexel University , , , ,","place":["Philadelphia, Pennsylvania, United States, 19104"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-8095-5285","authenticated-orcid":true,"given":"Ruocun","family":"Wang","sequence":"additional","affiliation":[{"name":"Drexel University , , , ,","place":["Philadelphia, Pennsylvania, United States, 19104"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-2381-9716","authenticated-orcid":true,"given":"Hyunho","family":"Kim","sequence":"additional","affiliation":[{"name":"Drexel University , , , ,","place":["Philadelphia, Pennsylvania, United States, 19104"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-3299-4092","authenticated-orcid":true,"given":"Pawe\u0142 Piotr","family":"Micha\u0142owski","sequence":"additional","affiliation":[{"name":"Institute of Microelectronics and Photonics , , ,","place":["Warsaw, Poland, 01-919"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-3157-8791","authenticated-orcid":true,"given":"Alexei","family":"Kornyshev","sequence":"additional","affiliation":[{"name":"Imperial College London , , White City Campus, Wood Lane , ,","place":["London, U.K., W12 0BZ"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-9423-4032","authenticated-orcid":true,"given":"Yury","family":"Gogotsi","sequence":"additional","affiliation":[{"name":"Drexel University , , , ,","place":["Philadelphia, Pennsylvania, United States, 19104"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,7,1]]},"reference":[{"key":"2026073109205693700_cit1","doi-asserted-by":"publisher","first-page":"459","DOI":"10.1038\/nnano.2015.37","article-title":"Water desalination using\nnanoporous single-layer graphene","volume":"10","author":"Surwade","year":"2015","journal-title":"Nat. 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Energy Mater."},{"key":"2026073109205693700_cit10","doi-asserted-by":"publisher","first-page":"1760","DOI":"10.1126\/science.1132195","article-title":"Anomalous Increase in\nCarbon Capacitance at Pore Sizes Less Than 1 Nanometer","volume":"313","author":"Chmiola","year":"2006","journal-title":"Science"},{"key":"2026073109205693700_cit11","doi-asserted-by":"publisher","first-page":"752","DOI":"10.1126\/science.1245711","article-title":"Precise and Ultrafast\nMolecular Sieving Through Graphene Oxide Membranes","volume":"343","author":"Joshi","year":"2014","journal-title":"Science"},{"key":"2026073109205693700_cit12","doi-asserted-by":"publisher","first-page":"387","DOI":"10.1038\/nmat3916","article-title":"Accelerating charging dynamics in\nsubnanometre pores","volume":"13","author":"Kondrat","year":"2014","journal-title":"Nat. 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Lett."},{"key":"2026073109205693700_cit33","doi-asserted-by":"publisher","first-page":"1339","DOI":"10.1126\/science.aat4191","article-title":"Anomalously\nlow dielectric\nconstant of confined water","volume":"360","author":"Fumagalli","year":"2018","journal-title":"Science"},{"key":"2026073109205693700_cit34","doi-asserted-by":"publisher","first-page":"606","DOI":"10.1038\/s41586-025-09558-y","article-title":"In-plane dielectric\nconstant and conductivity of confined water","volume":"646","author":"Wang","year":"2025","journal-title":"Nature"},{"key":"2026073109205693700_cit35","doi-asserted-by":"publisher","DOI":"10.1126\/science.abf1581","article-title":"The world of two-dimensional carbides\nand nitrides (MXenes)","volume":"372","author":"VahidMohammadi","year":"2021","journal-title":"Science"},{"key":"2026073109205693700_cit36","doi-asserted-by":"publisher","DOI":"10.1126\/sciadv.ado3998","article-title":"Comediation\nof voltage\ngating and ion charge in MXene membrane for controllable and selective\nmonovalent cation separation","volume":"10","author":"Wang","year":"2024","journal-title":"Sci. Adv."},{"key":"2026073109205693700_cit37","doi-asserted-by":"publisher","first-page":"1701","DOI":"10.1002\/smll.201102056","article-title":"The importance\nof dehydration\nin determining ion transport in narrow pores","volume":"8","author":"Richards","year":"2012","journal-title":"Small"},{"key":"2026073109205693700_cit38","doi-asserted-by":"publisher","first-page":"4719","DOI":"10.1021\/acs.nanolett.7b01399","article-title":"Dehydration as a Universal Mechanism\nfor Ion Selectivity in Graphene and Other Atomically Thin Pores","volume":"17","author":"Sahu","year":"2017","journal-title":"Nano Lett."},{"key":"2026073109205693700_cit39","doi-asserted-by":"publisher","DOI":"10.1016\/j.memsci.2021.119752","article-title":"The effect\nof D-spacing\non the ion selectivity performance of MXene membrane","volume":"639","author":"Arshadi","year":"2021","journal-title":"J. Membr. 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Sci."},{"key":"2026073109205693700_cit49","doi-asserted-by":"publisher","first-page":"2995","DOI":"10.1039\/FT9918702995","article-title":"Thermodynamics\nof solvation of ions. Part 5.\u2500Gibbs free energy of hydration\nat 298.15 K","volume":"87","author":"Marcus","year":"1991","journal-title":"J. Chem. Soc., Faraday Trans."},{"key":"2026073109205693700_cit50","doi-asserted-by":"publisher","first-page":"1381","DOI":"10.1021\/j150579a011","article-title":"Phenomenological\nTheory of Ion Solvation. Effective Radii of Hydrated Ions","volume":"63","author":"Nightingale","year":"1959","journal-title":"J. Phys. Chem. A"},{"key":"2026073109205693700_cit51","doi-asserted-by":"publisher","first-page":"75","DOI":"10.1007\/s10867-011-9243-7","article-title":"The relation between the structure of the first solvation shell and\nthe IR spectra of aqueous solutions","volume":"38","author":"Kumar","year":"2012","journal-title":"J. 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