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Yet, how lattice element chemistry and surface termination groups collectively regulate the structure and mobility of such interlayer water remains poorly understood. Here, we present a composition-controlled investigation of interlayer water dynamics in layered transition-metal nitride, carbide, and carbonitride systems using a systematic integration of quasi-elastic neutron scattering (QENS), ab initio molecular dynamics (AIMD) simulations, and density functional theory (DFT) calculations. QENS measurements show that nitride-rich systems host mobile, translationally diffusing water with thermally activated self-diffusion coefficients on the order of 10\u201310 m2 s\u20131, whereas mixed C\/N lattices confine water to localized, nontranslational motion that is insensitive to temperature. AIMD and DFT reveal that lattice C\/N chemistry and surface functional group composition reshape the first hydration layer by modulating the surface electronic structure and termination-dependent hydrogen-bond networks, leading to pronounced differences in water ordering and thermal resilience. On the other hand, fully carbide systems exhibit intermediate behavior, highlighting that water mobility is not primarily controlled by the hydration level alone but by the coupling between lattice composition and surface chemistry. Overall, this study establishes how surface chemistry and lattice composition jointly control interfacial hydrogen bond dynamics, offering a mechanistic framework for designing transition-metal layered materials with tailored interfacial transport properties.<\/jats:p>","DOI":"10.1021\/acs.chemmater.6c01283","type":"journal-article","created":{"date-parts":[[2026,7,27]],"date-time":"2026-07-27T05:08:58Z","timestamp":1785128938000},"page":"7965-7981","source":"Crossref","is-referenced-by-count":0,"title":["Interfacial\nHydrogen-Bond Dynamics in Transition Metal\nCompounds"],"prefix":"10.1021","volume":"38","author":[{"given":"David Kumar","family":"Yesudoss","sequence":"first","affiliation":[{"name":"Texas A&M University , , , ,","place":["College Station, Texas, United States, 77843"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Hao-En","family":"Lai","sequence":"additional","affiliation":[{"name":"Texas A&M University , , , ,","place":["College Station, Texas, United States, 77843"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-0213-2299","authenticated-orcid":true,"given":"Naresh C.","family":"Osti","sequence":"additional","affiliation":[{"name":"Oak Ridge National Laboratory , , , ,","place":["Oak Ridge, Tennessee, United States, 37831"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Bright","family":"Ngozichukwu","sequence":"additional","affiliation":[{"name":"Texas A&M University , , , ,","place":["College Station, Texas, United States, 77843"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Joshua","family":"Ferguson","sequence":"additional","affiliation":[{"name":"Texas A&M University , , , ,","place":["College Station, Texas, United States, 77843"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-5684-2675","authenticated-orcid":true,"given":"Eugene","family":"Mamontov","sequence":"additional","affiliation":[{"name":"Oak Ridge National Laboratory , , , ,","place":["Oak Ridge, Tennessee, United States, 37831"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-2358-3910","authenticated-orcid":true,"given":"Perla B.","family":"Balbuena","sequence":"additional","affiliation":[{"name":"Texas A&M University , , , ,","place":["College Station, Texas, United States, 77843"]},{"name":"Texas A&M University , , , ,","place":["College Station, Texas, United States, 77843"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-0734-5952","authenticated-orcid":true,"given":"Abdoulaye","family":"Djire","sequence":"additional","affiliation":[{"name":"Texas A&M University , , , ,","place":["College Station, Texas, United States, 77843"]},{"name":"Texas A&M University , , , ,","place":["College Station, Texas, United States, 77843"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,7,25]]},"reference":[{"issue":"6298","key":"2026081109072924000_cit1","doi-asserted-by":"publisher","first-page":"aac9439","DOI":"10.1126\/science.aac9439","article-title":"2D materials\nand van der Waals heterostructures","volume":"353","author":"Novoselov","year":"2016","journal-title":"Science"},{"issue":"24","key":"2026081109072924000_cit2","doi-asserted-by":"publisher","first-page":"5042","DOI":"10.1021\/cm049820r","article-title":"Investigation\nof\nthe State of Water in Hydrating Layered Sodium Disilicate in Crystalline\nand Amorphous Forms by Quasi-Elastic Neutron Scattering","volume":"16","author":"Phair","year":"2004","journal-title":"Chem. Mater."},{"issue":"49","key":"2026081109072924000_cit3","doi-asserted-by":"publisher","first-page":"19360","DOI":"10.1021\/jacs.9b09343","article-title":"Coupled\nCation\u2013Anion Dynamics Enhances Cation Mobility in Room-Temperature\nSuperionic Solid-State Electrolytes","volume":"141","author":"Zhang","year":"2019","journal-title":"J. Am.\nChem. Soc."},{"issue":"42","key":"2026081109072924000_cit4","doi-asserted-by":"publisher","first-page":"28795","DOI":"10.1021\/jacs.4c08063","article-title":"Oxide Acidity Modulates Structural Transformations\nin Hydrogen Titanates during Electrochemical Li-Ion Insertion","volume":"146","author":"Saeed","year":"2024","journal-title":"J. Am. Chem. 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Phys."},{"issue":"15","key":"2026081109072924000_cit24","doi-asserted-by":"publisher","first-page":"5314","DOI":"10.1021\/acs.chemmater.5b01623","article-title":"Effect\nof postetch annealing gas composition on the structural and electrochemical\nproperties of Ti2CTx MXene electrodes for supercapacitor\napplications","volume":"27","author":"Rakhi","year":"2015","journal-title":"Chem. Mater."},{"issue":"3","key":"2026081109072924000_cit25","doi-asserted-by":"publisher","first-page":"276","DOI":"10.1007\/s11467-015-0493-x","article-title":"Recent advances\nin MXene: Preparation,\nproperties, and applications","volume":"10","author":"Lei","year":"2015","journal-title":"Frontiers of Physics"},{"key":"2026081109072924000_cit26","doi-asserted-by":"crossref","first-page":"15","DOI":"10.1201\/9781003306511-4","article-title":"Two-dimensional\nnanocrystals produced by exfoliation\nof Ti3AlC2","volume-title":"MXenes","author":"Naguib","year":"2023"},{"issue":"11","key":"2026081109072924000_cit27","doi-asserted-by":"publisher","first-page":"13765","DOI":"10.1021\/acsanm.4c02503","article-title":"Nanolayered\nTi4N3Tx MXene Retains Its Electrocatalytic\nProperties after Prolonged Immersion in Solvents","volume":"7","author":"Ngozichukwu","year":"2024","journal-title":"ACS Appl. Nano Mater."},{"issue":"6","key":"2026081109072924000_cit28","doi-asserted-by":"publisher","first-page":"100634","DOI":"10.1016\/j.checat.2023.100634","article-title":"Pt-like catalytic activity\nfrom an atomistically engineered carbonitride MXene for sustainable\nhydrogen production","volume":"3","author":"Uwadiunor","year":"2023","journal-title":"Chem Catal."},{"issue":"1","key":"2026081109072924000_cit29","doi-asserted-by":"publisher","first-page":"657","DOI":"10.1038\/s41598-021-04640-7","article-title":"Ti2N nitride MXene evokes\nthe Mars-van Krevelen mechanism\nto achieve high selectivity for nitrogen reduction reaction","volume":"12","author":"Johnson","year":"2022","journal-title":"Sci. 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Chem.,\nInt. 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Surf. Sci."},{"issue":"37","key":"2026081109072924000_cit44","doi-asserted-by":"publisher","first-page":"25165","DOI":"10.1039\/D4TA03457K","article-title":"The fabrication\nof Ti3C2 and Ti3CN MXenes by electrochemical\netching","volume":"12","author":"Chan","year":"2024","journal-title":"J. Mater. Chem. A"},{"issue":"4","key":"2026081109072924000_cit45","doi-asserted-by":"publisher","first-page":"1153","DOI":"10.1016\/j.susc.2006.12.010","article-title":"Oxidation of vanadium nitride and titanium nitride\ncoatings","volume":"601","author":"Glaser","year":"2007","journal-title":"Surf. Sci."},{"issue":"7\u20138","key":"2026081109072924000_cit46","doi-asserted-by":"publisher","first-page":"529","DOI":"10.1002\/sia.740230713","article-title":"Electrochemical\nand thermal oxidation of TiN coatings studied by XPS","volume":"23","author":"Milos\u030cv","year":"1995","journal-title":"Surf. Interface Anal."},{"issue":"1","key":"2026081109072924000_cit47","doi-asserted-by":"publisher","first-page":"4541","DOI":"10.1038\/s41598-017-04804-4","article-title":"Re-distribution\nof oxygen at the interface between \u03b3-Al2O3 and TiN","volume":"7","author":"Filatova","year":"2017","journal-title":"Sci. Rep."},{"issue":"14","key":"2026081109072924000_cit48","doi-asserted-by":"publisher","first-page":"8859","DOI":"10.1021\/acsami.6b01490","article-title":"Effect of metal ion\nintercalation on the structure\nof MXene and water dynamics on its internal surfaces","volume":"8","author":"Osti","year":"2016","journal-title":"ACS Appl. Mater. Interfaces"},{"issue":"11","key":"2026081109072924000_cit49","doi-asserted-by":"publisher","first-page":"1902207","DOI":"10.1002\/admi.201902207","article-title":"Multiscale and multimodal characterization\nof 2D titanium carbonitride MXene","volume":"7","author":"Sun","year":"2020","journal-title":"Adv. Mater.\nInterfaces"},{"issue":"52","key":"2026081109072924000_cit50","doi-asserted-by":"publisher","first-page":"58378","DOI":"10.1021\/acsami.0c17536","article-title":"Structure and dynamics of aqueous\nelectrolytes confined\nin 2D-TiO2\/Ti3C2Tx MXene\nheterostructures","volume":"12","author":"Ganeshan","year":"2020","journal-title":"ACS Appl. Mater. Interfaces"},{"issue":"11","key":"2026081109072924000_cit51","doi-asserted-by":"publisher","first-page":"11118","DOI":"10.1021\/acsnano.7b05264","article-title":"Multimodality\nof structural, electrical, and gravimetric\nresponses of intercalated MXenes to water","volume":"11","author":"Muckley","year":"2017","journal-title":"ACS\nNano"},{"issue":"38","key":"2026081109072924000_cit52","doi-asserted-by":"publisher","first-page":"9444","DOI":"10.1073\/pnas.1807821115","article-title":"Origin of the emergent fragile-to-strong\ntransition in supercooled water","volume":"115","author":"Shi","year":"2018","journal-title":"Proc. Natl.\nAcad. 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