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However, the influence of electrode surface chemistry on NH4+ storage remains poorly understood. Two-dimensional Ti3C2Tx MXene, with metallic conductivity, tunable interlayer spacing, and abundant surface terminations, serves as an ideal platform to elucidate NH4+ storage mechanisms. Herein, the role of MXene surface termination in regulating NH4+ storage behavior is systematically investigated using density functional theory calculations and experimental validation. The calculations reveal that the \u2013N terminations offer moderate NH4+ adsorption and high electronic conductivity for rapid charge transfer and ion transport, whereas the \u2013O terminations exhibit stronger ion affinity and enhanced surface stability. Importantly, the mixed \u2013N\/\u2013O terminations effectively balance adsorption strength and transition-state stabilization, resulting in the lowest NH4+ migration barrier among the modeled pathways. The calculations employ idealized vacuum-separated surfaces with isolated NH4+ and do not explicitly include solvation or electrolyte effects. Guided by these findings, a mixed \u2013N\/\u2013O terminated Ti3C2Tx MXene is constructed via a urea-assisted hydrothermal strategy. The optimized NTC-20 electrode delivers 107 mAh g\u20131 at 1 A g\u20131, retains 67% capacity at 10 A g\u20131, and maintains 91% capacity after 10,000 cycles. Ex situ XRD, XPS, and FTIR analyses are consistent with reversible NH4+-associated changes in the local chemical environment and possible storage involving Ti\u2013N\u00b7\u00b7\u00b7H\u2013N and Ti\u2013O\u00b7\u00b7\u00b7H\u2013N interactions. Furthermore, the NTC-20\/\/MnO2\/CNTs full cell achieves an energy density of 26.7 Wh kg\u20131 at 1.3 kW kg\u20131. The results support a dominant role for mixed \u2013N\/\u2013O terminations in regulating NH4+ adsorption and diffusion, providing insights into surface-termination engineering for high-performance AAIBs.<\/jats:p>","DOI":"10.1021\/acsami.6c14469","type":"journal-article","created":{"date-parts":[[2026,10,12]],"date-time":"2026-10-12T21:01:52Z","timestamp":1791838912000},"page":"56169-56181","source":"Crossref","is-referenced-by-count":0,"title":["Mixed \u2013N\/\u2013O Surface Terminations Enable Fast Ammonium-Ion Storage in Ti3C2T\n                    <i>x<\/i>\n                    MXene"],"prefix":"10.1021","volume":"18","author":[{"given":"Xiang","family":"Liu","sequence":"first","affiliation":[{"name":"Southeast University , , ,","place":["Nanjing, P.R. China, 211189"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Mutian","family":"Zhang","sequence":"additional","affiliation":[{"name":"Southeast University , , ,","place":["Nanjing, P.R. China, 211189"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-2726-4236","authenticated-orcid":true,"given":"Wei","family":"Zheng","sequence":"additional","affiliation":[{"name":"Southeast University , , ,","place":["Nanjing, P.R. China, 211189"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Junjiang","family":"Fan","sequence":"additional","affiliation":[{"name":"Southeast University , , ,","place":["Nanjing, P.R. China, 211189"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Miaoxi","family":"Guo","sequence":"additional","affiliation":[{"name":"Southeast University , , ,","place":["Nanjing, P.R. China, 211189"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Li","family":"Yang","sequence":"additional","affiliation":[{"name":"Southeast University , , ,","place":["Nanjing, P.R. China, 211189"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-9798-9385","authenticated-orcid":true,"given":"ZhengMing","family":"Sun","sequence":"additional","affiliation":[{"name":"Southeast University , , ,","place":["Nanjing, P.R. China, 211189"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-1762-0540","authenticated-orcid":true,"given":"Guobing","family":"Ying","sequence":"additional","affiliation":[{"name":"Southeast University , , ,","place":["Nanjing, P.R. China, 211189"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,10,12]]},"reference":[{"issue":"14","key":"2026102609064364300_cit1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202115046","article-title":"The Emergence of Aqueous Ammonium-Ion Batteries","volume":"61","author":"Han","year":"2022","journal-title":"Angew. Chem., Int. 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