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Here, we resolve this long-standing limitation by establishing a hydrogen-pumping-inspired direct-current methodology with electronic blocking layers, enabling unambiguous decoupling of ionic and electronic transport in metallic solids. Ti3C2Tx membranes exhibit intrinsic proton conductivity of 9 \u00d7 10\u20134 S cm\u20131 at 90 \u00b0C with a low activation energy of 0.26 eV, consistent with water-mediated hopping in confined nanochannels. The successful operation of fuel cells employing Ti3C2Tx membranes as solid electrolytes provides strong evidence of bulk proton conduction. This unusual coexistence originates from intrinsically decoupled transport pathways, in which delocalized electrons are confined to the conductive Ti3C2 layers, whereas protons are transported through hydrogen-bonded water networks in the interlayer galleries. Density functional theory (DFT) calculations further support this picture by showing that the metallic band structure of Ti3C2Tx is preserved across different surface terminations, consistent with the decoupled nature of proton and electron transport. Leveraging this coupled transport behavior, hydrogen separation is achieved at 80 \u00b0C through a mechanism fundamentally distinct from conventional molecular sieving. These findings redefine the functional classification of MXenes, establishing them as a new class of proton\/electron mixed-conducting layered solids.<\/jats:p>","DOI":"10.1021\/jacs.6c08714","type":"journal-article","created":{"date-parts":[[2026,8,4]],"date-time":"2026-08-04T13:15:37Z","timestamp":1785849337000},"page":"33474-33485","source":"Crossref","is-referenced-by-count":0,"title":["Intrinsic\nProton Conduction in Metallic Ti3C2T\n                    <i>x<\/i>\n                    MXene Membranes Revealed\nby Direct-Current Decoupling"],"prefix":"10.1021","volume":"148","author":[{"given":"Kaito","family":"Takegami","sequence":"first","affiliation":[{"name":"Kumamoto University , , 2-39-1 Kurokami , Chuo-Ku, ,","place":["Kumamoto, Japan, 860-8555"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-3369-3371","authenticated-orcid":true,"given":"Kazuto","family":"Hatakeyama","sequence":"additional","affiliation":[{"name":"Kumamoto University , , 2-39-1 Kurokami , Chuo-Ku, ,","place":["Kumamoto, Japan, 860-8555"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Tatsuki","family":"Tsugawa","sequence":"additional","affiliation":[{"name":"Kumamoto University , , 2-39-1 Kurokami , Chuo-Ku, ,","place":["Kumamoto, Japan, 860-8555"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Satsuki","family":"Tomatsu","sequence":"additional","affiliation":[{"name":"Kumamoto University , , 2-39-1 Kurokami , Chuo-Ku, ,","place":["Kumamoto, Japan, 860-8555"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Asahi","family":"Yuji","sequence":"additional","affiliation":[{"name":"Kumamoto University , , 2-39-1 Kurokami , Chuo-Ku, ,","place":["Kumamoto, Japan, 860-8555"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0009-0001-5327-3753","authenticated-orcid":true,"given":"Yuichi","family":"Sakuda","sequence":"additional","affiliation":[{"name":"Kumamoto University , , 2-39-1 Kurokami , Chuo-Ku, ,","place":["Kumamoto, Japan, 860-8555"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-0032-1897","authenticated-orcid":true,"given":"Shintaro","family":"Ida","sequence":"additional","affiliation":[{"name":"Kumamoto University , , 2-39-1 Kurokami , Chuo-Ku, ,","place":["Kumamoto, Japan, 860-8555"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,7,29]]},"reference":[{"key":"2026081210093433000_cit1","doi-asserted-by":"publisher","DOI":"10.1002\/celc.202300846","article-title":"Proton-Conducting\nPolymers: Key to Next-Generation Fuel Cells, Electrolyzers, Batteries,\nActuators, and Sensors","volume":"11","author":"Nagao","year":"2024","journal-title":"ChemElectrochem"},{"issue":"16","key":"2026081210093433000_cit2","doi-asserted-by":"publisher","first-page":"8416","DOI":"10.1021\/acs.chemrev.9b00842","article-title":"Proton Transport in\nMetal-Organic Frameworks","volume":"120","author":"Lim","year":"2020","journal-title":"Chem. 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