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Herein, a facile and controllable strategy, which combines heat treatment with phosphorous (P) doping by using sodium phosphinate (NaH2PO2) as a phosphorus source, is used to modify Ti3C2Tx. The intercalated ions from NaH2PO2 act as \u201cpillars\u201d to expand the interlayer space of MXene, which is conducive to electrolyte ion diffusion. On the other hand, P doping tailors the surface electronic state of MXene, optimizing electronic conductivity and reducing the free energy of H+ diffusion on the MXene surface. Meanwhile, P sites with lower electronegativity owning good electron donor characteristics are easy to share electrons with H+, which is beneficial to charge storage. Moreover, the adopted heat treatment replaces \u2013F terminations with O-containing groups, which enhances the hydrophilicity and provides sufficient active sites. The change in surface functional groups increases the content of high valence-stated Ti with a high electrochemical activity that can accommodate more electrons during discharge. Synergistic modification of interlayer structure and chemical state improves the possibility of Ti3C2Tx for accommodating more H+ ions. Consequently, the modified electrode delivers a specific capacitance of 510 F g\u22121 at 2 mV s\u22121, and a capacitance retention of 90.2% at 20 A g\u22121 after 10,000 cycles. The work provides a coordinated strategy for the rational design of high-capacitance Ti3C2Tx MXene electrodes.<\/jats:p>","DOI":"10.3390\/molecules28134892","type":"journal-article","created":{"date-parts":[[2023,6,22]],"date-time":"2023-06-22T02:09:17Z","timestamp":1687399757000},"page":"4892","update-policy":"https:\/\/doi.org\/10.3390\/mdpi_crossmark_policy","source":"Crossref","is-referenced-by-count":20,"title":["Phosphorus Doping Strategy-Induced Synergistic Modification of Interlayer Structure and Chemical State in Ti3C2Tx toward Enhancing Capacitance"],"prefix":"10.3390","volume":"28","author":[{"given":"Lihong","family":"Chen","sequence":"first","affiliation":[{"name":"School of Materials Science and Engineering, Qingdao University of Science and Technology, Qingdao 266042, China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yifan","family":"Bi","sequence":"additional","affiliation":[{"name":"School of Materials Science and Engineering, Qingdao University of Science and Technology, Qingdao 266042, China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yunqi","family":"Jing","sequence":"additional","affiliation":[{"name":"College of Environment and Safety Engineering, Qingdao University of Science and Technology, Qingdao 266042, China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jun","family":"Dai","sequence":"additional","affiliation":[{"name":"College of Electromechanical Engineering, Qingdao University of Science and Technology, Qingdao 266061, China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zhenjiang","family":"Li","sequence":"additional","affiliation":[{"name":"School of Materials Science and Engineering, Qingdao University of Science and Technology, Qingdao 266042, China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Changlong","family":"Sun","sequence":"additional","affiliation":[{"name":"School of Materials Science and Engineering, Qingdao University of Science and Technology, Qingdao 266042, China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Alan","family":"Meng","sequence":"additional","affiliation":[{"name":"State Key Laboratory Base of Eco-Chemical Engineering, College of Chemistry and Molecular Engineering, Qingdao University of Science and Technology, Qingdao 266042, China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Haijiao","family":"Xie","sequence":"additional","affiliation":[{"name":"Hangzhou Yanqu Information Technology Co., Ltd., Hangzhou 310003, China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Minmin","family":"Hu","sequence":"additional","affiliation":[{"name":"School of Materials Science and Engineering, Qingdao University of Science and Technology, Qingdao 266042, China"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"1968","published-online":{"date-parts":[[2023,6,21]]},"reference":[{"key":"ref_1","doi-asserted-by":"crossref","first-page":"1901081","DOI":"10.1002\/aenm.201901081","article-title":"A new view of supercapacitors: Integrated supercapacitors","volume":"9","author":"Zhu","year":"2019","journal-title":"Adv. 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