MXene异质结Ti-O-H-O电子快速通道促进高效率储钾

doi:10.15541/jim20240130

无机材料学报 ›› 2024, Vol. 39 ›› Issue (11): 1212-1220.DOI: 10.15541/jim20240130 CSTR: 32189.14.10.15541/jim20240130

所属专题：【能源环境】超级电容器,锂金属电池,钠离子电池和水系电池(202409)；【能源环境】超级电容器(202409)

MXene异质结Ti-O-H-O电子快速通道促进高效率储钾

晁少飞¹(), 薛艳辉¹, 吴琼¹(), 伍复发¹, MUHAMMAD Sufyan Javed², 张伟³

1.辽宁工业大学材料科学与工程学院, 锦州 121001
2.兰州大学物理科学与技术学院, 兰州 730000
3.吉林大学材料科学与工程学院, 汽车材料教育部重点实验室, 吉林省高效清洁能源材料国际合作重点实验室, 电子显微镜中心, 未来科学国际合作联合实验室, 长春 130012

收稿日期:2024-03-19 修回日期:2024-06-18 出版日期:2024-11-20 网络出版日期:2024-07-15
通讯作者: 吴琼, 教授. E-mail: wuqiong9918@126.com
作者简介:晁少飞(2000-), 男, 硕士研究生. E-mail: mxenemax@126.com
基金资助:
国家自然科学基金(51971106);辽宁省“揭榜挂帅”科技攻关项目(2023JH1/10400055);辽宁省自然科学基金计划(2024-MS-076);辽宁省教育厅基础科学研究项目(LJKMZ20220961);国家级大学生创新创业训练项目(202310154013)

Efficient Potassium Storage through Ti-O-H-O Electron Fast Track of MXene Heterojunction

CHAO Shaofei¹(), XUE Yanhui¹, WU Qiong¹(), WU Fufa¹, MUHAMMAD Sufyan Javed², ZHANG Wei³

1. School of Materials Science and Engineering, Liaoning University of Technology, Jinzhou 121001, China
2. School of Physical Science and Technology, Lanzhou University, Lanzhou 730000, China
3. Key Laboratory of Automobile Materials MOE, Jilin Provincial International Cooperation, Key Laboratory of High-Efficiency Clean Energy Materials, Electron Microscopy Center, International Center of Future Science, School of Materials Science & Engineering, Jilin University, Changchun 130012, China

Received:2024-03-19 Revised:2024-06-18 Published:2024-11-20 Online:2024-07-15
Contact: WU Qiong, professor. E-mail: wuqiong9918@126.com
About author:CHAO Shaofei (2000-), male, Master candidate. E-mail: mxenemax@126.com
Supported by:
National Natural Science Foundation of China(51971106);“Open Bidding for Selecting the Best Candidates” Science and Technology Project of Liaoning Province(2023JH1/10400055);Natural Science Foundation of Liaoning Province(2024-MS-076);Basic Scientific Research Project of Higher Education Department of Liaoning Province(LJKMZ20220961);National College Students Innovation and Entrepreneurship Training Program(202310154013)

摘要/Abstract

摘要：

二维层状结构MXenes因其优异的电学性能、可调控的表面官能团而被广泛应用于钾离子超级电容器领域, 但其有限的双电容存储容量严重限制了MXenes在电极材料方面的应用。本工作采用“路易斯酸熔盐预刻蚀+液相刻蚀+原位水热复合”策略, 制备了以Ti₃C₂为基体、表面包覆MnO₂的Ti₃C₂基异质结, 以提高电极材料对钾离子的储存。采用基于密度泛函理论的第一性原理计算方法, 研究了Ti₃C₂基异质结界面之间的连接方式、电学性质以及钾离子吸附规律的变化。结果表明构建的Ti₃C₂基异质结对钾离子的最大吸附量是Ti₃C₂的3倍左右, 且Ti-O-H-O连接通道使MnO₂内部的自由电子数量增多, 使Ti₃C₂基异质结表现出优异的电学性能。三电极体系下的电化学测试结果表明Ti₃C₂基异质结在1 A·g^-1的电流密度下能够提供431 F·g^-1的比电容, 远远高于Ti₃C₂(128 F·g^-1)。并通过动力学分析阐述了Ti₃C₂基异质结的赝电容储能机理, 在100 mV·s^-1的扫描速率下, 其赝电容贡献比例高达89%, 此外Ti₃C₂基异质结表现出较小的电化学阻抗, 从而提高了钾离子传输速率、电子转移速率。本研究通过构筑Ti₃C₂基异质结, 提高了基体Ti₃C₂的电化学性能, 并阐述了相应的储能机理, 这为设计其他MXenes基电极材料提供了理论基础。

关键词: Ti₃C₂基异质结, 离子吸附, 动力学分析, 钾离子存储, 超级电容器

Abstract:

MXenes with two-dimensional layered structure are widely used in the field of potassium ion supercapacitors because of their excellent electrical properties and adjustable surface functional groups, but their limited dual-capacitor storage capacity severely retards the application of MXenes materials in electrode materials. In this work, the strategy of “Lewis acid molten salt pre-etching + liquid phase etching + in situ hydrothermal recombination” was used to prepare the Ti₃C₂-based heterojunction with Ti₃C₂ as matrix and MnO₂ coated surface to improve the storage of potassium ions in electrode materials. The connection mode, electrical properties and the change of potassium adsorption law at Ti₃C₂-based heterojunction interfaces were studied by using the first principles calculation method based on density functional theory. The results show that the maximum adsorption capacity of potassium ions in the constructed Ti₃C₂-based heterojunction is about 3 times that of Ti₃C₂. The presence of Ti-O-H-O connecting channel increases the number of free electrons in MnO₂, causing Ti₃C₂-based heterojunction exhibiting excellent electrical properties. The electrochemical test results of the three-electrode system show that, at a current density of 1 A·g^-1, Ti₃C₂-based heterojunction can provide 431 F·g^-1 specific capacitance which is much higher than 128 F·g^-1 of bare Ti₃C₂. At a voltage sweep rate of 100 mV·s^-1, the contribution of pseudocapacitance is up to 89%. In addition, the Ti₃C₂-based heterojunction exhibits lower electrochemical impedance, which improves the potassium ion transport rate and electron transfer rate. Therefore, this study demonstrates that the electrochemical performance of Ti₃C₂ matrix can be improved by constructing Ti₃C₂-based heterojunction, and the corresponding energy storage mechanism can provide a theoretical basis for the design of other MXenes-based electrode materials.

Key words: Ti₃C₂-based heterojunction, ion adsorption, kinetic analysis, potassium-ion storage, supercapacitor

中图分类号:

TQ174

晁少飞, 薛艳辉, 吴琼, 伍复发, MUHAMMAD Sufyan Javed, 张伟. MXene异质结Ti-O-H-O电子快速通道促进高效率储钾[J]. 无机材料学报, 2024, 39(11): 1212-1220.

CHAO Shaofei, XUE Yanhui, WU Qiong, WU Fufa, MUHAMMAD Sufyan Javed, ZHANG Wei. Efficient Potassium Storage through Ti-O-H-O Electron Fast Track of MXene Heterojunction[J]. Journal of Inorganic Materials, 2024, 39(11): 1212-1220.

图/表 7

图1 Ti3C2基异质结的结构与形貌表征

Fig. 1 Structure and morphology characterization of Ti3C2-based heterojunction (a-c) SEM images of (a) Ti3Al-ZnC2, (b) Ti3C2 and (c) Ti3C2-based heterojunction; (d-f) XRD patterns of Ti3Al-ZnC2, Ti3C2 and Ti3C2-based heterojunction; (g) Atomic structure diagram of preparation of Ti3C2 Colorful figures are available on website

图2 Ti3C2基异质结之间的结合规律

Fig. 2 Binding rules between Ti3C2-based heterojunction Colorful figures are available on website

图3 Ti3C2基异质结的电化学储钾性能测试

Fig. 3 Electrochemical potassium storage performance tests of Ti3C2-based heterojunction (a) CV curves of Ti3C2 and Ti3C2-based heterojunction in a three-electrode system at a scan rate of 100 mV·s-1; (b) GCD curves of Ti3C2 and Ti3C2-based heterojunction at a current density of 1 A·g-1; (c) GCD curves of Ti3C2-based heterojunction at different current densities; (d) CV curves and (e) GCD curves of Ti3C2-based heterojunction in a double electrode system; (f) Ragone plot of energy density and power density[37⇓⇓⇓⇓⇓⇓-44]; (g, h) Schematic diagrams of two hybrid supercapacitors; (i) Practical application of Ti3C2-based heterojunction hybrid supercapacitors Colorful figures are available on website

图4 Ti3C2基异质结的动力学分析及储能机理

Fig. 4 Dynamic analysis and energy storage mechanism of Ti3C2-based heterojunction (a) CV curves of Ti3C2-based heterojunction at different scanning rates; (b) Relationship between the peak current and the scanning rate at a specific potential; (c) Pseudocapacitance ratio diagram of Ti3C2-based heterojunction at 100 mV·s-1; (d) Pseudocapacitance ratio of Ti3C2-based heterojunction at different scanning rates; (e) EIS plots of Ti3C2-based heterojunction and MnO2; (f) Magnified plots of a region in (e) with inset showing corresponding equivalent circuit; (g) Schematic diagram of mechanism of pseudocapacitance changed with Mn valence Colorful figures are available on website

图5 Ti3C2基异质结和Ti3C2对钾离子的吸附规律

Fig. 5 Adsorption rule of potassium ion on Ti3C2-based heterojunction and bare Ti3C2 Colorful figures are available on website

图6 Ti3C2基异质结的电子能带结构与态密度图

Fig. 6 Electron band structure and state density diagrams of Ti3C2-based heterojunction (a, b) Band structure diagrams of MnO2; (c) DOS diagram of MnO2; (d) PDOS diagrams of Mn and O atoms in MnO2; (e, f) PDOS diagrams of the distribution of electron orbitals of Mn and O atoms in valence and conduction bands; (g) PDOS diagram of each atom in Ti3C2-based heterojunction; (h) PDOS diagrams of Mn and O atoms in valence band of Ti3C2-based heterojunction; (i) PDOS diagrams of Mn and O atoms in conduction band of Ti3C2-based heterojunction with inset showing the band structure diagram of Ti3C2-based heterojunction Colorful figures are available on website

图7 Ti3C2基异质结的差分电荷密度图

Fig. 7 Differential charge density diagrams of Ti3C2-based heterojunction (a-c) 3D top views of differential charge density diagrams of three heterojunctions; (d-f) 3D differential charge density and 2D differential charge density section diagrams of (d) Ti(I), (e) Ti(Ⅱ) and (f) Ti(Ⅲ) connected heterojunction with MnO2 Colorful figures are available on website

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MXene异质结Ti-O-H-O电子快速通道促进高效率储钾

Efficient Potassium Storage through Ti-O-H-O Electron Fast Track of MXene Heterojunction

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