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上海第二工业大学《Small》:多维MC@MXene碳纳米管复合材料,用于锂离子电池

2026-01-27

1成果简介 
        介孔碳材料是先进锂离子电池的有前景的阳极,但其性能仍受限于结构稳定性差和电化学界面不稳定。为克服这些问题,本文,上海第二工业大学汪玲玲 教授、 上海大学张海娇 研究员等在《Small》期刊发表名为“Multi-Dimensional Engineering Enables Interfacial and Mechanical Stability of Mesoporous Carbon Anode for Lithium-Ion Batteries”的论文,研究设计了一种多维集成架构:以介孔碳(MC)球体为核心,外层包裹二维Ti?C?T_x MXene纳米片,并在MXene表面原位生长一维碳纳米管(MC@MXene-CNTs)。
        在这种定制结构中,介孔碳芯为锂存储提供了短扩散距离,而MXene涂层增强了整个电极的柔韧性,并作为CNT生长的催化基底。垂直排列的碳纳米管形成互连导电网络,不仅优化电荷传输、防止MXene重堆叠,还实现了介孔碳颗粒间的桥接。通过精妙整合一维、二维与三维结构单元,该复合材料展现出卓越的锂存储性能,包括高可逆容量与优异倍率性能。通过原位电化学阻抗谱(EIS)、X射线光电子能谱(XPS)深度剖析及密度泛函理论(DFT)计算,系统探究了支撑这些性能提升的电化学机理。本研究为先进储能系统中高性能电极材料的理性设计提供了基础性认识。
        2图文导读




  
         图1、a) Schematic diagram of the synthesis process of MC@MXene-CNTs. b,c) SEM images, d,e) TEM images, f,g), HRTEM images, and h) STEM image and corresponding elemental distribution of MC@MXene-CNTs.





        图2、a) XRD patterns, b) Raman spectra, and c) FT-IR spectra of MC@MXene-CNTs, MC@MXene and MC. d) N2 adsorption-desorption isotherm and corresponding pore size distribution (inset) of MC@MXene-CNTs. e) XPS survey spectra of MC@MXene-CNTs, and high-resolution spectra of f) C 1s, g) Ti 2p, h) O 1s, and i) N 1s.





        图3. a) CV curves of the first three cycles at a scanning rate of 0.1 mV s?1, and b) GCD curves of the MC@MXene-CNTs electrode at 100 mA g?1. c) Cycling performance of MC@MXene-CNTs, MC@MXene and MC electrodes at 100 mA g?1 d) Cycling performance comparison between MC@MXene-CNTs electrode and other carbon-based electrodes (the details are listed in Table S3). e) Rate performance of MC@MXene-CNTs, MC@MXene and MC electrodes. f) Rate performance comparison between MC@MXene-CNTs electrode and other carbon-based electrodes. g) Cycling performance of the three electrodes at a high current density of 1000 mA g?1.





        图4、a) CV curves of the MC@MXene-CNTs electrode at different scanning rates, and b) b values plotted for the anode and cathode peaks. c) The contributions of capacitance behavior (blue area) and diffusion behavior (pink area) at 1.0 mV s?1. d) The normalized contribution ratios of capacitance behavior and diffusion behavior at different scanning rates. e) GITT voltage curves, and f) Li diffusion coefficients. g,h) DRT transformation patterns of the EIS spectrum of MC@MXene-CNTs. i) Surface contact angles of MC@MXene-CNTs, MC@MXene and MC electrodes at 0 and 4s.+





        图5、a,b) XPS deep etching spectra of C 1s, O 1s and F 1s for MC@MXene-CNTs and MC@MXene electrodes after cycling. c–e) The elemental contents of C, O and F at different etching times. f,g) Schematic illustration of the SEI composition distributions for MC@MXene-CNTs and MC@MXene electrodes.





        图6、SEM images of a–c) MC@MXene-CNTs, d-f) MC@MXene, and g–i) MC electrodes before and after cycling. j) Schematic diagram of the structural evolution of the three electrodes after cycling.





        图7、a) Adsorption energy of Li on carbon layer, C-Ti3C2(-X, X = F, O, OH) and C-Ti3C2(-X) CNT systems, respectively. b–e) Charge density difference and electron transfer between Li and substrates of C-Ti3C2, C-Ti3C2F2, C-Ti3C2O2 and C-Ti3C2(OH)2, respectively. Yellow and cyan areas exhibit the electron accumulation and depletion areas, respectively. f) Schematic diagram of the energy storage advantages of the MC@MXene-CNTs anode for lithium-ion batteries.
        3小结 
        综上所述,通过静电自组装与原位催化生长工艺,成功设计出兼具刚性与柔性的多维电极材料,该材料战略性地整合了内层介孔碳、中间二维MXene柔性层及外层坚固的一维碳纳米管。电化学动力学、蚀刻XPS分析及密度泛函理论计算均证实,该独特结构通过协同效应实现卓越性能:丰富的锂离子存储位点、优异的界面稳定性及高效离子传输通道共同赋能。所得MC@MXene-CNTs电极不仅展现出高比容量和卓越的倍率性能,循环耐久性也显著提升:在100 mA g?1电流密度下经150次循环后仍保持671.9 mAh g?1的高可逆容量。即使在1000 mA g?1的高电流密度下,经600次循环后可逆容量仍保持在593.6 mAh g?1。本研究为构建适用于先进储能领域的多维框架电极材料提供了宝贵启示。
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