表面端基卤化Ti3C2 MXene应用于锂离子电池高容量电极材料的研究

doi:10.15541/jim20210550

无机材料学报 ›› 2022, Vol. 37 ›› Issue (6): 660-668.DOI: 10.15541/jim20210550

所属专题：【虚拟专辑】计算材料；【信息功能】Max层状材料、MXene及其他二维材料

表面端基卤化Ti₃C₂ MXene应用于锂离子电池高容量电极材料的研究

肖美霞¹(), 李苗苗¹, 宋二红²(), 宋海洋¹(), 李钊¹, 毕佳颖¹

1.西安石油大学材料科学与工程学院, 西安 710065
2.中国科学院上海硅酸盐研究所高性能陶瓷和超微结构国家重点实验室, 上海 200050

收稿日期:2021-08-29 修回日期:2021-10-24 出版日期:2022-06-20 网络出版日期:2021-12-16
通讯作者: 宋二红, 副研究员. E-mail: ehsong@mail.sic.ac.cn;
宋海洋, 教授. E-mail: ygsfshy@sohu.com
作者简介:肖美霞(1982-), 女, 副教授. E-mail: mxxiao@xsyu.edu.cn
基金资助:
国家自然科学基金(51801155);陕西省科学基金(2021JZ-53);上海市自然科学基金(21ZR1472900);陕西省教育厅科研计划(21JK0848);西安石油大学研究生创新项目基金(YCS20211059);西安石油大学材料科学与工程学院西安市高性能油气田材料重点实验室项目

Halogenated Ti₃C₂ MXene as High Capacity Electrode Material for Li-ion Batteries

XIAO Meixia¹(), LI Miaomiao¹, SONG Erhong²(), SONG Haiyang¹(), LI Zhao¹, BI Jiaying¹

1. College of Materials Science and Engineering, Xi’an Shiyou University, Xi’an 710065, China
2. State Key Laboratory of High Performance Ceramics and Superfine Microstructure, Shanghai Institute of Ceramics, Chinese Academy of Sciences, Shanghai 200050, China

Received:2021-08-29 Revised:2021-10-24 Published:2022-06-20 Online:2021-12-16
Contact: SONG Erhong, associate professor. E-mail: ehsong@mail.sic.ac.cn;
SONG Haiyang, professor. E-mail: ygsfshy@sohu.com
About author:XIAO Meixia (1982–), female, associate professor. E-mail: mxxiao@xsyu.edu.cn
Supported by:
National Natural Science Foundation of China(51801155);Science Foundation of Shanxi Province,(2021JZ-53);Shanghai Natural Science Foundation(21ZR1472900);Scientific Research Program Funded by Shaanxi Provincial Education Department(21JK0848);Program for Graduate Innovation Fund of Xian Shiyou University(YCS20211059);Fund of Xi'an Key Laboratory of High Performance Oil and Gas Field Materials, School of Material Science and Engineering, Xi'an Shiyou University

摘要/Abstract

摘要：

Mxenes以其优异的比表面积、高导电率和组分可调性而受到广泛研究, 并用作高效锂离子电池的电极材料。然而, 其有限的存储容量以及锂离子扩散引起的剧烈晶格膨胀限制了MXenes作为电极材料的应用。本研究设计了具有代表性的MXene材料卤化(氟化、氯化或溴化)-Ti₃C₂。采用基于密度泛函理论的范德瓦耳斯修正的第一性原理计算方法研究了表面端基(T=F^-、Cl^-和Br^-)修饰对锂离子电池中Ti₃C₂负极的原子结构、电学性质、力学性质以及电化学性能的影响。研究表明, Ti₃C₂T₂单层具有良好的结构稳定性、力学性质和导电性质。相比Ti₃C₂F₂和Ti₃C₂Br₂, Ti₃C₂Cl₂单层具有较大的弹性模量(沿二维薄膜两个方向的弹性模量分别为321.70和329.43 N/m)、较低的锂离子扩散势垒(0.275 eV)、开路电压(0.54 V)和较大的理论存储容量(化学计量比为Ti₃C₂Cl₂Li₆时达674.21 mA·h/g), 这表明Ti₃C₂Cl₂单层作为锂电池电极具有良好的安全稳定性和充放电速率。此外, 端基氯化扩大了层间距, 进而提高了Ti₃C₂Cl₂中锂离子的可穿透性和快速充放电速率。本研究表明, 表面氯化的Ti₃C₂纳米薄膜是一种很有前途的锂电池负极材料, 为其它的MXenes基电极材料设计与开发提供了重要的设计思路。

关键词: MXenes, Ti₃C₂, 表面端基修饰, 第一性原理计算, 锂离子电池负极, 层间距

Abstract:

MXenes have been widely studied for their excellent specific surface area, high conductivity and composition tunability, which have been used as a highly efficient electrode material for lithium-ion batteries (LIBs). However, limited storage capacity and severe lattice expansion caused by Li-ions diffusion restrict the application of MXenes as electrode materials. Here, Ti₃C₂ MXenes with surface halogenation (fluorination, chlorination and bromination) as representative MXene materials were designed. Effects of surface functionalization on the atomic structures, electronic properties, mechanical properties, and electrochemical performance of Ti₃C₂T₂ (T = F, Cl and Br) anode in LIBs were investigated using first-principles calculations based on density functional theory with van der Waals correction. The results reveal that Ti₃C₂T₂ MXenes exhibit metallic conductivity with improved structural stability and mechanical strength. Compared with Ti₃C₂F₂ and Ti₃C₂Br₂, Ti₃C₂Cl₂ exhibits the large elastic modulus (321.70 and 329.43 N/m along x and y directions, respectively), low diffusion barrier (0.275 eV), high open circuit voltage (0.54 eV), and storage capacity (674.21 mA·h/g) with stoichiometric ratio of Ti₃C₂Cl₂Li₆, which renders the enhanced rate performance and endures the repeated lattice expansion and contraction during the charge/ discharge process. Moreover, surface chlorination yields expanded interlayer spacing, which can improve Li-ion accessibility and fast charge-discharge rate in Ti₃C₂Cl₂. The research demonstrates that Cl^- terminated Ti₃C₂ is a promising anode material, and provides effective and reversible routes to engineering other MXenes as anode materials for LIBs.

Key words: MXenes, Ti₃C₂, surface end group modification, first-principles calculation, Li-ion battery anode, interlayer spacing

中图分类号:

TM911

肖美霞, 李苗苗, 宋二红, 宋海洋, 李钊, 毕佳颖. 表面端基卤化Ti₃C₂ MXene应用于锂离子电池高容量电极材料的研究[J]. 无机材料学报, 2022, 37(6): 660-668.

XIAO Meixia, LI Miaomiao, SONG Erhong, SONG Haiyang, LI Zhao, BI Jiaying. Halogenated Ti₃C₂ MXene as High Capacity Electrode Material for Li-ion Batteries[J]. Journal of Inorganic Materials, 2022, 37(6): 660-668.

图/表 12

图1 M1、M2、M3和M4结构的Ti3C2T2原子构型的俯视图和主视图

Fig. 1 Top and side views of M1, M2, M3, and M4 Ti3C2T2 configurations Blue, black and nattier blue balls represent Ti, C and T atoms, respectively, where T denotes F, Cl or Br atoms Colorful views ave arailable on website

表1 四种构型的Ti3C2T2形成能Ef(eV)

Table 1 Formation energy Ef of (eV) Ti3C2T2 with four configurations

Ti₃C₂T₂	M1/eV	M2/eV	M3/eV	M4/eV
Ti₃C₂F₂	-4.23	-4.60	-4.94	-4.77
Ti₃C₂Cl₂	-2.44	-3.07	-3.33	-3.20
Ti₃C₂Br₂	-1.95	-2.57	-2.81	-2.69

表2 M3-Ti3C2T2的晶格常数a、键长lTi2-T和lTi2-C

Table 2 Lattice parameters a of M3-Ti3C2T2 and corresponding bond lengths of lTi2-T and lTi2-C

Ti₃C₂T₂	a /nm	l_Ti2-T/nm	l_Ti2-C/nm
Ti₃C₂F₂	0.308	0.217	0.208
Ti₃C₂Cl₂	0.319	0.251	0.211
Ti₃C₂Br₂	0.325	0.264	0.213

图2 M3-Ti3C2T2部分态密度(PDOS)和电荷密度差图

Fig. 2 Partial density of states (PDOS) and electron density difference of M3-Ti3C2T2 Blue, black and nattier blue balls represent Ti, C and T atoms, respectively, and red- and blue-colored regions indicate electron accumulation and depletion, respectively Colorful figures are available on website

图3 M3-Ti3C2T2中沿(a) x和(b) y方向的应变-应变能曲线及(c) x和y方向的弹性模量

Fig. 3 Strain energy to strain curves of M3-Ti3C2T2 along (a) x- and (b) y-direction, respectively, and (c) elasticmodulus values in x and y directions Blue, black and nattier blue balls represent Ti, C and T atoms, respectively Colorful figures are available on website

表3 当锂离子吸附在Ti3C2T2表面上形成稳定的M3-Ti3C2T2-Li时, 锂离子的吸附能(Eab)、电荷转移量(Δq)和吸附高度(Δh)

Table 3 Adsorption energy (Eab), charge transfer amount (Δq) and adsorption height (Δh), of Liion for stable M3-Ti3C2T2-Li with Liion adsorbed on Ti3C2T2 surface

Ti₃C₂T₂-Li	E_ab/eV	Δq/e	Δh/nm
M3-Ti₃C₂F₂-Li_T2	-1.21	0.61	0.021
M3-Ti₃C₂Cl₂-Li_T1	-0.72	0.40	0.026
M3-Ti₃C₂Br₂-Li_T1	-0.41	0.33	0.028

图4 (a) Ti3C2F2、(b) Ti3C2Cl2和(c) Ti3C2Br2上锂离子迁移路径示意图, 及锂离子在(d) Ti3C2F2、(e) Ti3C2Cl2和(f) Ti3C2Br2表面迁移的过渡态和相应的能量分布

Fig. 4 Schematic diagram of Li-ion migration path on (a) Ti3C2F2, (b) Ti3C2Cl2 and (c) Ti3C2Br2, and corresponding energy profiles and transition states of Li-ion migration on (d) Ti3C2F2, (e) Ti3C2Cl2 and (f) Ti3C2Br2 surfaces Colorful figures are available on website

图5 吸附多层锂离子的 (a) Ti3C2F2、(b) Ti3C2Cl2和(c) Ti3C2Br2的俯视图和主视图

Fig. 5 Top and side views of (a) Ti3C2F2, (b) Ti3C2Cl2 and (c) Ti3C2Br2 with the adsorption of multi-layer Liions Blue, black, nattier blue, and purple balls represent Ti, C, T, and Li atoms, respectively. 1 Å=0.1 nm Colorful figures are available on website

表4 M3-Ti3C2T2吸附多层锂离子时平均开路电压OCV、双层锂离子时吸附能(E2nd)和三层锂离子时吸附能(E3rd), 以及最大理论存储容量(CM)

Table 4 Average open circuit voltage (OCV), adsorption energies of the Liions on the double (E2nd) and triple (E3rd) layers, and the maximum theoretical capacity (CM) of the multi-layer Li-ion adsorption of M3-Ti3C2T2

Ti₃C₂T₂	OCV_1st/V	OCV_2nd/V	OCV_3rd/V	E_2nd/eV	E_3rd/eV	CM /(mA h·g^-1)
Ti₃C₂F₂	0.57	0.61	-	-5.25	-	521.41
Ti₃C₂Cl₂	0.37	0.53	0.54	-5.48	-4.51	674.21
Ti₃C₂Br₂	0.34	0.51	0.52	-5.39	-4.45	491.14

图6 吸附最多锂离子时M3-Ti3C2T2电极的部分态密度(PDOS)

Fig. 6 Partial density of states (PDOS) of M3-Ti3C2T2 electrode with the maximum adsorption of Liions

图7 双层Ti3C2Cl2的三种堆垛结构的俯视图和主视图

Fig. 7 Top and side views of three feasible stacking configurations of double Ti3C2Cl2. Blue, black, green, and purple balls represent Ti, C, T, and Li atoms, respectively; Colorful figures are available on website

图8 D33-Ti3C2Cl2中(a)锂离子扩散路径示意图、(b)过渡态构型和相应的能量分布, 以及(c)锂离子迁移的初始态和过渡态的原子结构和层间距离

Fig. 8 (a) Schematic illustration of the diffusion path of Liion, (b) corresponding energy profiles and configurations of transition states, (c) atomic structures and interlayer distances at initial and transition states of D33-Ti3C2Cl2 during interlayer Li-ion migration. Blue, black and green balls represent Ti, C and T atoms, respectively. 1 Å =0.1 nm; Colorful figures are available on website

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表面端基卤化Ti₃C₂ MXene应用于锂离子电池高容量电极材料的研究

Halogenated Ti₃C₂ MXene as High Capacity Electrode Material for Li-ion Batteries

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