Mechanistic Probing of Encapsulation and Confined Growth of Lithium Crystals in Carbonaceous Nanotubes

Wei, Ping1; Cheng, Yong1; Yan, Xiaolin1; Ye, Weibin1; Lan, Xiangna1; Wang, Lina2,3; Sun, Jingjie1; Yu, Zhiyang4; Luo, Guangfu2,3; Yang, Yong1; Rummeli, Mark H.5,6,7,8; Wang, Ming-Sheng1

2021-10-01

10.1002/adma.202105228

ADVANCED MATERIALS   影响因子和分区

0935-9648

1521-4095

Encapsulation of lithium in the confined spaces within individual nanocapsules is intriguing and highly desirable for developing high-performance Li metal anodes. This work aims for a mechanistic understanding of Li encapsulation and its confined growth kinetics inside 1D enclosed spaces. To achieve this, amorphous carbon nanotubes are employed as a model host using in situ transmission electron microscopy. The carbon shells have dual roles, providing geometric/mechanical constraints and electron/ion transport channels, which profoundly alter the Li growth patterns. Li growth/dissolution takes place via atom addition/removal at the free surfaces through Li+ diffusion along the shells in the electric field direction, resulting in the formation of unusual Li structures, such as poly-crystalline nanowires and free-standing 2D ultrathin (1-2 nm) Li membranes. Such confined front-growth processes are dominated by Li {110} or {200} growing faces, distinct from the root growth of single-crystal Li dendrites outside the nanotubes. Controlled experiments show that high lithiophilicity/permeability, enabled by sufficient nitrogen/oxygen doping or pre-lithiation, is critical for the stable encapsulation of lithium inside carbonaceous nanocapsules. First-principles-based calculations reveal that N/O doping can reduce the diffusion barrier for Li+ penetration, and facilitate Li filling driven by energy minimization associated with the formation of low-energy Li/C interfaces.

2D Li crystals amorphous carbon nanotubes in situ TEM Li encapsulation lithium metal anodes spatially confined growth

SCI ; EI

英语

NI论文

其他

National Natural Science Foundation of China[52172240,21935009,52071225] ; Fundamental Research Funds for the Central Universities[20720200075] ; Czech Republic under the ERDF program "Institute of Environmental Technology-Excellent Research"[CZ.02.1.01/0.0/0.0/16_019/0000853] ; Sino-German Research Institute[GZ 1400] ; Guangdong Provincial Key Laboratory of Computational Science and Material Design[2019B030301001]

Chemistry ; Science & Technology - Other Topics ; Materials Science ; Physics

Chemistry, Multidisciplinary ; Chemistry, Physical ; Nanoscience & Nanotechnology ; Materials Science, Multidisciplinary ; Physics, Applied ; Physics, Condensed Matter

WOS:000707325200001

WILEY-V C H VERLAG GMBH

20214211025474

Amorphous carbon ; Anodes ; Calculations ; Carbon nanotubes ; Crystal atomic structure ; Diffusion barriers ; Electric fields ; Growth kinetics ; Lithium ; Nanocapsules ; Single crystals

Lithium and Alloys:542.4 ; Alkali Metals:549.1 ; Electricity: Basic Concepts and Phenomena:701.1 ; Electron Tubes:714.1 ; Optical Devices and Systems:741.3 ; Nanotechnology:761 ; Mathematics:921 ; Atomic and Molecular Physics:931.3 ; Solid State Physics:933 ; Crystalline Solids:933.1 ; Crystal Lattice:933.1.1 ; Amorphous Solids:933.2

MATERIALS SCIENCE

Web of Science

1.Xiamen Univ, Coll Chem & Chem Engn, Coll Mat, State Key Lab Phys Chem Solid Surfaces Coll Mat, Xiamen 361005, Peoples R China
2.Southern Univ Sci & Technol, Dept Mat Sci & Engn, Shenzhen 518055, Peoples R China
3.Southern Univ Sci & Technol, Guangdong Prov Key Lab Computat Sci & Mat Design, Shenzhen 518055, Peoples R China
4.Fuzhou Univ, Coll Chem, State Key Lab Photocatalysis Energy & Environm, Fuzhou 350002, Peoples R China
5.Soochow Univ, Key Lab Adv Carbon Mat & Wearable Energy Technol, Soochow Inst Energy & Mat Innovat SIEMIS, Coll Energy, Suzhou 215006, Peoples R China
6.Polish Acad Sci, Ctr Polymer & Carbon Mat, M Curie Sklodowskiej 34, PL-41819 Zabrze, Poland
7.VSB Tech Univ Ostrava, Inst Environm Technol, 17 Listopadu 15, Ostrava 70833, Czech Republic
8.Helmholtzstr 20, D-01069 Dresden, Germany

Wei, Ping,Cheng, Yong,Yan, Xiaolin,et al. Mechanistic Probing of Encapsulation and Confined Growth of Lithium Crystals in Carbonaceous Nanotubes[J]. ADVANCED MATERIALS,2021,33.

Wei, Ping.,Cheng, Yong.,Yan, Xiaolin.,Ye, Weibin.,Lan, Xiangna.,...&Wang, Ming-Sheng.(2021).Mechanistic Probing of Encapsulation and Confined Growth of Lithium Crystals in Carbonaceous Nanotubes.ADVANCED MATERIALS,33.

Wei, Ping,et al."Mechanistic Probing of Encapsulation and Confined Growth of Lithium Crystals in Carbonaceous Nanotubes".ADVANCED MATERIALS 33(2021).