Crystallographic Insight of Reduced Lattice Volume Expansion in Mesoporous Cu2+-Doped TiNb2O7 Microspheres during Li+ Insertion

Yang, Chengfu; Ma, Dongwei; Yang, Jing; Manawan, Maykel; Zhao, Ting; Feng, Yuanyuan; Li, Jiahui; Liu, Zhongzhu; Zhang, Yong‐Wei; Von Dreele, Robert B.; Toby, Brian H.; Albarrán, Carlos León; Pan, Jia Hong

doi:10.1002/adfm.202212854

Crystallographic Insight of Reduced Lattice Volume Expansion in Mesoporous Cu²⁺-Doped TiNb₂O₇ Microspheres during Li⁺ Insertion

Journal Article · Tue Jan 24 23:00:00 EST 2023 · Advanced Functional Materials

DOI:https://doi.org/10.1002/adfm.202212854· OSTI ID:1972286

Yang, Chengfu ^[1]; Ma, Dongwei ^[1]; Yang, Jing ^[2]; Manawan, Maykel ^[3]; Zhao, Ting ^[4]; Feng, Yuanyuan ^[1]; Li, Jiahui ^[1]; Liu, Zhongzhu ^[5]; Zhang, Yong‐Wei ^[2]; Von Dreele, Robert B. ^[6]; Toby, Brian H. ^[6]; Albarrán, Carlos León ^[7]; ^[8]

North China Electric Power University, Beijing (China)
Institute of High Performance Computing Agency for Science, Technology and Research (A*STAR) (Singapore)
Universitas Pertahanan Indonesia, Tajur (Indonesia)
University of Chinese Academy of Sciences, Beijing (China)
CITIC Metal Co., Ltd, Beijing (China)
Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
University of Southampton (United Kingdom)
North China Electric Power University, Beijing (China); Imperial College, London (United Kingdom)

TiNb₂O₇ represents a promising anode material for lithium-ion batteries (LIBs), but its practical applications are currently hampered by the non-negligible volumetric expansion and contraction during the charge/discharge process and the sluggish ion/electron kinetics. Here a combination technique is reported by systematically optimizing the porous and spherical morphology, crystal structure, and surface decoration of mesoporous Cu²⁺-doped TiNb₂O₇ microspheres to enhance the electrochemical Li⁺ storage performance and stability simultaneously. The Cu²⁺ dopants preferentially replace Ti⁴⁺ in crystal lattices, which decreases the Li⁺ diffusion barrier and increases the electronic conductivity, as confirmed by density functional theory (DFT) calculation and demonstrated by diverse electrochemical characterizations. The successful Cu²⁺ doping significantly reduces the lattice expansion coefficient from 7.26% to 4.61% after Li⁺ insertion along the b-axis of TiNb₂O₇, as visualized from in situ and ex situ XRD analysis. The optimal 5% Cu²⁺-doped TiNb₂O₇ with surface coating of N-doped carbon exhibits significantly enhanced specific capacity and rate and cyclic performances in both half- and full-cell configurations, demonstrating an excellent electrochemical behavior for fast-charging LIB applications.

View Accepted Manuscript (DOE)

Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); Central Universities

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1972286

Journal Information:: Advanced Functional Materials, Journal Name: Advanced Functional Materials Journal Issue: 15 Vol. 33; ISSN 1616-301X

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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Crystallographic Insight of Reduced Lattice Volume Expansion in Mesoporous Cu²⁺-Doped TiNb₂O₇ Microspheres during Li⁺ Insertion