Issue

Vol. 18 (2026)

Crystallographic Engineering Enables Fast Low-Temperature Ion Transport of TiNb2O7 for Cold-Region Lithium-Ion Batteries

https://doi.org/10.1007/s40820-025-01949-0
Lihua Wei
State Key Laboratory of Space Power‑Sources, School of Chemistry and Chemical Engineering, Harbin Institute of Technology, Harbin 150001, People’s Republic of China
Shenglu Geng
State Key Laboratory of Space Power‑Sources, School of Chemistry and Chemical Engineering, Harbin Institute of Technology, Harbin 150001, People’s Republic of China
Hailu Liu
State Key Laboratory of Space Power‑Sources, School of Chemistry and Chemical Engineering, Harbin Institute of Technology, Harbin 150001, People’s Republic of China
Liang Deng
State Key Laboratory of Space Power‑Sources, School of Chemistry and Chemical Engineering, Harbin Institute of Technology, Harbin 150001, People’s Republic of China
Yiyang Mao
State Key Laboratory of Space Power‑Sources, School of Chemistry and Chemical Engineering, Harbin Institute of Technology, Harbin 150001, People’s Republic of China
Yanbin Ning
State Key Laboratory of Space Power‑Sources, School of Chemistry and Chemical Engineering, Harbin Institute of Technology, Harbin 150001, People’s Republic of China
Biqiong Wang
China Tower Corporation Limited No, 9 Dongran North Street, Haidian District, Beijing 100089, People’s Republic of China
Yueping Xiong
State Key Laboratory of Space Power‑Sources, School of Chemistry and Chemical Engineering, Harbin Institute of Technology, Harbin 150001, People’s Republic of China
Yan Zhang
State Key Laboratory of Space Power‑Sources, School of Chemistry and Chemical Engineering, Harbin Institute of Technology, Harbin 150001, People’s Republic of China
Shuaifeng Lou
State Key Laboratory of Space Power‑Sources, School of Chemistry and Chemical Engineering, Harbin Institute of Technology, Harbin 150001, People’s Republic of China

Corresponding Author: Shuaifeng Lou

shuaifeng.lou@hit.edu.cn

Nano-Micro Letters, Vol. 18 (2026), Article Number: 91

Abstract

TiNb2O7 represents an up-and-coming anode material for fast-charging lithium-ion batteries, but its practicalities are severely impeded by slow transfer rates of ionic and electronic especially at the low-temperature conditions. Herein, we introduce crystallographic engineering to enhance structure stability and promote Li+ diffusion kinetics of TiNb2O7 (TNO). The density functional theory computation reveals that Ti4+ is replaced by Sb5+ and Nb5+ in crystal lattices, which can reduce the Li+ diffusion impediment and improve electronic conductivity. Synchrotron radiation X-ray 3D nano-computed tomography and in situ X-ray diffraction measurement confirm the introduction of Sb/Nb alleviates volume expansion during lithiation and delithiation processes, contributing to enhancing structure stability. Extended X-ray absorption fine structure spectra results verify that crystallographic engineering also increases short Nb-O bond length in TNO-Sb/Nb. Accordingly, the TNO-Sb/Nb anode delivers an outstanding capacity retention rate of 89.8% at 10 C after 700 cycles and excellent rate performance (140.4 mAh g−1 at 20 C). Even at −30 °C, TNO-Sb/Nb anode delivers a capacity of 102.6 mAh g−1 with little capacity degeneration for 500 cycles. This work provides guidance for the design of fast-charging batteries at low-temperature condition.


Highlights:
1 Sb element is introduced into TiNb2O7 successfully.
2 Such crystallographic engineering can narrow the bandgap and broaden the Li+ transport channel, making TNO-Sb/Nb electrode possess a better low-temperature performance.
3 Such a synergy effect enables TNO-Sb/Nb with large reversible capacity, superior rate performance (140.4 mAh g−1 at 20 C), and a high durability of 500 cycles even at −30 °C, holding brand promises in practical applications.

Keywords

Lithium-ion batteries Low-temperature conditions Crystallographic engineering TiNb2O7 Structure stability
Wei, Lihua, Shenglu Geng, Hailu Liu, Liang Deng, Yiyang Mao, Yanbin Ning, Biqiong Wang, Yueping Xiong, Yan Zhang, and Shuaifeng Lou. 2026. “Crystallographic Engineering Enables Fast Low-Temperature Ion Transport of TiNb2O7 for Cold-Region Lithium-Ion Batteries”. Nano-Micro Letters 18 (January):91. https://doi.org/10.1007/s40820-025-01949-0.
Download Citation
Endnote/Zotero/Mendeley (RIS)
BibTeX
References
  1. C.-Y. Wang, T. Liu, X.-G. Yang, S. Ge, N.V. Stanley et al., Fast charging of energy-dense lithium-ion batteries. Nature 611(7936), 485–490 (2022). https://doi.org/10.1038/s41586-022-05281-0
  2. J. Liu, M. Yue, S. Wang, Y. Zhao, J. Zhang, A review of performance attenuation and mitigation strategies of lithium-ion batteries. Adv. Funct. Mater. 32(8), 2107769 (2022). https://doi.org/10.1002/adfm.202107769
  3. M. Weiss, R. Ruess, J. Kasnatscheew, Y. Levartovsky, N.R. Levy et al., Fast charging of lithium-ion batteries: a review of materials aspects. Adv. Energy Mater. 11(33), 2101126 (2021). https://doi.org/10.1002/aenm.202101126
  4. L. Zhao, B. Ding, X.-Y. Qin, Z. Wang, W. Lv et al., Revisiting the roles of natural graphite in ongoing lithium-ion batteries. Adv. Mater. 34(18), 2106704 (2022). https://doi.org/10.1002/adma.202106704
  5. J. Bi, Z. Du, J. Sun, Y. Liu, K. Wang et al., On the road to the frontiers of lithium-ion batteries: a review and outlook of graphene anodes. Adv. Mater. 35(16), 2210734 (2023). https://doi.org/10.1002/adma.202210734
  6. T. Gao, Y. Han, D. Fraggedakis, S. Das, T. Zhou et al., Interplay of lithium intercalation and plating on a single graphite p. Joule 5(2), 393–414 (2021). https://doi.org/10.1016/j.joule.2020.12.020
  7. J. Hou, M. Yang, D. Wang, J. Zhang, Fundamentals and challenges of lithium ion batteries at temperatures between −40 and 60 °C. Adv. Energy Mater. 10(18), 1904152 (2020). https://doi.org/10.1002/aenm.201904152
  8. Y. Liu, Y. Zhu, Y. Cui, Challenges and opportunities towards fast-charging battery materials. Nat. Energy 4(7), 540–550 (2019). https://doi.org/10.1038/s41560-019-0405-3
  9. C.-Y. Wang, G. Zhang, S. Ge, T. Xu, Y. Ji et al., Lithium-ion battery structure that self-heats at low temperatures. Nature 529(7587), 515–518 (2016). https://doi.org/10.1038/nature16502
  10. L. Zhang, C. Zhu, S. Yu, D. Ge, H. Zhou, Status and challenges facing representative anode materials for rechargeable lithium batteries. J. Energy Chem. 66, 260–294 (2022). https://doi.org/10.1016/j.jechem.2021.08.001
  11. J.-T. Han, Y.-H. Huang, J.B. Goodenough, New anode framework for rechargeable lithium batteries. Chem. Mater. 23(8), 2027–2029 (2011). https://doi.org/10.1021/cm200441h
  12. Y. Yang, J. Zhao, Wadsley-Roth crystallographic shear structure niobium‐based oxides: promising anode materials for high‐safety lithium‐ion batteries. Adv. Sci. 8(12), 2004855 (2021). https://doi.org/10.1002/advs.202004855
  13. Y. Zhang, W. Zhao, C. Kang, S. Geng, J. Zhu et al., Phase-junction engineering triggered built-in electric field for fast-charging batteries operated at −30 °C. Matter 6(6), 1928–1944 (2023). https://doi.org/10.1016/j.matt.2023.03.026
  14. S. Geng, Y. Zhang, L. Shi, A. Shi, L. Zhou et al., Enabling 20 min fast-charging Ah-level pouch cell by tailoring the electronic structure and ion diffusion in TiNb2O7. Energy Storage Mater. 68, 103339 (2024). https://doi.org/10.1016/j.ensm.2024.103339
  15. A. Shi, Y. Zhang, S. Geng, X. Song, G. Yin et al., Highly oxidized state dopant induced Nb-O bond distortion of TiNb2O7 for extremely fast-charging batteries. Nano Energy 123, 109349 (2024). https://doi.org/10.1016/j.nanoen.2024.109349
  16. L. Yin, D. Pham-Cong, I. Jeon, J.-P. Kim, J. Cho et al., Electrochemical performance of vertically grown WS2 layers on TiNb2O7 nanostructures for lithium-ion battery anodes. Chem. Eng. J. 382, 122800 (2020). https://doi.org/10.1016/j.cej.2019.122800
  17. F. Yu, B. Miglani, S. Yuan, R. Yekani, K.H. Bevan et al., Fe3+-substitutional doping of nanostructured single-crystal TiNb2O7 for long-stable cycling of ultra-fast charging anodes. Nano Energy 133, 110494 (2025). https://doi.org/10.1016/j.nanoen.2024.110494
  18. I. Jeon, L. Yin, D. Yang, H. Chen, S.W. Go et al., Enhanced Li storage of pure crystalline-C60 and TiNb2O7-nanostructure composite for Li-ion battery anodes. J. Energy Chem. 97, 478–485 (2024). https://doi.org/10.1016/j.jechem.2024.06.004
  19. B. Guo, X. Yu, X.-G. Sun, M. Chi, Z.-A. Qiao et al., A long-life lithium-ion battery with a highly porous TiNb2O7 anode for large-scale electrical energy storage. Energy Environ. Sci. 7(7), 2220–2226 (2014). https://doi.org/10.1039/C4EE00508B
  20. H. Wang, R. Qian, Y. Cheng, H.-H. Wu, X. Wu et al., Micro/nanostructured TiNb2O7-related electrode materials for high-performance electrochemical energy storage: recent advances and future prospects. J. Mater. Chem. A 8(36), 18425–18463 (2020). https://doi.org/10.1039/D0TA04209A
  21. R. Zhan, S. Liu, W. Wang, Z. Chen, S. Tu et al., Micrometer-scale single crystalline ps of niobium titanium oxide enabling an Ah-level pouch cell with superior fast-charging capability. Mater. Horiz. 10(11), 5246–5255 (2023). https://doi.org/10.1039/D3MH01160G
  22. R. Wang, L. Wang, R. Liu, X. Li, Y. Wu et al., “Fast-charging” anode materials for lithium-ion batteries from perspective of ion diffusion in crystal structure. ACS Nano 18(4), 2611–2648 (2024). https://doi.org/10.1021/acsnano.3c08712
  23. L. Hu, L. Luo, L. Tang, C. Lin, R. Li et al., Ti2Nb2xO4+5x anode materials for lithium-ion batteries: a comprehensive review. J. Mater. Chem. A 6(21), 9799–9815 (2018). https://doi.org/10.1039/c8ta00895g
  24. H. Song, Y.-T. Kim, A Mo-doped TiNb2O7 anode for lithium-ion batteries with high rate capability due to charge redistribution. Chem. Commun. 51(48), 9849–9852 (2015). https://doi.org/10.1039/C5CC02221E
  25. Y. Sheng, X. Yue, W. Hao, Y. Dong, Y. Liu et al., Balancing the ion/electron transport of graphite anodes by a La-doped TiNb2O7 functional coating for fast-charging Li-ion batteries. Nano Lett. 24(12), 3694–3701 (2024). https://doi.org/10.1021/acs.nanolett.3c05151
  26. S. Zhu, M. Su, S. Lu, S. Yang, Y. Huang et al., Enhanced performance of Mo-doped TiNb2O7 anode material for lithium-ion batteries via KOH sub-molten salt synthesis. Appl. Surf. Sci. 669, 160507 (2024). https://doi.org/10.1016/j.apsusc.2024.160507
  27. C. Yang, D. Ma, J. Yang, M. Manawan, T. Zhao et al., Crystallographic insight of reduced lattice volume expansion in mesoporous Cu2+-doped TiNb2O7 microspheres during Li+ insertion. Adv. Funct. Mater. 33(15), 2212854 (2023). https://doi.org/10.1002/adfm.202212854
  28. Y. Zhang, C. Kang, W. Zhao, B. Sun, X. Xiao et al., Crystallographic engineering to reduce diffusion barrier for enhanced intercalation pseudocapacitance of TiNb2O7 in fast-charging batteries. Energy Storage Mater. 47, 178–186 (2022). https://doi.org/10.1016/j.ensm.2022.01.061
  29. G. Yu, J. Huang, X. Bai, T. Li, S. Song et al., Engineering of cerium modified TiNb2O7 nanops for low-temperature lithium-ion battery. Small 20(34), e2308858 (2024). https://doi.org/10.1002/smll.202308858
  30. X. Jin, Y. Deng, H. Tian, M. Zhou, W. Tang et al., Homovalent doping: an efficient strategy of the enhanced TiNb2O7 anode for lithium-ion batteries. Green Energy Environ. 9(8), 1257–1266 (2024). https://doi.org/10.1016/j.gee.2023.01.007
  31. C. Yang, C. Lin, S. Lin, Y. Chen, J. Li, Cu0.02Ti0.94Nb2.04O7: an advanced anode material for lithium-ion batteries of electric vehicles. J. Power. Sources 328, 336–344 (2016). https://doi.org/10.1016/j.jpowsour.2016.08.027
  32. J. Gao, X. Cheng, S. Lou, Y. Ma, P. Zuo et al., Self-doping Ti1-xNb2+xO7 anode material for lithium-ion battery and its electrochemical performance. J. Alloys Compd. 728, 534–540 (2017). https://doi.org/10.1016/j.jallcom.2017.09.045
  33. X. Cao, H. Li, Y. Qiao, P. He, Y. Qian et al., Reversible anionic redox chemistry in layered Li4/7[□1/7Mn6/7]O2 enabled by stable Li-O-vacancy configuration. Joule 6(6), 1290–1303 (2022). https://doi.org/10.1016/j.joule.2022.05.006
  34. J. Ma, Y. Xiang, J. Xu, W. Zhang, H. Zhang et al., Reducing lithium-diffusion barrier on the wadsley-Roth crystallographic shear plane via low-valent cation doping for ultrahigh power lithium-ion batteries. Adv. Energy Mater. 15(12), 2403623 (2025). https://doi.org/10.1002/aenm.202403623
  35. T. Brezesinski, J. Wang, S.H. Tolbert, B. Dunn, Ordered mesoporous alpha-MoO3 with iso-oriented nanocrystalline walls for thin-film pseudocapacitors. Nat. Mater. 9(2), 146–151 (2010). https://doi.org/10.1038/nmat2612
  36. S. Lou, X. Cheng, Y. Zhao, A. Lushington, J. Gao et al., Superior performance of ordered macroporous TiNb2O7 anodes for lithium ion batteries: understanding from the structural and pseudocapacitive insights on achieving high rate capability. Nano Energy 34, 15–25 (2017). https://doi.org/10.1016/j.nanoen.2017.01.058
  37. L. Zhu, S. Xiang, M. Wang, D. Sun, X. Zhang et al., Lattice regulation boosts working voltage and energy density of Na3.12Fe2.44(P2O7)2 cathode for sodium-ion batteries. Adv. Funct. Mater. 35(26), 2419611 (2025). https://doi.org/10.1002/adfm.202419611
  38. B. Peng, Y. Chen, F. Wang, Z. Sun, L. Zhao et al., Unusual site-selective doping in layered cathode strengthens electrostatic cohesion of alkali-metal layer for practicable sodium-ion full cell. Adv. Mater. 34(6), e2103210 (2022). https://doi.org/10.1002/adma.202103210
  39. L. Du, Y. Zhang, Y. Xiao, D. Yuan, M. Yao et al., A defect-rich carbon induced built-in interfacial electric field accelerating ion-conduction towards superior-stable solid-state batteries. Energy Environ. Sci. 18(6), 2949–2961 (2025). https://doi.org/10.1039/D4EE05966B
  40. L. Xu, M. Yao, L. Du, Y. Chen, Y. Wei et al., Accelerating lithium ion conduction via activated interfacial dipole layer for long-life and high-voltage solid-state lithium-metal battery. J. Energy Chem. 108, 92–100 (2025). https://doi.org/10.1016/j.jechem.2025.03.073
  41. Q. Wang, Y. Zhang, M. Yao, K. Li, L. Xu et al., A lithium-selective “OR-gate” enables fast-kinetics and ultra-stable Li-rich cathodes for polymer-based solid-state batteries. Energy Environ. Sci. 18(6), 2931–2939 (2025). https://doi.org/10.1039/D4EE05264A
  42. Y. Zhang, Y. Chen, M. Yan, F. Chen, Reconstruction of relaxation time distribution from linear electrochemical impedance spectroscopy. J. Power. Sources 283, 464–477 (2015). https://doi.org/10.1016/j.jpowsour.2015.02.107
  43. Y. Lu, C.-Z. Zhao, R. Zhang, H. Yuan, L.-P. Hou et al., The carrier transition from Li atoms to Li vacancies in solid-state lithium alloy anodes. Sci. Adv. 7(38), eabi5520 (2021). https://doi.org/10.1126/sciadv.abi5520
  44. Y. Zhang, M. Yao, P. Jing, Y. Fu, W. Wang et al., Achieving a highly reversible four-electron redox of S/Cu2S for aqueous Zn/S─Cu battery. Angew. Chem. Int. Ed. 137(25), e202501205 (2025). https://doi.org/10.1002/ange.202501205
  45. P. Xue, C. Guo, L. Tan, Hydrogen-bonding crosslinking MXene to highly mechanically stable and super-zincophilic host for stable Zn metal anode. Chem. Eng. J. 472, 145056 (2023). https://doi.org/10.1016/j.cej.2023.145056
  46. S. Li, X. Cao, C.N. Schmidt, Q. Xu, E. Uchaker et al., TiNb2O7/graphene composites as high-rate anode materials for lithium/sodium ion batteries. J. Mater. Chem. A 4(11), 4242–4251 (2016). https://doi.org/10.1039/C5TA10510B
  47. A.G. Ashish, P. Arunkumar, B. Babu, P. Manikandan, S. Sarang et al., TiNb2O7/Graphene hybrid material as high performance anode for lithium-ion batteries. Electrochim. Acta 176, 285–292 (2015). https://doi.org/10.1016/j.electacta.2015.06.122
  48. Y. Zhang, M. Zhang, Y. Liu, H. Zhu, L. Wang et al., Oxygen vacancy regulated TiNb2O7 compound with enhanced electrochemical performance used as anode material in Li-ion batteries. Electrochim. Acta 330, 135299 (2020). https://doi.org/10.1016/j.electacta.2019.135299
  49. G. Wang, Z. Wen, L. Du, Y.-E. Yang, S. Li et al., Hierarchical Ti-Nb oxide microspheres with synergic multiphase structure as ultra-long-life anode materials for lithium-ion batteries. J. Power. Sources 367, 106–115 (2017). https://doi.org/10.1016/j.jpowsour.2017.09.061
  50. X. Wang, G. Shen, Intercalation pseudo-capacitive TiNb2O7@carbon electrode for high-performance lithium ion hybrid electrochemical supercapacitors with ultrahigh energy density. Nano Energy 15, 104–115 (2015). https://doi.org/10.1016/j.nanoen.2015.04.011
  51. H. Li, L. Shen, G. Pang, S. Fang, H. Luo et al., TiNb2O7 nanops assembled into hierarchical microspheres as high-rate capability and long-cycle-life anode materials for lithium ion batteries. Nanoscale 7(2), 619–624 (2015). https://doi.org/10.1039/C4NR04847D
  52. S. Gong, Y. Wang, Q. Zhu, M. Li, Y. Wen et al., High-rate lithium storage performance of TiNb2O7 anode due to single-crystal structure coupling with Cr3+-doping. J. Power. Sources 564, 232672 (2023). https://doi.org/10.1016/j.jpowsour.2023.232672
  53. H. Bian, J. Gu, Z. Song, H. Gong, Z. Zhang et al., An effective strategy to achieve high-power electrode by tin doping: Snx-TiNb2O7 as a promising anode material with a large capacity and high-rate performance for lithium-ion batteries. J. Mater. Sci. Mater. Electron. 34(26), 1826 (2023). https://doi.org/10.1007/s10854-023-11183-2
Read More
Author biographies are not available.
Download this PDF file
PDF SUPPLEMENTARY FILE
Statistic
Read Counter : 838 Download : 635

Most read articles by the same author(s)

1 2 > >>