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Progress and perspectives of the covalent organic frameworks in regulating interface chemistry for high‐energy density Li metal batteries AITranslate

Qi An1; Lu Liu1; Panpan Mao1; Fanyu Xie1; Yufeng Fan1; Huaiyu Shao3; Hong Guo1,2;
1.International Joint Research Center for Advanced Energy Materials of Yunnan Province, School of Materials and Energy, Yunnan University, Kunming 650091, China
2.Southwest United Graduate School, Kunming 650091, China
3.Institute of Applied Physics and Materials Engineering, University of Macau, Macau 999078, China
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Abstract AITranslate

Lithium metal is regarded as an ideal anode material for high-energy-density batteries due to its high theoretical capacity and low electrochemical potential. However, its practical application is hindered by unstable electrode-electrolyte interfaces and lithium dendrite growth. Covalent organic frameworks (COFs), with ordered ion transport channels and abundant lithiophilic sites, offer a promising solution by facilitating uniform lithium deposition, suppressing dendrites, and mitigating side reactions. This review presents a comprehensive overview of the application of COFs in various battery components for regulating interfacial chemistry and inhibiting dendrite growth. The design concepts and synthesis techniques of COFs are explained in detail, and the discussion of present issues and potential future research avenues is included in the end.

KeyWords AITranslate

covalent organic frameworks interface chemistry lithium dendrites lithium metal batteries

1.B. Liu, J. G. Zhang, and W. Xu, "Advancing Lithium Metal Batteries," Joule 2, no. 5 (2018): 833–845, https://doi.org/10.1016/j.joule.2018.03.008.

2.L. C. Kong, Y. Li, C. Peng, et al., "Achieving Burst Li+ Channels via Quasi-Two-Dimensional Fluorinated Metal-Organic Framework Modulating Functionalized Interface," Nature Communications 16 (2025): 1885, https://doi.org/10.1038/s41467-025-57106-z.

3.C. Zhang, J. M. Yu, Y. Y. Cui, et al., "An Electron-Blocking Interface for Garnet-Based Quasi-Solid-State Lithium-Metal Batteries to Improve Lifespan," Nature Communications 15 (2024): 5325, https://doi.org/10.1038/s41467-024-49715-x.

4.Y. J. Lei, L. F. Zhao, W. H. Lai, et al., "Electrochemical Coupling in Subnanometer Pores/Channels for Rechargeable Batteries," Chemical Society Reviews 53, no. 8 (2024): 3829–3895, https://doi.org/10.1039/D3CS01043K.

5.Y. J. Lei, X. X. Lu, H. Yoshikawa, et al., "Understanding the Charge Transfer Effects of Single Atoms for Boosting the Performance of Na-S Batteries," Nature Communications 15 (2024): 3325, https://doi.org/10.1038/s41467-024-47628-3.

6.L. F. Zhao, Y. Tao, Y. Y. Zhang, et al., "A Critical Review on Room-Temperature Sodium-Sulfur Batteries: from Research Advances to Practical Perspectives," Advanced Materials 36, no. 25 (2024): 2402337, https://doi.org/10.1002/adma.202402337.

7.Q. An, Q. Liu, P. P. Mao, et al., "Developing the Tandem Structure to Regulate Interfacial Chemistry and Promote Ion Transport Kinetics toward High-Voltage Lithium Metal Batteries," Angewandte Chemie International Edition 64, no. 19 (2025): e202422539, https://doi.org/10.1002/anie.202422539.

8.M. S. Kim, Z. W. Zhang, P. E. Rudnicki, et al., "Suspension Electrolyte with Modified Li+ Solvation Environment for Lithium Metal Batteries," Nature Materials 21 (2022): 445–454, https://doi.org/10.1038/s41563-021-01172-3.

9.Z. W. Zhang, Y. Z. Li, R. Xu, et al., "Capturing the Swelling of Solid-Electrolyte Interphase in Lithium Metal Batteries," Science 375 (2022): 66–70, https://doi.org/10.1126/science.abi8703.

10.Y. Zhao, T. H. Zhou, T. Ashirov, et al., "Fluorinated Ether Electrolyte with Controlled Solvation Structure for High Voltage Lithium Metal Batteries," Nature Communications 13 (2022): 2575, https://doi.org/10.1038/s41467-022-29199-3.

11.Q. An, H. E. Wang, G. F. Zhao, et al., "Understanding Dual-Polar Group Functionalized COFs for Accelerating Li-ion Transport and Dendrite-Free Deposition in Lithium Metal Anodes," Energy Environmental Materials 6, no. 2 (2023): e12345, https://doi.org/10.1002/eem2.12345.

12.Y. C. Wen, J. Y. Ding, J. Liu, M. Zhu, and R. Z. Hu, "A Separator Rich in SnF2 and NO3- Directs an Ultra-Stable Interface toward High Performance Li Metal Batteries," Energy Environmental Science 16, no. 7 (2023): 2957–2967, https://doi.org/10.1039/D3EE00664F.

13.W. L. Qin, D. D. Han, X. W. Zhang, et al., "Redox-Active Metal-Covalent Organic Frameworks for Dendrite-Free Lithium Metal Batteries," Advanced Materials 37, no. 14 (2025): 2418638, https://doi.org/10.1002/adma.202418638.

14.Q. An, L. L. Wang, G. F. Zhao, et al., "Constructing Cooperative Interface via Bi-Functional COF for Facilitating the Sulfur Conversion and Li+ Dynamics," Advanced Materials 36, no. 4 (2024): 2305818, https://doi.org/10.1002/adma.202305818.

15.Y. Yang, Z. Y. Sun, Y. W. Wu, et al., "Porous Organic Framework Materials (MOF, COF, and HOF) as the Multifunctional Separator for Rechargeable Lithium Metal Batteries," Small 20, no. 37 (2024): 2401457, https://doi.org/10.1002/smll.202401457.

16.C. H. Zhang, Z. Luo, K. A. Chen, et al., "Urea-Linked Covalent Organic Framework as a Li-Ion Guided Channel Enabling Ultra-Stable Lithium Metal Anode in Carbonate-Based Electrolyte," Angewandte Chemie International Edition 64, no. 22 (2025): e202500314, https://doi.org/10.1002/anie.202500314.

17.Y. X. Yang, C. H. Zhang, G. F. Zhao, et al., "Regulating the Electron Structure of Covalent Organic Frameworks by Strong Electron-Withdrawing Nitro to Construct Specific Li+ Oriented Channel," Advanced Energy Materials 13, no. 26 (2023): 2300725, https://doi.org/10.1002/aenm.202300725.

18.C. Li, D. D. Wang, G. S. Ho, et al., "Anthraquinone-Based Silicate Covalent Organic Frameworks as Solid Electrolyte Interphase for High-Performance Lithium-Metal Batteries," Journal of the American Chemical Society 145, no. 45 (2023): 24603–24614, https://doi.org/10.1021/jacs.3c06723.

19.C. H. Zhang, J. Y. Xie, C. T. Zhao, et al., "Regulating the Lithium Ions’ Local Coordination Environment through Designing a COF with Single Atomic Co Site to Achieve Dendrite-Free Lithium-Metal Batteries," Advanced Materials 35, no. 40 (2023): 2304511, https://doi.org/10.1002/adma.202304511.

20.L. G. Yue, X. Y. Wang, L. Chen, et al., "In Situ Interface Engineering of Highly Nitrogen Rich Triazine-Based Covalent Organic Frameworks for an Ultra-Stable, Dendrite-Free Lithium-Metal Anode," Energy Environmental Science 17, no. 3 (2024): 1117–1131, https://doi.org/10.1039/D3EE02803H.

21.G. Feng, Q. Y. Ma, D. Luo, et al., "Designing Cooperative Ion Transport Pathway in Ultra-Thin Solid-State Electrolytes toward Practical Lithium Metal Batteries," Angewandte Chemie International Edition 64, no. 1 (2025): e202413306, https://doi.org/10.1002/anie.202413306.

22.S. Y. Yu, G. F. Zhao, H. Y. Zhu, et al., "Constructing Donor-Acceptor Li+ Transfer Channels Based on Covalent Organic Frameworks for Quasi-Solid-State Li Batteries," Science China Chemistry 68 (2025): 6073–6082, https://doi.org/10.1007/s11426-025-2882-7.

23.C. H. Zhang, L. W. Zhao, F. K. Li, et al., "Optimizing the Electron Density of PVDF-HFP-Based Solid Polymer Electrolyte by Donor-Acceptor COF toward High-Performance Solid-State Lithium Metal Batteries," Advanced Materials 37, no. 44 (2025): e13427, https://doi.org/10.1002/adma.202513427.

24.G. F. Zhao, H. Ma, C. H. Zhang, et al., "Constructing Donor–Acceptor‑Linked COFs Electrolytes to Regulate Electron Density and Accelerate the Li+ Migration in Quasi‑Solid‑State Battery," Nano-Micro Letters 17 (2025): 21, https://doi.org/10.1007/s40820-024-01509-y.

25.W. Z. Liang, X. Y. Zhou, B. Zhang, et al., "The Versatile Establishment of Charge Storage in Polymer Solid Electrolyte with Enhanced Charge Transfer for LiF-Rich SEI Generation in Lithium Metal Batteries," Angewandte Chemie International Edition 63, no. 18 (2024): e202320149, https://doi.org/10.1002/anie.202320149.

26.X. Y. Xu, S. Q. Zhang, K. Xu, H. Z. Chen, X. L. Fan, and N. Huang, "Janus Dione-Based Conjugated Covalent Organic Frameworks with High Conductivity as Superior Cathode Materials," Journal of the American Chemical Society 145, no. 2 (2023): 1022–1030, https://doi.org/10.1021/jacs.2c10509.

27.Z. D. Zhao, W. J. Chen, S. Impeng, et al., "Covalent Organic Framework-Based Ultrathin Crystalline Porous Film: Manipulating Uniformity of Fluoride Distribution for Stabilizing Lithium Metal Anode," Journal of Materials Chemistry A 8, no. 6 (2020): 3459–3467, https://doi.org/10.1039/C9TA13384D.

28.Y. F. Yuan, Z. Y. Zhang, Z. Y. Zhang, et al., "Highly Conductive Imidazolate Covalent Organic Frameworks with Ether Chains as Solid Electrolytes for Lithium Metal Batteries," Angewandte Chemie International Edition 63, no. 18 (2024): e202402202, https://doi.org/10.1002/anie.202402202.

29.C. Q. Li, A. Yu, W. K. Zhao, et al., "Extending the π-Conjugation of a Donor-Acceptor Covalent Organic Framework for High-Rate and High-Capacity Lithium-Ion Batteries," Angewandte Chemie International Edition 63, no. 48 (2024): e202409421, https://doi.org/10.1002/anie.202409421.

30.S. Zheng, Y. B. Fu, C. Song, et al., "Anode-Protective Covalent Organic Framework Layer with Synergistic Cation–Anion Regulation for Dendrite-Free Lithium Metal Batteries," Journal of the American Chemical Society 147, no. 34 (2025): 31249–31259, https://doi.org/10.1021/jacs.5c10386.

31.Y. X. Chen, J. He, M. J. Li, et al., "Regulation of Interfacial Ion Transport via Honeycomb-Architected Covalent Organic Frameworks for Lithium Metal Batteries," Advanced Materials 38, no. 4 (2026): e12997, https://doi.org/10.1002/adma.202512997.

32.M. H. Gu, J. X. Wu, C. Li, et al., "Mechanically Assisted Li+-Conduction in Crown Ether-Covalent Organic Frameworks for Lithium Metal Batteries," Advanced Materials 38, no. 5 (2026): e11473, https://doi.org/10.1002/adma.202511473.

33.A. P. Coˆt́e, A. I. Benin, N. W. Ockwig, M. O’Keeffe, A. J. Matzger, and O. M. Yaghi, "Porous, Crystalline, Covalent Organic Frameworks," Science 310, no. 5751 (2005): 1166–1170, https://doi.org/10.1126/science.1120411.

34.Z. W. Yang, J. J. Li, Y. H. Wang, et al., "Metal/Covalent-Organic Framework-Based Biosensors for Nucleic Acid Detection," Coordination Chemistry Reviews 491, no. 15 (2023): 215249, https://doi.org/10.1016/j.ccr.2023.215249.

35.H. H. Pan, Y. F. Ren, and Q. Wang, "New Vitality of Covalent Organic Frameworks Endued by Phthalocyanine: Yesterday, Today, and Tomorrow," Coordination Chemistry Reviews 527, no. 15 (2025): 216404, https://doi.org/10.1016/j.ccr.2024.216404.

36.L. Goswami, A. Kushwaha, M. Shabbir, P. K. Dikshit, S. Oh, and U. Bhan, "Covalent Organic Frameworks (COFs) and COFs-Based Hybrid Architectonics: A Promising Material Platform for Organic Micropollutants Detection and Removal from Wastewater," Coordination Chemistry Reviews 527, no. 15 (2025): 216398, https://doi.org/10.1016/j.ccr.2024.216398.

37.K. Y. Geng, T. He, R. Y. Liu, et al., "Covalent Organic Frameworks: Design, Synthesis, and Functions," Chemical Reviews 120, no. 16 (2020): 8814–8933, https://doi.org/10.1021/acs.chemrev.9b00550.

38.X. J. Sun, M. T. Di, J. Liu, L. Gao, X. M. Yan, and G. H. He, "Continuous Covalent Organic Frameworks Membranes: from Preparation Strategies to Applications," Small 19, no. 44 (2023): 2303757, https://doi.org/10.1002/smll.202303757.

39.T. Li, Y. Pan, B. B. Shao, et al., "Covalent–Organic Framework (COF)-Core–Shell Composites: Classification, Synthesis, Properties, and Applications," Advanced Functional Materials 33, no. 45 (2023): 2304990, https://doi.org/10.1002/adfm.202304990.

40.M. Chafiq, A. Chaouiki, and Y. G. Ko, "Advances in COFs for Energy Storage Devices: Harnessing the Potential of Covalent Organic Framework Materials," Energy Storage Materials 63 (2023): 103014, https://doi.org/10.1016/j.ensm.2023.103014.

41.S. Y. Ding and W. Wang, "Covalent Organic Frameworks (COFs): from Design to Applications," Chemical Society Reviews 42, no. 45 (2013): 548–568, https://doi.org/10.1039/C2CS35072F.

42.P. Kuhn, M. Antonietti, and A. Thomas, "Porous, Covalent Triazine-Based Frameworks Prepared by Ionothermal Synthesis," Angewandte Chemie International Edition 47, no. 18 (2008): 3450–3453, https://doi.org/10.1002/anie.200705710.

43.L. Fang, H. Xu, S. Y. Qiu, et al., "Autocatalytic Interfacial Synthesis of Self-Standing Amide-Linked Covalent Organic Framework Membranes," Angewandte Chemie International Edition 64, no. 13 (2025): e202423220, https://doi.org/10.1002/anie.202423220.

44.S. Chandra, S. Kandambeth, B. P. Biswal, et al., "Chemically Stable Multilayered Covalent Organic Nanosheets from Covalent Organic Frameworks via Mechanical Delamination," Journal of the American Chemical Society 135, no. 47 (2013): 17853–17861, https://doi.org/10.1021/ja408121p.

45.C. H. Zhang, F. K. Li, T. T. Gu, et al., "Covalent Organic Frameworks for High-Performance Rechargeable Lithium Metal Batteries: Strategy, Mechanism, and Application," Progress in Materials Science 152 (2025): 101455, https://doi.org/10.1016/j.pmatsci.2025.101455.

46.K. M. Diederichsen, E. J. McShane, and B. D. McCloskey, "Promising Routes to a High Li+ Transference Number Electrolyte for Lithium Ion Batteries," ACS Energy Letters 2, no. 11 (2017): 2563–2575, https://doi.org/10.1021/acsenergylett.7b00792.

47.Y. M. Hu, L. J. Wayment, C. Haslam, et al., "Covalent Organic Framework Based Lithium-Ion Battery: Fundamental, Design and Characterization," EnergyChem 3, no. 1 (2021): 100048, https://doi.org/10.1016/j.enchem.2020.100048.

48.B. Q. Xiong, X. W. Zhou, G. L. Xu, et al., "In Situ Construction of an Ultrarobust and Lithiophilic Li-Enriched Li–N Nanoshield for High-Performance Ge-Based Anode Materials," ACS Energy Letters 5, no. 11 (2020): 3490–3497, https://doi.org/10.1021/acsenergylett.0c02121.

49.Y. Wang, Z. T. Qu, S. T. Geng, et al., "Anode-Free Lithium Metal Batteries Based on an Ultrathin and Respirable Interphase Layer," Angewandte Chemie International Edition 62, no. 27 (2023): e202304978, https://doi.org/10.1002/anie.202304978.

50.A. J. Hu, W. Chen, X. C. Du, et al., "An Artificial Hybrid Interphase for an Ultrahigh-Rate and Practical Lithium Metal Anode," Energy Environmental Science 14, no. 7 (2021): 4115–4124, https://doi.org/10.1039/D1EE00508A.

51.Z. H. Li, W. Y. Ji, T.-X. Wang, et al., "Guiding Uniformly Distributed Li–Ion Flux by Lithiophilic Covalent Organic Framework Interlayers for High-Performance Lithium Metal Anodes," ACS Applied Materials & Interfaces 13, no. 19 (2021): 22586–22596, https://doi.org/10.1021/acsami.1c04517.

52.S. Y. Zhou, S. Yang, D. Cai, et al., "Cofactor-Assisted Artificial Enzyme with Multiple Li-Bond Networks for Sustainable Polysulfide Conversion in Lithium–Sulfur Batteries," Advanced Science 9, no. 3 (2022): 2104205, https://doi.org/10.1002/advs.202104205.

53.N. Sahiner, S. Demirci, and K. Sel, "Covalent Organic Framework Based on Melamine and Dibromoalkanes for Versatile Use," Journal of Porous Materials 23 (2016): 1025–1035, https://doi.org/10.1007/s10934-016-0160-9.

54.H. Y. Duan, K. Li, M. Xie, et al., "Scalable Synthesis of Ultrathin Polyimide Covalent Organic Framework Nanosheets for High-Performance Lithium–Sulfur Batteries," Journal of the American Chemical Society 143, no. 46 (2021): 19446–19453, https://doi.org/10.1021/jacs.1c08675.

55.J. Xie, J. L. Ye, F. Pan, et al., "Incorporating Flexibility into Stiffness: Self-Grown Carbon Nanotubes in Melamine Sponges Enable a Lithium-Metal-Anode Capacity of 15 mAh cm−2 Cyclable at 15 mA cm−2," Advanced Materials 31, no. 7 (2019): 1805654, https://doi.org/10.1002/adma.201805654.

56.Q. Wu, M. D. Fang, S. Z. Jiao, et al., "Phase Regulation Enabling Dense Polymer-Based Composite Electrolytes for Solid-State Lithium Metal Batteries," Nature Communications 14 (2023): 6296, https://doi.org/10.1038/s41467-023-41808-3.

57.D. C. Zhang, Y. X. Liu, D. D. Li, et al., "Salt Dissociation and Localized High-Concentration Solvation at the Interface of a Fluorinated Gel and Polymer Solid Electrolyte," Energy Environmental Science 18, no. 1 (2025): 227–235, https://doi.org/10.1039/D4EE04078C.

58.H. N. Chen, D. H. Li, M. Lin, et al., "Regulating the Isomerization Geometry and Energy State of Covalent Organic Frameworks for Enhanced Oxygen Reduction Activity," Advanced Materials 37, no. 13 (2025): 2500063, https://doi.org/10.1002/adma.202500063.

Basic Information:

DOI：10.23919/CHAIN.2025.000020

Chinese Library Classification Number:

Citation Information:

Lithium metal is regarded as an ideal anode material for high-energy-density batteries due to its high theoretical capacity and low electrochemical potential. However, its practical application is hindered by unstable electrode-electrolyte interfaces and lithium dendrite growth. Covalent organic frameworks (COFs), with ordered ion transport channels and abundant lithiophilic sites, offer a promising solution by facilitating uniform lithium deposition, suppressing dendrites, and mitigating side reactions. This review presents a comprehensive overview of the application of COFs in various battery components for regulating interfacial chemistry and inhibiting dendrite growth. The design concepts and synthesis techniques of COFs are explained in detail, and the discussion of present issues and potential future research avenues is included in the end.

quote

GB/T 7714-2015 [1] Qi An, Lu Liu, Panpan Mao, et al. Progress and perspectives of the covalent organic frameworks in regulating interface chemistry for high‐energy density Li metal batteries[J]. Chain, 2026, 3(1): 1-13. DOI:10.23919/CHAIN.2025.000020.
MLA [1] Qi An, et al., "Progress and perspectives of the covalent organic frameworks in regulating interface chemistry for high‐energy density Li metal batteries." Chain, vol. 3, no. 1, 2026, pp. 1-13, https://doi.org/10.23919/CHAIN.2025.000020.
APA [1] Qi An, Lu Liu, Panpan Mao, Fanyu Xie, Yufeng Fan, Huaiyu Shao, & Hong Guo. (2026). Progress and perspectives of the covalent organic frameworks in regulating interface chemistry for high‐energy density Li metal batteries. Chain, 3(1), 1-13. https://doi.org/10.23919/CHAIN.2025.000020
IEEE [1] Qi An, Lu Liu, Panpan Mao, Fanyu Xie, Yufeng Fan, Huaiyu Shao, and Hong Guo, "Progress and perspectives of the covalent organic frameworks in regulating interface chemistry for high‐energy density Li metal batteries," Chain, vol. 3, no. 1, pp. 1-13, 2026, doi: 10.23919/CHAIN.2025.000020. keywords: {covalent organic frameworks;interface chemistry;lithium dendrites;lithium metal batteries}