Turn off MathJax
Article Contents
Tianqin Huang, Pengrui Sun, Ruiqi Yong, Yan Wang, Ying Zhao, Chuhan Huang, Wei Zhou, Lifeng Ding, Lu Guo, Xianfen Wang, Meng Ding. Engineering LDH-Derived LiCoMnO4 Spinel/MXene Heterostructures via a Dual-Tuning Strategy for Efficient Lithium Extraction from Low-Grade Brines. Green Energy&Environment. doi: 10.1016/j.gee.2026.03.019
Citation: Tianqin Huang, Pengrui Sun, Ruiqi Yong, Yan Wang, Ying Zhao, Chuhan Huang, Wei Zhou, Lifeng Ding, Lu Guo, Xianfen Wang, Meng Ding. Engineering LDH-Derived LiCoMnO4 Spinel/MXene Heterostructures via a Dual-Tuning Strategy for Efficient Lithium Extraction from Low-Grade Brines. Green Energy&Environment. doi: 10.1016/j.gee.2026.03.019

Engineering LDH-Derived LiCoMnO4 Spinel/MXene Heterostructures via a Dual-Tuning Strategy for Efficient Lithium Extraction from Low-Grade Brines

doi: 10.1016/j.gee.2026.03.019
  • Electrochemical lithium extraction from low-grade salt lake brines is a sustainable approach to reliable and cost-efficient lithium supply, yet it is hindered by sluggish diffusion kinetics and the severe interference from competing Mg2+ ions. This study proposes a “dual-tuned” strategy to engineer a high-performance electrode by simultaneously optimizing the intrinsic crystal architecture and the extrinsic conductive network. First, nanosized LiCoMnO4 (LCMO) spinels (∼100 nm) were synthesized via a topotactic transformation from ultrathin Co-Mn-layered double hydroxide (LDH) precursors, effectively shortening ion diffusion paths. Second, these nano-spinels were integrated with Ti3C2Tx MXene nanosheets to construct a 3D conductive framework that accelerates electron transport. The optimized 50%LCMO/MXene electrode achieved a superior lithium adsorption capacity of 188.55 mg g–1 (4.45 mmol g–1) and remarkable stability (87.6% retention over 200 cycles). Mechanistic investigations via ex-situ XPS and DFT revealed a distinct adsorption pathway: Li+ undergoes bulk intercalation driven by reversible lattice volume evolution, while Mg2+ is restricted to surface accumulation. Moreover, DFT analysis reveals that the Mn environment remains remarkably rigid. This local electronic rigidity minimizes the Jahn-Teller effect and Mn dissolution, providing a fundamental structural explanation for the electrode’s enhanced durability.

     

  • loading
  • [1]
    A. Alessia, B. Alessandro, V.-G. Maria, V.-A. Carlos, B. Francesca, J. Clean. Prod. 300 (2021) 126954.
    [2]
    C.B. Tabelin, J. Dallas, S. Casanova, T. Pelech, G. Bournival, S. Saydam, I. Canbulat, Miner. Eng. 163 (2021) 106743.
    [3]
    P. Greim, A.A. Solomon, C. Breyer, Nat. Commun. 11 (2020) 4570.
    [4]
    M.L. Vera, W.R. Torres, C.I. Galli, A. Chagnes, V. Flexer, Nat. Rev. Earth Environ. 4 (2023) 149-165.
    [5]
    Q. Lu, P. Liu, T. Zhou, R. Huang, K. Zhang, L. Hu, R. Liu, Z. Ren, J. Wang, X. Wang, Nano Res. 17 (2024) 2563-2573.
    [6]
    H. Zhang, Z. Zhao, Y. Wang, K. Ni, Y. Wang, L. Zhu, J. Liu, X. Zhao, Acta Phys. -Chim. Sin. 42 (2026) 100130.
    [7]
    J.F. Song, L.D. Nghiem, X.-M. Li, T. He, Environ. Sci.: Water Res. Technol. 3 (2017) 593-597.
    [8]
    X. Zhao, S. Yang, X. Song, Y. Wang, H. Zhang, M. Li, Y. Wang, Adv. Sci. 11 (2024) 2405176.
    [9]
    M. Yong, M. Tang, L. Sun, F. Xiong, L. Xie, G. Zeng, X. Ren, K. Wang, Y. Cheng, Z. Li, E. Li, X. Zhang, H. Wang, Nat. Sustain. 7 (2024) 1662-1671.
    [10]
    S. Zhang, X. Wei, X. Cao, M. Peng, M. Wang, L. Jiang, J. Jin, Nat. Commun. 15 (2024) 238.
    [11]
    C.-Y. Zhong, Y.-P. Lv, W.-F. Wen, Q. Chen, W.-M. Zhang, ACS Sustain. Chem. Eng. 10 (2022) 6045-6056.
    [12]
    Q. Li, M. Elimelech, Environ. Sci. Technol. 38 (2004) 4683-4693.
    [13]
    S. An, Z. Li, X. Wang, T. Xu, L. Feng, Z. Lai, Nat. Water 3 (2025) 1449-1458.
    [14]
    D. Weng, H. Duan, Y. Hou, J. Huo, L. Chen, F. Zhang, J. Wang, Prog. Nat. Sci.: Mater. Int. 30 (2020) 139-152.
    [15]
    A. Battistel, M.S. Palagonia, D. Brogioli, F. La Mantia, R. Trocoli, Adv. Mater. 32 (2020) 1905440.
    [16]
    J. Ren, H. Zhu, Y. Fang, W. Li, S. Lan, S. Wei, Z. Yin, Y. Tang, Y. Ren, Q. Liu, Carbon Neutralization 2 (2023) 339-377.
    [17]
    J. Huang, L. Xue, Y. Huang, Y. Jiang, P. Wu, X. Fan, J. Zhu, Nat. Commun. 15 (2024) 6666.
    [18]
    X. Hou, X. Liu, H. Wang, X. Zhang, J. Zhou, M. Wang, Energy Storage Mater. 57 (2023) 577-606.
    [19]
    Y. Xu, Y. Li, X. Zhao, Y. Li, X.L. Li, J. Wang, H.Y. Yang, Nano Lett. 25 (2025) 995-1001.
    [20]
    Y. Huang, Y. Dong, S. Li, J. Lee, C. Wang, Z. Zhu, W. Xue, Y. Li, J. Li, Adv. Energy Mater. 11 (2021) 2000997.
    [21]
    L. Xiong, Y. Xu, T. Tao, J.B. Goodenough, J. Power Sources 199 (2012) 214-219.
    [22]
    A. Gutierrez, A. Manthiram, J. Electrochem. Soc. 160 (2013) A901.
    [23]
    Y. Shin, A. Manthiram, J. Electrochem. Soc. 151 (2004) A204.
    [24]
    J. Tang, Q. Luo, Z. Wu, K. Shi, Chem. Eng. J. 505 (2025) 159256.
    [25]
    R. Sharma, Nihal, M. Sharma, J.K. Goswamy, J. Electrochem. Soc. 169 (2022) 083505.
    [26]
    S.-M. Bak, K.-W. Nam, C.-W. Lee, K.-H. Kim, H.-C. Jung, X.-Q. Yang, K.-B. Kim, J. Mater. Chem. 21 (2011) 17309-17315.
    [27]
    J. Wang, C.-F. Du, Y. Xue, X. Tan, J. Kang, Y. Gao, H. Yu, Q. Yan, Exploration 1 (2021) 20210024.
    [28]
    N. Xue, X. Wu, H. Shi, Y. Zhang, Y. Zhang, Y. Lv, X. Zhang, X. Chen, Y. Yu, W. Liu, ACS Nano 18 (2024) 33743-33753.
    [29]
    S. Vijayan, B. Kirubasankar, P. Pazhamalai, A.K. Solarajan, S. Angaiah, ChemElectroChem 4 (2017) 2059-2067.
    [30]
    L. Li, X. Ke, S. Wang, Z. Jiang, Y. Guo, C. Kuai, Chin. Chem. Lett. 36 (2025) 110423.
    [31]
    S.M.M. Alonzo, B.P. Bastakoti, Mater. Today Nano 32 (2025) 100704.
    [32]
    V. Paulraj, S. Kanthasamy, S. Thangavelu, New J. Chem. 49 (2025) 20209-20221.
    [33]
    M. Ghidiu, M.R. Lukatskaya, M.-Q. Zhao, Y. Gogotsi, M.W. Barsoum, Nature 516 (2014) 78-81.
    [34]
    Z. Meng, H. Yan, P. Qin, X. Zhou, X. Wang, H. Chen, L. Liu, Z. Liu, Adv. Funct. Mater. 33 (2023) 2305225.
    [35]
    K.F. Ortega, S. Anke, S. Salamon, F. Ozcan, J. Heese, C. Andronescu, J. Landers, H. Wende, W. Schuhmann, M. Muhler, T. Lunkenbein, M. Behrens, Chem. Eur. J. 23 (2017) 12443-12449.
    [36]
    R. Malik, D. Burch, M. Bazant, G. Ceder, Nano Lett. 10 (2010) 4123-4127.
    [37]
    C. He, J. Zhang, D. Mantzavinos, A. Katsaounis, D.H. Si, Z. Yan, H.Y. Zhang, Z.W. Jiang, Angew. Chem. Int. Ed. 64 (2025) e202420295.
    [38]
    Y.-W. Zhou, E. Ibanez-Ale, N. Lopez, B. Roldan Cuenya, C.S. Kley, Nat. Chem. 18 (2025) 473-481.
    [39]
    X. An, Z. Du, B. Qiao, S. Wang, P. Wang, X. Ma, Y. Li, X. Du, X. Hao, G. Guan, Desalination 591 (2024) 118016.
    [40]
    C. Zhang, J. Zheng, Z. Chen, J. Xu, Adv. Funct. Mater. 36 (2025) e19049.
    [41]
    B. Hu, B. Zhang, Y. Wang, M. Li, J. Yang, J. Liu, Desalination 560 (2023) 116662.
    [42]
    C. He, J. Zhang, R. Song, D. Mantzavinos, A. Katsaounis, R. Weng, X. Wang, Z. Yan, Y. Qu, W. Lu, Z. Jiang, Adv. Funct. Mater. 36 (2025) e22607.
    [43]
    J. Makela, A. Lahti, M. Tuominen, M. Yasir, M. Kuzmin, P. Laukkanen, K. Kokko, M.P.J. Punkkinen, H. Dong, B. Brennan, R.M. Wallace, Sci. Rep. 9 (2019) 1462.
    [44]
    Y. Zhang, Y. Liu, Z. Liu, X. Wu, Y. Wen, H. Chen, X. Ni, G. Liu, J. Huang, S. Peng, J. Energy Chem. 64 (2022) 23-32.
    [45]
    X. Zhao, Y. Wang, Y. Wang, H. Zhang, Z. Zhao, L. Zhu, Y. Wang, Chem. Eng. J. 521 (2025) 166575.
    [46]
    Y. Ren, J. He, S. Jiang, R. He, Q. Liang, B. Zhu, Y. Wen, S. Zhuang, Mater. Lett. 357 (2024) 135765.
    [47]
    X. Zhao, Y. Gong, K. Gao, Y. Wang, H.Y. Yang, Chem. Eng. J. 474 (2023) 145975.
    [48]
    J. Tang, Q. Luo, K. Shi, Ceram. Int. 51 (2025) 51526-51534.
    [49]
    X. Pei, Y. Mu, X. Dong, C. Ding, L. Xu, M. Cui, C. Meng, Y. Zhang, Carbon Neutralization 2 (2023) 115-126.
    [50]
    X. Zhao, L. Zheng, Y. Hou, Y. Wang, L. Zhu, Chem. Eng. J. 450 (2022) 138454.
    [51]
    M. Ding, S. Fan, S. Huang, M.E. Pam, L. Guo, Y. Shi, H.Y. Yang, ACS Appl. Energy Mater. 2 (2019) 1812-1822.
    [52]
    H.-L. Girard, H. Wang, A. D’entremont, L. Pilon, J. Phys. Chem. C 119 (2015) 11349-11361.
    [53]
    J. Cui, T. Huang, Y. Zhao, A. Bentley, M. Xu, L. Guo, M. Ding, H.Y. Yang, Sep. Purif. Technol. 339 (2024) 126613.
    [54]
    J. Wang, J. Polleux, J. Lim, B. Dunn, J. Phys. Chem. C 111 (2007) 14925-14931.
    [55]
    R. Yong, Y. Zhao, C. Huang, P. Sun, W. Zhou, T. Huang, Y. Wei, K. Kajanann, K. Fan, K. Lin, Y. Wang, L. Ding, M. Ding, Chem. Eng. J. 524 (2025) 169685.
    [56]
    W. Zhou, T. Huang, Y. Zhao, D. Kang, C. Huang, M. Ding, Chem. Eng. J. 508 (2025) 161124.
    [57]
    T. Elmakki, S. Zavahir, H.K. Shon, G.H. Gago, H. Park, D.S. Han, Desalination 593 (2025) 118195.
    [58]
    Z.-Y. Guo, Z.-Y. Ji, J. Wang, X.-F. Guo, J.-S. Liang, Desalination 533 (2022) 115767.
    [59]
    Y. Wu, P. Shi, Y. Zhong, R. Cai, Energy Fuels 37 (2023) 4083-4093.
    [60]
    M. Kerroumi, M. Karbak, H. Afaryate, A. El-Bchiri, M. Aqil, B. Manoun, Y. Tamraoui, H. Girault, F. Ghamouss, Electrochim. Acta 509 (2025) 145286.
    [61]
    H. Zhang, Z. Huang, L. Zhao, Z. Guo, J. Wang, J. Liu, Y. Zhao, F. Li, P. Zhang, Z.-Y. Ji, Chem. Eng. J. 482 (2024) 148802.
    [62]
    S. Kim, J. Lee, S. Kim, S. Kim, J. Yoon, Energy Technol. 6 (2018) 340-344.
    [63]
    X. Zhao, G. Li, M. Feng, Y. Wang, Electrochim. Acta 331 (2020) 135285.
    [64]
    C. Huang, T. Huang, X.L. Li, W. Zhou, M. Ding, J. Mater. Chem. A 12 (2024) 8734-8746.
    [65]
    B. Hu, Y. Wang, B. Zhang, X. Song, H. Jiang, J. Ma, J. Liu, Sep. Purif. Technol. 348 (2024) 127693.
    [66]
    Y. Tesfamhret, H. Liu, Z. Chai, E. Berg, R. Younesi, ChemElectroChem 8 (2021) 1516-1523.
    [67]
    Z. Zhu, G. Li, Mater. Today Energy 53 (2025) 102000.
    [68]
    Y. Qiao, H. Zhang, Y. Nian, Y. Li, C. Xiao, T. Wang, Y. Wang, M. Wen, Y. Han, J. Qiu, ACS Nano 19 (2025) 41777-41788.
    [69]
    X. Li, Z. Ao, J. Liu, H. Sun, A.I. Rykov, J. Wang, ACS Nano 10 (2016) 11532-11540.
    [70]
    T. Chen, G. Sai Gautam, W. Huang, G. Ceder, Chem. Mater. 30 (2018) 153-162.
    [71]
    M. Zhao, X. Zhang, H. Yu, Y. Xie, T. Yi, Energy Environ. Mater. 8 (2025) e70060.
    [72]
    Y. Pan, A. Hu, R. Xu, J. Chen, B. Yang, T. Li, K. Li, Y. Li, Z.W. Seh, J. Long, ACS Sustain. Chem. Eng. 12 (2024) 17177-17189.
    [73]
    M. Abbate, F.M.F. De Groot, J.C. Fuggle, A. Fujimori, O. Strebel, F. Lopez, M. Domke, G. Kaindl, G.A. Sawatzky, M. Takano, Y. Takeda, H. Eisaki, S. Uchida, Phys. Rev. B 46 (1992) 4511-4519.
    [74]
    Y. Shao-Horn, S.A. Hackney, A.J. Kahaian, K.D. Kepler, E. Skinner, J.T. Vaughey, M.M. Thackeray, J. Power Sources 81-82 (1999) 496-499.
    [75]
    S. Choi, W. Feng, Y. Xia, ACS Omega 9 (2024) 18688-18708.
    [76]
    H. Kawai, M. Nagata, H. Tukamoto, A.R. West, J. Power Sources 81-82 (1999) 67-72.
    [77]
    L. Xu, T. Wu, P.R.C. Kent, D.-E. Jiang, Phys. Rev. Mater. 5 (2021) 054007.
  • 加载中

Catalog

    通讯作者: 陈斌, bchen63@163.com
    • 1. 

      沈阳化工大学材料科学与工程学院 沈阳 110142

    1. 本站搜索
    2. 百度学术搜索
    3. 万方数据库搜索
    4. CNKI搜索

    Article Metrics

    Article views (5) PDF downloads(0) Cited by()
    Proportional views

    /

    DownLoad:  Full-Size Img  PowerPoint
    Return
    Return