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Citation: Yang LU, Xiang CHEN, Chen-Zi ZHAO, Qiang ZHANG. Machine Learning towards Screening Solid-state Lithium Ion Conductors[J]. Chinese Journal of Structural Chemistry, ;2020, 39(1): 8-10. doi: 10.14102/j.cnki.0254-5861.2011-2710 shu

Machine Learning towards Screening Solid-state Lithium Ion Conductors

  • Beijing Key Laboratory of Green Chemical Reaction Engineering and Technology, Department of Chemical Engineering, Tsinghua University, Beijing 100084, China

  • Corresponding author: Qiang ZHANG, zhang-qiang@mails.tsinghua.edu.cn
  • Received Date: 20 December 2019
    Accepted Date: 26 December 2019

    Fund Project: the National Key Research and Development Program 2016YFA0202500National Natural Science Foundation of China 21825501

Figures(1)

  • Machine learning is an emerging method to discover new materials with specific characteristics. An unsupervised machine learning research is highlighted to discover new potential lithium ionic conductors by screening and clustering lithium compounds, providing inspirations for the development of solid-state electrolytes and practical batteries.

  • Solid-state chemistry is drawing increasing attention due to the rise of solid-state electrolytes (SSEs). SSEs enable the accelerated migration of multiple anions such as lithium (Li) and sodium at solid-state mode. Compared with routine organic liquid electrolytes in Li batteries, solid Li ionic conductors (SSLCs) can realize high thermal stability, high ionic conductivity, and wide electrochemical windows, which enables the application of Li metal anodes[1]. Consequently, SSLCs have been treated as a promising solution to break through the anxiety of limited energy density of conventional Li-ion batteries. Tremendous efforts have been devoted to this field and have achieved significant progresses[2]. However, the experimentally synthesized solid electrolytes cannot meet the multiple requirements in practical batteries, which is calling for emerging methodology and instructions to explore advanced solid-state electrolytes.

    Figure 1

    Figure 1.  Unsupervised clustering results for Li contained compounds. Most high ionic conductive materials are located in groups V and VI, which possess mild distortion anion structures. The materials in groups V and VI exhibit obvious talents of high ionic conductivity[11], which are concentrated for the subsequent screening
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    The known SSLCs exhibit various crystalline structures, including layered patterns (Li3N), garnet (Li7La3Zr2O12), NASICON (Li1.5Al0.5Ti0.5(PO4)3), perovskite (Li0.5La0.5TiO3), anti-perovskite (Li3OX, X = Cl and Br), thio-LISICON (Li10GeP2S12, LGPS) and argyrodite (Li6PS5X, X = Cl, Br, and I)[3-7]. These typical ionic conductors possess disparate crystalline structure, physical/chemical properties, and ionic conductivities, whose internal connection is difficult to be completely analyzed and unraveled. Therefore, designing brand-new Li ionic conductive materials confronts tremendous challenges. Conventional explorations depending on experimental try and errors are not effective. Based on the already known materials, a rapid exploration and screening impel the development of material genome engineering[8]. Mo and co-authors have conducted much beneficial work towards the prediction of (electro)chemical stability against Li metal and the electrochemical window of multiple solid-state electrolytes, affording an accurate guidance for interfacial engineering[9, 10]. The supervised learning methods require abundant data to train the models. A large amount of involved data guarantees the accuracy of the trained model. However, the kinds of known SSLCs are insufficient to conduct supervised machine learning with a high accuracy. Most Li contained compounds do not possess high ionic conductivities, which cannot be treated as training materials. In order to figure out the disadvantages, Mo, Ling, and co-workers creatively conducted an unsupervised machine learning study, which is a new route to unravel the interior differences between SSLCs and thus can predict new potential SSLCs[11]. The unsupervised machine learning model simultaneously divides the data into different groups according to data characteristics.

    In the unsupervised model, the authors designed a protocol as follows: digitalizing Li-contained compounds, clustering the targeted groups, and running ab initio molecular dynamics (AIMD) simulations to verify the predicted objects. The anion framework of Li-contained compounds is firstly digitalized by the modified XRD (mXRD) representation. In order to highlight the structural crystal features, only the anion framework is considered. The mXRD means that the characteristics of the anion frameworks are transformed into a group of lattice parameters shown in XRD patterns. Each compound will be simplified into a vector. Then the mXRD clustering classified compounds by their characteristics of their anion framework structures. The Li ions located in the highly symmetric lattices are constrained at the well-defined sites. The highly disordered framework will also locally trap ions and hinder possible percolations. It is concluded that anion frameworks with a mild distortion, which are located between the highly symmetric lattices and the highly disordered ones, possess high ionic conductivities. This fruitful insight affords a great reference for further screening of ionic conductors. The groups with mild distortion are further screened by AIMD simulation to choose objects with high ionic conductivities. More significantly, the unsupervised method dramatically shrinks the range for screening and increases screening efficiency compared with the conventional high throughput methods. The unsupervised machine learning is appropriate to estimate potential materials with high ionic conductivities. The results for screening also provide targets for experimental attempts. Because the new predicted materials exhibit disparate crystal structures, the results can also help to broaden the thoughts.

    The solid Li ionic conductor is a complicated system, involving many chemical and physical parameters. This unsupervised machine learning system does not cover sufficient details in solid Li ionic conductors. Therefore, the accuracy of the machine learning model can be further improved. The unsupervised machine learning method is a new brand route for predictions, integrating the high throughput results towards screening solid-state lithium ion conductors for next-generation batteries.


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      Xiao, W.; Wang, J.; Fan, L.; Zhang, J.; Li, X. Recent advances in Li1+xAlxTi2−x(PO4)3 solid-state electrolyte for safe lithium batteries. Energy Storage Mater. 2019, 19, 379–400.  doi: 10.1016/j.ensm.2018.10.012

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